Articles | Volume 13, issue 6
https://doi.org/10.5194/amt-13-3119-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-13-3119-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Jun 2020
Research article |
| 12 Jun 2020
| 12 Jun 2020
Implementation of a chemical background method for atmospheric OH measurements by laser-induced fluorescence: characterisation and observations from the UK and China
Robert Woodward-Massey
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
now at: College of Environmental Sciences and Engineering, Peking
University, Beijing, 100871, China
Eloise J. Slater
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
Jake Alen
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
Trevor Ingham
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Atmospheric Science, University of Leeds, Leeds,
LS2 9JT, UK
Danny R. Cryer
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
Leanne M. Stimpson
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
Chunxiang Ye
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
now at: College of Environmental Sciences and Engineering, Peking
University, Beijing, 100871, China
Paul W. Seakins
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
Lisa K. Whalley
CORRESPONDING AUTHOR
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
National Centre for Atmospheric Science, University of Leeds, Leeds,
LS2 9JT, UK
School of Chemistry, University of Leeds, Leeds, LS2 9JT, UK
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Yaru Wang, Yi Chen, Suzhen Chi, Jianshu Wang, Chong Zhang, Weixiong Zhao, Weili Lin, and Chunxiang Ye
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-192, https://doi.org/10.5194/amt-2023-192, 2023
Revised manuscript not accepted
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Wanyun Xu, Yuxuan Bian, Weili Lin, Yingjie Zhang, Yaru Wang, Zhiqiang Ma, Xiaoyi Zhang, Gen Zhang, Chunxiang Ye, and Xiaobin Xu
Atmos. Chem. Phys., 23, 7635–7652, https://doi.org/10.5194/acp-23-7635-2023, https://doi.org/10.5194/acp-23-7635-2023, 2023
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Tropospheric ozone (O3) and peroxyacetyl nitrate (PAN) are both photochemical pollutants harmful to the ecological environment and human health, especially in the Tibetan Plateau (TP). However, the factors determining their variations in the TP have not been comprehensively investigated. Results from field measurements and observation-based models revealed that day-to-day variations in O3 and PAN were in fact controlled by distinct physiochemical processes.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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Lizi Tang, Min Hu, Dongjie Shang, Xin Fang, Jianjiong Mao, Wanyun Xu, Jiacheng Zhou, Weixiong Zhao, Yaru Wang, Chong Zhang, Yingjie Zhang, Jianlin Hu, Limin Zeng, Chunxiang Ye, Song Guo, and Zhijun Wu
Atmos. Chem. Phys., 23, 4343–4359, https://doi.org/10.5194/acp-23-4343-2023, https://doi.org/10.5194/acp-23-4343-2023, 2023
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There was an evident distinction in the frequency of new particle formation (NPF) events at Nam Co station on the Tibetan Plateau: 15 % in pre-monsoon season and 80 % in monsoon season. The frequent NPF events in monsoon season resulted from the higher frequency of southerly air masses, which brought the organic precursors to participate in the NPF process. It increased the amount of aerosol and CCN compared with those in pre-monsoon season, which may markedly affect earth's radiation balance.
Simone T. Andersen, Beth S. Nelson, Katie A. Read, Shalini Punjabi, Luis Neves, Matthew J. Rowlinson, James Hopkins, Tomás Sherwen, Lisa K. Whalley, James D. Lee, and Lucy J. Carpenter
Atmos. Chem. Phys., 22, 15747–15765, https://doi.org/10.5194/acp-22-15747-2022, https://doi.org/10.5194/acp-22-15747-2022, 2022
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The cycling of NO and NO2 is important to understand to be able to predict O3 concentrations in the atmosphere. We have used long-term measurements from the Cape Verde Atmospheric Observatory together with model outputs to investigate the cycling of nitrogen oxide (NO) and nitrogen dioxide (NO2) in very clean marine air. This study shows that we understand the processes occurring in very clean air, but with small amounts of pollution in the air, known chemistry cannot explain what is observed.
Hao Yin, Youwen Sun, Justus Notholt, Mathias Palm, Chunxiang Ye, and Cheng Liu
Atmos. Chem. Phys., 22, 14401–14419, https://doi.org/10.5194/acp-22-14401-2022, https://doi.org/10.5194/acp-22-14401-2022, 2022
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Improved knowledge of the chemistry and drivers of surface ozone over the Qinghai-Tibet Plateau (QTP) is significant for regulatory and control purposes in this high-altitude region in the Himalayas. Our study investigates the processes and drivers of surface ozone anomalies by using machine-learning model-based meteorological normalization methods between 2015 and 2020 in urban areas over the QTP. This study can provide valuable implication for ozone mitigation over the QTP.
Yuhan Liu, Xuejiao Wang, Jing Shang, Weiwei Xu, Mengshuang Sheng, and Chunxiang Ye
Atmos. Chem. Phys., 22, 11347–11358, https://doi.org/10.5194/acp-22-11347-2022, https://doi.org/10.5194/acp-22-11347-2022, 2022
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In this study, the influence of HCHO on renoxification on nitrate-doped TiO2 particles is investigated by using an experimental chamber. Mass NOx release is suggested to follow the NO−3-NO3·-HNO3-NOx pathway, with HCHO involved in the transformation of NO3· to HNO3 through hydrogen abstraction. Our proposed reaction mechanism by which HCHO promotes photocatalytic renoxification is helpful for deeply understanding the atmospheric photochemical processes and nitrogen cycling.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Marios Panagi, Roberto Sommariva, Zoë L. Fleming, Paul S. Monks, Gongda Lu, Eloise A. Marais, James R. Hopkins, Alastair C. Lewis, Qiang Zhang, James D. Lee, Freya A. Squires, Lisa K. Whalley, Eloise J. Slater, Dwayne E. Heard, Robert Woodward-Massey, Chunxiang Ye, and Joshua D. Vande Hey
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-379, https://doi.org/10.5194/acp-2022-379, 2022
Revised manuscript not accepted
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A dispersion model and a box model were combined to investigate the evolution of VOCs in Beijing once they are emitted from anthropogenic sources. It was determined that during the winter time the VOC concentrations in Beijing are driven predominantly by sources within Beijing and by a combination of transport and chemistry during the summer. Furthermore, the results in the paper highlight the need for a season specific policy.
Yuting Zhu, Youfeng Wang, Xianliang Zhou, Yasin F. Elshorbany, Chunxiang Ye, Matthew Hayden, and Andrew J. Peters
Atmos. Chem. Phys., 22, 6327–6346, https://doi.org/10.5194/acp-22-6327-2022, https://doi.org/10.5194/acp-22-6327-2022, 2022
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The daytime chemistry of nitrous acid (HONO), which plays an important role in the oxidation capacity of the troposphere, is not well understood. In this work, we report new field measurement results of HONO and the relevant parameters in the marine boundary layer at Tudor Hill Marine Atmospheric Observatory in Bermuda. We evaluate the daytime HONO budgets in air masses under different types of interaction with the island and examine the strengths of different HONO formation and loss mechanisms.
Zara S. Mir, Matthew Jamieson, Nicholas R. Greenall, Paul W. Seakins, Mark A. Blitz, and Daniel Stone
Atmos. Meas. Tech., 15, 2875–2887, https://doi.org/10.5194/amt-15-2875-2022, https://doi.org/10.5194/amt-15-2875-2022, 2022
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In this work we describe the development and characterisation of an experiment using laser flash photolysis coupled with time-resolved mid-infrared (mid-IR) quantum cascade laser (QCL) absorption spectroscopy, with initial results reported for measurements of the infrared spectrum, kinetics, and product yields for the reaction of the CH2OO Criegee intermediate with SO2. This work has significance for the identification and measurement of reactive trace species in complex systems.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J1 Bloss, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-207, https://doi.org/10.5194/acp-2022-207, 2022
Preprint withdrawn
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We measured radicals (OH, HO2, RO2) and OH reactivity at a UK coastal site and compared our observations to the predictions of an MCMv3.3.1 box model. We find variable agreement between measured and modelled radical concentrations and OH reactivity, where the levels of agreement for individual species display strong dependences on NO concentrations. The most substantial disagreement is found for RO2 at high NO (> 1 ppbv), when RO2 levels are underpredicted by a factor of ~10–30.
Beth S. Nelson, Gareth J. Stewart, Will S. Drysdale, Mike J. Newland, Adam R. Vaughan, Rachel E. Dunmore, Pete M. Edwards, Alastair C. Lewis, Jacqueline F. Hamilton, W. Joe Acton, C. Nicholas Hewitt, Leigh R. Crilley, Mohammed S. Alam, Ülkü A. Şahin, David C. S. Beddows, William J. Bloss, Eloise Slater, Lisa K. Whalley, Dwayne E. Heard, James M. Cash, Ben Langford, Eiko Nemitz, Roberto Sommariva, Sam Cox, Shivani, Ranu Gadi, Bhola R. Gurjar, James R. Hopkins, Andrew R. Rickard, and James D. Lee
Atmos. Chem. Phys., 21, 13609–13630, https://doi.org/10.5194/acp-21-13609-2021, https://doi.org/10.5194/acp-21-13609-2021, 2021
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Ozone production at an urban site in Delhi is sensitive to volatile organic compound (VOC) concentrations, particularly those of the aromatic, monoterpene, and alkene VOC classes. The change in ozone production by varying atmospheric pollutants according to their sources, as defined in an emissions inventory, is investigated. The study suggests that reducing road transport emissions alone does not reduce reactive VOCs in the atmosphere enough to perturb an increase in ozone production.
Esther Borrás, Luis A. Tortajada-Genaro, Milagro Ródenas, Teresa Vera, Thomas Speak, Paul Seakins, Marvin D. Shaw, Alastair C. Lewis, and Amalia Muñoz
Atmos. Meas. Tech., 14, 4989–4999, https://doi.org/10.5194/amt-14-4989-2021, https://doi.org/10.5194/amt-14-4989-2021, 2021
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This work presents promising results in the characterization of specific atmospheric pollutants (oxygenated VOCs) present at very low but highly relevant concentrations.
We carried out this research at EUPHORE facilities within the framework of the EUROCHAMP project. A new analytical method, with high robustness and precision, also clean in the use of solvents, low cost, and easily adaptable for use in mobile laboratories for air quality monitoring, is presented.
Claire E. Reeves, Graham P. Mills, Lisa K. Whalley, W. Joe F. Acton, William J. Bloss, Leigh R. Crilley, Sue Grimmond, Dwayne E. Heard, C. Nicholas Hewitt, James R. Hopkins, Simone Kotthaus, Louisa J. Kramer, Roderic L. Jones, James D. Lee, Yanhui Liu, Bin Ouyang, Eloise Slater, Freya Squires, Xinming Wang, Robert Woodward-Massey, and Chunxiang Ye
Atmos. Chem. Phys., 21, 6315–6330, https://doi.org/10.5194/acp-21-6315-2021, https://doi.org/10.5194/acp-21-6315-2021, 2021
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The impact of isoprene on atmospheric chemistry is dependent on how its oxidation products interact with other pollutants, specifically nitrogen oxides. Such interactions can lead to isoprene nitrates. We made measurements of the concentrations of individual isoprene nitrate isomers in Beijing and used a model to test current understanding of their chemistry. We highlight areas of uncertainty in understanding, in particular the chemistry following oxidation of isoprene by the nitrate radical.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Weili Lin, Feng Wang, Chunxiang Ye, and Tong Zhu
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-32, https://doi.org/10.5194/tc-2021-32, 2021
Preprint withdrawn
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Field observations found that released NOx on the glacier surface of the Tibetan Plateau, an important snow-covered region in the northern mid-latitudes, had a higher concentration than in Antarctic and Arctic regions. Such evidence, and such high fluxes as observed here on the Tibetan plateau is novel. That such high concentrations of nitrogen oxides can be found in remote areas is interesting and important for the oxidative budget of the boundary layer.
Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Archit Mehra, Stephen D. Worrall, Asan Bacak, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Tuan Vu, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 2125–2147, https://doi.org/10.5194/acp-21-2125-2021, https://doi.org/10.5194/acp-21-2125-2021, 2021
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To understand how emission controls will impact ozone, an understanding of the sources and sinks of OH and the chemical cycling between peroxy radicals is needed. This paper presents measurements of OH, HO2 and total RO2 taken in central Beijing. The radical observations are compared to a detailed chemistry model, which shows that under low NO conditions, there is a missing OH source. Under high NOx conditions, the model under-predicts RO2 and impacts our ability to model ozone.
Mike J. Newland, Daniel J. Bryant, Rachel E. Dunmore, Thomas J. Bannan, W. Joe F. Acton, Ben Langford, James R. Hopkins, Freya A. Squires, William Dixon, William S. Drysdale, Peter D. Ivatt, Mathew J. Evans, Peter M. Edwards, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, C. Nicholas Hewitt, James D. Lee, Tianqu Cui, Jason D. Surratt, Xinming Wang, Alastair C. Lewis, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 21, 1613–1625, https://doi.org/10.5194/acp-21-1613-2021, https://doi.org/10.5194/acp-21-1613-2021, 2021
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We report the formation of secondary pollutants in the urban megacity of Beijing that are typically associated with remote regions such as rainforests. This is caused by extremely low levels of nitric oxide (NO), typically expected to be high in urban areas, observed in the afternoon. This work has significant implications for how we understand atmospheric chemistry in the urban environment and thus for how to implement effective policies to improve urban air quality.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
Eloise J. Slater, Lisa K. Whalley, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Leigh R. Crilley, Louisa Kramer, William Bloss, Tuan Vu, Yele Sun, Weiqi Xu, Siyao Yue, Lujie Ren, W. Joe F. Acton, C. Nicholas Hewitt, Xinming Wang, Pingqing Fu, and Dwayne E. Heard
Atmos. Chem. Phys., 20, 14847–14871, https://doi.org/10.5194/acp-20-14847-2020, https://doi.org/10.5194/acp-20-14847-2020, 2020
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The paper details atmospheric chemistry in a megacity (Beijing), focussing on radicals which mediate the formation of secondary pollutants such as ozone and particles. Highly polluted conditions were experienced, including the highest ever levels of nitric oxide (NO), with simultaneous radical measurements. Radical concentrations were large during "haze" events, demonstrating active photochemistry. Modelling showed that our understanding of the chemistry at high NOx levels is incomplete.
Daniel J. Bryant, William J. Dixon, James R. Hopkins, Rachel E. Dunmore, Kelly L. Pereira, Marvin Shaw, Freya A. Squires, Thomas J. Bannan, Archit Mehra, Stephen D. Worrall, Asan Bacak, Hugh Coe, Carl J. Percival, Lisa K. Whalley, Dwayne E. Heard, Eloise J. Slater, Bin Ouyang, Tianqu Cui, Jason D. Surratt, Di Liu, Zongbo Shi, Roy Harrison, Yele Sun, Weiqi Xu, Alastair C. Lewis, James D. Lee, Andrew R. Rickard, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 20, 7531–7552, https://doi.org/10.5194/acp-20-7531-2020, https://doi.org/10.5194/acp-20-7531-2020, 2020
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Using the chemical composition of offline filter samples, we report that a large share of oxidized organic aerosol in Beijing during summer is due to isoprene secondary organic aerosol (iSOA). iSOA organosulfates showed a strong correlation with the product of ozone and particulate sulfate. This highlights the role of both photochemistry and the availability of particulate sulfate in heterogeneous reactions and further demonstrates that iSOA formation is controlled by anthropogenic emissions.
Lavinia Onel, Alexander Brennan, Michele Gianella, James Hooper, Nicole Ng, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 13, 2441–2456, https://doi.org/10.5194/amt-13-2441-2020, https://doi.org/10.5194/amt-13-2441-2020, 2020
Fanhao Meng, Min Qin, Ke Tang, Jun Duan, Wu Fang, Shuaixi Liang, Kaidi Ye, Pinhua Xie, Yele Sun, Conghui Xie, Chunxiang Ye, Pingqing Fu, Jianguo Liu, and Wenqing Liu
Atmos. Chem. Phys., 20, 5071–5092, https://doi.org/10.5194/acp-20-5071-2020, https://doi.org/10.5194/acp-20-5071-2020, 2020
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Nitrous acid (HONO), a major precursor of the OH radical, plays a key role in atmospheric chemistry, but its sources are still debated. The first high-resolution vertical measurements of HONO and NO2 were conducted in Beijing to investigate the nocturnal sources of HONO at different stages of pollution. The ground surface dominated HONO production by heterogeneous conversion of NO2 during clean episodes, but the aerosol production was an important nighttime HONO source during haze episodes.
Thomas H. Speak, Mark A. Blitz, Daniel Stone, and Paul W. Seakins
Atmos. Meas. Tech., 13, 839–852, https://doi.org/10.5194/amt-13-839-2020, https://doi.org/10.5194/amt-13-839-2020, 2020
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OH and HO2 radicals are important trace constituents of the atmosphere that are closely coupled via several types of reaction. This paper describes a new laboratory method to simultaneously determine OH kinetics and HO2 yields from chemical processes. The instrument also provides some time resolution on HO2 detection allowing one to separate HO2 produced from the target reaction from HO2 arising from secondary chemistry. Examples of applications are presented.
Yingruo Li, Ziqiang Tan, Chunxiang Ye, Junxia Wang, Yanwen Wang, Yi Zhu, Pengfei Liang, Xi Chen, Yanhua Fang, Yiqun Han, Qi Wang, Di He, Yao Wang, and Tong Zhu
Atmos. Chem. Phys., 19, 13841–13857, https://doi.org/10.5194/acp-19-13841-2019, https://doi.org/10.5194/acp-19-13841-2019, 2019
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Vehicle emissions are a major source of Beijing's pollution. Various vehicle emission control policies have been implemented at great cost, but there is a lack of appropriate methods to evaluate the effectiveness of such policies. Here we developed a new method to evaluate the effectiveness of vehicle emission control policies during APEC. Our findings are instructive for air pollution control policy making.
Yanhua Fang, Chunxiang Ye, Junxia Wang, Yusheng Wu, Min Hu, Weili Lin, Fanfan Xu, and Tong Zhu
Atmos. Chem. Phys., 19, 12295–12307, https://doi.org/10.5194/acp-19-12295-2019, https://doi.org/10.5194/acp-19-12295-2019, 2019
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Year-long observations of PM2.5, gaseous pollutants, and meteorological parameters in Beijing were analysed to investigate sulfate formation. RH and O3 concentrations above thresholds of 45 % and 35 ppb, respectively, greatly accelerated sulfate formation. Ambient changes in RH and O3 contributed to variations in sulfate formation among different seasons and pollution levels. A shift from gas-phase to multiphase SO2 oxidation contributed to fast sulfate formation under polluted conditions.
Michael Hollaway, Oliver Wild, Ting Yang, Yele Sun, Weiqi Xu, Conghui Xie, Lisa Whalley, Eloise Slater, Dwayne Heard, and Dantong Liu
Atmos. Chem. Phys., 19, 9699–9714, https://doi.org/10.5194/acp-19-9699-2019, https://doi.org/10.5194/acp-19-9699-2019, 2019
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This study, for the first time, uses combinations of aerosol and lidar data to drive an offline photolysis scheme. Absorbing species are shown to have the greatest impact on photolysis rate constants in the winter and scattering aerosol are shown to dominate responses in the summer. During haze episodes, aerosols are shown to produce a greater impact than cloud cover. The findings demonstrate the potential photochemical impacts of haze pollution in a highly polluted urban environment.
Zongbo Shi, Tuan Vu, Simone Kotthaus, Roy M. Harrison, Sue Grimmond, Siyao Yue, Tong Zhu, James Lee, Yiqun Han, Matthias Demuzere, Rachel E. Dunmore, Lujie Ren, Di Liu, Yuanlin Wang, Oliver Wild, James Allan, W. Joe Acton, Janet Barlow, Benjamin Barratt, David Beddows, William J. Bloss, Giulia Calzolai, David Carruthers, David C. Carslaw, Queenie Chan, Lia Chatzidiakou, Yang Chen, Leigh Crilley, Hugh Coe, Tie Dai, Ruth Doherty, Fengkui Duan, Pingqing Fu, Baozhu Ge, Maofa Ge, Daobo Guan, Jacqueline F. Hamilton, Kebin He, Mathew Heal, Dwayne Heard, C. Nicholas Hewitt, Michael Hollaway, Min Hu, Dongsheng Ji, Xujiang Jiang, Rod Jones, Markus Kalberer, Frank J. Kelly, Louisa Kramer, Ben Langford, Chun Lin, Alastair C. Lewis, Jie Li, Weijun Li, Huan Liu, Junfeng Liu, Miranda Loh, Keding Lu, Franco Lucarelli, Graham Mann, Gordon McFiggans, Mark R. Miller, Graham Mills, Paul Monk, Eiko Nemitz, Fionna O'Connor, Bin Ouyang, Paul I. Palmer, Carl Percival, Olalekan Popoola, Claire Reeves, Andrew R. Rickard, Longyi Shao, Guangyu Shi, Dominick Spracklen, David Stevenson, Yele Sun, Zhiwei Sun, Shu Tao, Shengrui Tong, Qingqing Wang, Wenhua Wang, Xinming Wang, Xuejun Wang, Zifang Wang, Lianfang Wei, Lisa Whalley, Xuefang Wu, Zhijun Wu, Pinhua Xie, Fumo Yang, Qiang Zhang, Yanli Zhang, Yuanhang Zhang, and Mei Zheng
Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, https://doi.org/10.5194/acp-19-7519-2019, 2019
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APHH-Beijing is a collaborative international research programme to study the sources, processes and health effects of air pollution in Beijing. This introduction to the special issue provides an overview of (i) the APHH-Beijing programme, (ii) the measurement and modelling activities performed as part of it and (iii) the air quality and meteorological conditions during joint intensive field campaigns as a core activity within APHH-Beijing.
Chunxiang Ye, Xianliang Zhou, Dennis Pu, Jochen Stutz, James Festa, Max Spolaor, Catalina Tsai, Christopher Cantrell, Roy L. Mauldin III, Andrew Weinheimer, Rebecca S. Hornbrook, Eric C. Apel, Alex Guenther, Lisa Kaser, Bin Yuan, Thomas Karl, Julie Haggerty, Samuel Hall, Kirk Ullmann, James Smith, and John Ortega
Atmos. Chem. Phys., 18, 9107–9120, https://doi.org/10.5194/acp-18-9107-2018, https://doi.org/10.5194/acp-18-9107-2018, 2018
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Substantial levels of HONO existed during the day throughout the troposphere over the southeastern US during NOMADSS 2013. Particulate nitrate photolysis appeared to be the major volume HONO source, while NOx was an important HONO precursor only in industrial and urban plumes. HONO was not a significant OH radical precursor in the rural troposphere away from the ground surface; however, its production from particulate nitrate photolysis was an important renoxification pathway.
Jacob T. Shaw, Richard T. Lidster, Danny R. Cryer, Noelia Ramirez, Fiona C. Whiting, Graham A. Boustead, Lisa K. Whalley, Trevor Ingham, Andrew R. Rickard, Rachel E. Dunmore, Dwayne E. Heard, Ally C. Lewis, Lucy J. Carpenter, Jacqui F. Hamilton, and Terry J. Dillon
Atmos. Chem. Phys., 18, 4039–4054, https://doi.org/10.5194/acp-18-4039-2018, https://doi.org/10.5194/acp-18-4039-2018, 2018
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The lifetime of a chemical in the atmosphere is largely governed by the rate of its reaction with the hydroxyl radical (OH). Measurements of rates for many of the thousands of identified volatile organic compounds (VOCs) have yet to be determined experimentally. We have developed a new technique for the rapid determination of gas-phase rate coefficients for the simultaneous reactions between multiple VOCs and OH. The method is tasted across a range of scenarios and is used to derive new values.
Daniel Stone, Tomás Sherwen, Mathew J. Evans, Stewart Vaughan, Trevor Ingham, Lisa K. Whalley, Peter M. Edwards, Katie A. Read, James D. Lee, Sarah J. Moller, Lucy J. Carpenter, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 3541–3561, https://doi.org/10.5194/acp-18-3541-2018, https://doi.org/10.5194/acp-18-3541-2018, 2018
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Halogen chemistry in the troposphere impacts oxidising capacity, but model studies assessing the nature of these impacts can vary according to the model framework used. In this work we present simulations of OH and HO2 radicals using both box and global model frameworks, and compare to observations made at the Cape Verde Atmospheric Observatory. We highlight, and rationalise, differences between the model frameworks.
Lisa K. Whalley, Daniel Stone, Rachel Dunmore, Jacqueline Hamilton, James R. Hopkins, James D. Lee, Alastair C. Lewis, Paul Williams, Jörg Kleffmann, Sebastian Laufs, Robert Woodward-Massey, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, https://doi.org/10.5194/acp-18-2547-2018, 2018
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This paper presents the first radical observations made in London and subsequent model comparisons. This work highlights that there are uncertainties in the degradation mechanism of complex biogenic and diesel-related VOC species under low-NOx conditions and under high-NOx conditions there is a missing source of RO2 radicals. The impact of these model uncertainties on in situ ozone production as a function of NOx is discussed.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Lavinia Onel, Alexander Brennan, Michele Gianella, Grace Ronnie, Ana Lawry Aguila, Gus Hancock, Lisa Whalley, Paul W. Seakins, Grant A. D. Ritchie, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 4877–4894, https://doi.org/10.5194/amt-10-4877-2017, https://doi.org/10.5194/amt-10-4877-2017, 2017
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Hydroperoxy (HO2) radicals are key intermediates participating in a rapid chemical cycling at the centre of the tropospheric oxidation. Fluorescence assay by gas expansion (FAGE) technique is the most commonly used for the HO2 measurements in the atmosphere. However, FAGE is an indirect technique, requiring calibration. This work finds a good agreement between the indirect FAGE method and the direct cavity ring-down spectroscopy method and hence validates FAGE and the FAGE calibration method.
Lavinia Onel, Alexander Brennan, Paul W. Seakins, Lisa Whalley, and Dwayne E. Heard
Atmos. Meas. Tech., 10, 3985–4000, https://doi.org/10.5194/amt-10-3985-2017, https://doi.org/10.5194/amt-10-3985-2017, 2017
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Methyl peroxy (CH3O2) radicals are the most abundant organic peroxy radical species and are critical intermediates in rapid chemical cycling at the heart of tropospheric oxidation. Despite their importance, at present CH3O2 radicals are not specifically measured in the atmosphere by any direct or indirect method. This work presents a new method for the selective and sensitive detection of CH3O2 radicals and its use for the measurement of CH3O2 in the atmospheric simulation chamber HIRAC.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Birger Bohn, Dwayne E. Heard, Nikolaos Mihalopoulos, Christian Plass-Dülmer, Rainer Schmitt, and Lisa K. Whalley
Atmos. Meas. Tech., 9, 3455–3466, https://doi.org/10.5194/amt-9-3455-2016, https://doi.org/10.5194/amt-9-3455-2016, 2016
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Filter radiometers are instruments that quantify the rate of formation of excited oxygen atoms from photolysis of ozone in the atmosphere. The excited oxygen atoms are important for the atmospheric self-cleaning ability. The radiometers were characterised by measurements of their spectral response. Together with field comparisons with a reference instrument, the characterisations improved the performance. That will help to better understand atmospheric photochemistry in future research.
Daniel Stone, Lisa K. Whalley, Trevor Ingham, Peter M. Edwards, Danny R. Cryer, Charlotte A. Brumby, Paul W. Seakins, and Dwayne E. Heard
Atmos. Meas. Tech., 9, 2827–2844, https://doi.org/10.5194/amt-9-2827-2016, https://doi.org/10.5194/amt-9-2827-2016, 2016
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OH reactivity is the total pseudo-first-order loss rate coefficient describing the removal of OH radicals to all sinks in the atmosphere. Measurements of ambient OH reactivity can be used to discover the extent to which measured OH sinks contribute to the total OH loss rate. In this work, we describe the design and characterisation of an instrument to measure OH reactivity using laser flash photolysis coupled to laser-induced fluorescence (LFP-LIF) spectroscopy.
Chris Reed, Charlotte A. Brumby, Leigh R. Crilley, Louisa J. Kramer, William J. Bloss, Paul W. Seakins, James D. Lee, and Lucy J. Carpenter
Atmos. Meas. Tech., 9, 2483–2495, https://doi.org/10.5194/amt-9-2483-2016, https://doi.org/10.5194/amt-9-2483-2016, 2016
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A new method of measuring nitrous acid (HONO), a potent mediator of air quality in the atmosphere as well as an important indoor pollutant, is presented. The new method relies on simple, proven techniques already widely applied to other atmospheric compounds. The technique can be retrofitted to existing analysers at minimal cost, or developed into instruments capable of very fast measurement which allow for more complex analysis of the behaviour of HONO.
Frank A. F. Winiberg, Terry J. Dillon, Stephanie C. Orr, Christoph B. M Groß, Iustinian Bejan, Charlotte A. Brumby, Matthew J. Evans, Shona C. Smith, Dwayne E. Heard, and Paul W. Seakins
Atmos. Chem. Phys., 16, 4023–4042, https://doi.org/10.5194/acp-16-4023-2016, https://doi.org/10.5194/acp-16-4023-2016, 2016
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OH radicals are important intermediates in the atmosphere, and the high concentrations observed in tropical regions are yet to be fully explained. Radical-radical reactions such as the title reaction can contribute to OH formation. This is the most fully comprehensive study of the CH3C(O)O2 + HO2 reaction with direct observation of products in all reaction channels. The implications of the new measurements on OH, PAN and NOx concentrations are considered via global models.
J. D. Lee, L. K. Whalley, D. E. Heard, D. Stone, R. E. Dunmore, J. F. Hamilton, D. E. Young, J. D. Allan, S. Laufs, and J. Kleffmann
Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, https://doi.org/10.5194/acp-16-2747-2016, 2016
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This paper presents field measurements of HONO and a range of other gas phase and particulate species from an urban background site in London. The measured daytime HONO cannot be reproduced with a simple box model and thus a significant daytime missing source of HONO is present. We show that this missing source could be responsible for 40 % of the OH radical source and 57 % of the OH initiation; hence its potential importance for atmospheric oxidation and ozone production.
Lisa K. Whalley, Daniel Stone, Brian Bandy, Rachel Dunmore, Jacqueline F. Hamilton, James Hopkins, James D. Lee, Alastair C. Lewis, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, https://doi.org/10.5194/acp-16-2109-2016, 2016
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
L. K. Whalley, D. Stone, I. J. George, S. Mertes, D. van Pinxteren, A. Tilgner, H. Herrmann, M. J. Evans, and D. E. Heard
Atmos. Chem. Phys., 15, 3289–3301, https://doi.org/10.5194/acp-15-3289-2015, https://doi.org/10.5194/acp-15-3289-2015, 2015
F. A. F. Winiberg, S. C. Smith, I. Bejan, C. A. Brumby, T. Ingham, T. L. Malkin, S. C. Orr, D. E. Heard, and P. W. Seakins
Atmos. Meas. Tech., 8, 523–540, https://doi.org/10.5194/amt-8-523-2015, https://doi.org/10.5194/amt-8-523-2015, 2015
P. S. J. Matthews, M. T. Baeza-Romero, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 14, 7397–7408, https://doi.org/10.5194/acp-14-7397-2014, https://doi.org/10.5194/acp-14-7397-2014, 2014
D. Stone, M. J. Evans, H. Walker, T. Ingham, S. Vaughan, B. Ouyang, O. J. Kennedy, M. W. McLeod, R. L. Jones, J. Hopkins, S. Punjabi, R. Lidster, J. F. Hamilton, J. D. Lee, A. C. Lewis, L. J. Carpenter, G. Forster, D. E. Oram, C. E. Reeves, S. Bauguitte, W. Morgan, H. Coe, E. Aruffo, C. Dari-Salisburgo, F. Giammaria, P. Di Carlo, and D. E. Heard
Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, https://doi.org/10.5194/acp-14-1299-2014, 2014
L. K. Whalley, M. A. Blitz, M. Desservettaz, P. W. Seakins, and D. E. Heard
Atmos. Meas. Tech., 6, 3425–3440, https://doi.org/10.5194/amt-6-3425-2013, https://doi.org/10.5194/amt-6-3425-2013, 2013
P. M. Edwards, M. J. Evans, K. L. Furneaux, J. Hopkins, T. Ingham, C. Jones, J. D. Lee, A. C. Lewis, S. J. Moller, D. Stone, L. K. Whalley, and D. E. Heard
Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, https://doi.org/10.5194/acp-13-9497-2013, 2013
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
Related subject area
Subject: Gases | Technique: In Situ Measurement | Topic: Instruments and Platforms
Deployment and evaluation of an NH4+∕ H3O+ reagent ion switching chemical ionization mass spectrometer for the detection of reduced and oxygenated gas-phase organic compounds
An economical tunable diode laser spectrometer for fast-response measurements of water vapor in the atmospheric boundary layer
Eddy covariance with slow-response greenhouse gas analysers on tall towers: bridging atmospheric and ecosystem greenhouse gas networks
Development of a portable laser-flash photolysis Faraday rotation spectrometer for measuring atmospheric total OH reactivity
An overview of outdoor low-cost gas-phase air quality sensor deployments: current efforts, trends, and limitations
Multiphysical description of atmospheric pressure interface chemical ionisation in MION2 and Eisele type inlets
A portable nitrogen dioxide instrument using cavity-enhanced absorption spectroscopy
Development and deployment of a mid-cost CO2 sensor monitoring network to support atmospheric inverse modeling for quantifying urban CO2 emissions in Paris
UAV-based in situ measurements of CO2 and CH4 fluxes over complex natural ecosystems
Advances in OH reactivity instruments for airborne field measurements
A new aerial approach for quantifying and attributing methane emissions: implementation and validation
Vertical profiles and surface distributions of trace gases (CO, O3, NO, NO2) in the Arctic wintertime boundary layer using low-cost sensors during ALPACA-2022
Drone CO2 measurements during the Tajogaite volcanic eruption
Multi-decadal atmospheric carbon dioxide measurements in Hungary, central Europe
Reliable water vapour isotopic composition measurements at low humidity using frequency-stabilised cavity ring-down spectroscopy
A measurement system for CO2 and CH4 emissions quantification of industrial sites using a new in situ concentration sensor operated on board uncrewed aircraft vehicles
Using metal oxide gas sensors to estimate the emission rates and locations of methane leaks in an industrial site: assessment with controlled methane releases
The ASK-16 Motorized Glider: An Airborne Eddy Covariance Platform to measure Turbulence, Energy and Matter Fluxes
Toward on-demand measurements of greenhouse gas emissions using an uncrewed aircraft AirCore system
Long-term evaluation of commercial air quality sensors: an overview from the QUANT (Quantification of Utility of Atmospheric Network Technologies) study
In-flight characterization of a compact airborne quantum cascade laser absorption spectrometer
Full characterization and calibration of a transfer standard monitor for atmospheric radon measurements
Observing low-altitude features in ozone concentrations in a shoreline environment via uncrewed aerial systems
Development of a Peltier-based chilled-mirror hygrometer for tropospheric and lower stratospheric water vapor measurements
An integrated uncrewed aerial vehicle platform with sensing and sampling systems for the measurement of air pollutant concentrations
Design and evaluation of a low-cost sensor node for near-background methane measurement
Development of a Multichannel Organics In situ enviRonmental Analyzer (MOIRA) for mobile measurements of volatile organic compounds
Evaluation of Aeris mid-infrared absorption (MIRA), Picarro CRDS (cavity ring-down spectroscopy) G2307, and dinitrophenylhydrazine (DNPH)-based sampling for long-term formaldehyde monitoring efforts
Performance characterization of a laminar gas inlet
Validation and field application of a low-cost device to measure CO2 and evapotranspiration (ET) fluxes
Identifying and correcting interferences to PTR-ToF-MS measurements of isoprene and other urban volatile organic compounds
Development of a continuous UAV-mounted air sampler and application to the quantification of CO2 and CH4 emissions from a major coking plant
Uptake behavior of polycyclic aromatic compounds during field calibrations of the XAD-based passive air sampler across seasons and locations
Effect of land–sea air mass transport on spatiotemporal distributions of atmospheric CO2 and CH4 mixing ratios over the southern Yellow Sea
HYPHOP: a tool for high-altitude, long-range monitoring of hydrogen peroxide and higher organic peroxides in the atmosphere
Portable, low-cost samplers for distributed sampling of atmospheric gases
SI-traceable validation of a laser spectrometer for balloon-borne measurements of water vapor in the upper atmosphere
Field evaluation of low-cost electrochemical air quality gas sensors under extreme temperature and relative humidity conditions
A novel, cost-effective analytical method for measuring high-resolution vertical profiles of stratospheric trace gases using a gas chromatograph coupled with an electron capture detector
Ethylene oxide monitor with part-per-trillion precision for in situ measurements
Development of an automated pump-efficiency measuring system for ozonesondes utilizing an airbag-type flowmeter
Short-term variability of atmospheric helium revealed through a cryo-enrichment method
Using tunable infrared laser direct absorption spectroscopy for ambient hydrogen chloride detection: HCl-TILDAS
New methods for the calibration of optical resonators: integrated calibration by means of optical modulation (ICOM) and narrow-band cavity ring-down (NB-CRD)
A modular field system for near-surface, vertical profiling of the atmospheric composition in harsh environments using cavity ring-down spectroscopy
Field comparison of two novel open-path instruments that measure dry deposition and emission of ammonia using flux-gradient and eddy covariance methods
Development of multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle for investigating volatile organic compounds' vertical distribution in the planetary boundary layer
Electrochemical sensors on board a Zeppelin NT: in-flight evaluation of low-cost trace gas measurements
Evaluating the performance of a Picarro G2207-i analyser for high-precision atmospheric O2 measurements
Airborne flux measurements of ammonia over the southern Great Plains using chemical ionization mass spectrometry
Cort L. Zang and Megan D. Willis
Atmos. Meas. Tech., 18, 17–35, https://doi.org/10.5194/amt-18-17-2025, https://doi.org/10.5194/amt-18-17-2025, 2025
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Atmospheric chemistry of the diverse pool of reactive organic carbon (ROC; all organic species excluding methane) controls air quality, both indoors and outdoors, and influences Earth's climate. However, many important ROC compounds in the atmosphere are difficult to measure. We demonstrate measurement of diverse ROC compounds in a single instrument at a forested site. This approach can improve our ability to measure a broad range of atmospheric ROC.
Emily D. Wein, Lars E. Kalnajs, and Darin W. Toohey
Atmos. Meas. Tech., 17, 7097–7107, https://doi.org/10.5194/amt-17-7097-2024, https://doi.org/10.5194/amt-17-7097-2024, 2024
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We describe a low-cost and small research-grade spectrometer for measurements of water vapor in the boundary layer. The instrument uses small Arduino microcontrollers and inexpensive laser diodes to reduce cost while maintaining high performance comparable to more expensive instruments. Performance was assessed with intercomparisons between commercially available instruments outdoors. The design's simplicity, performance, and price point allow it to be accessible to a variety of users.
Pedro Henrique Herig Coimbra, Benjamin Loubet, Olivier Laurent, Laura Bignotti, Mathis Lozano, and Michel Ramonet
Atmos. Meas. Tech., 17, 6625–6645, https://doi.org/10.5194/amt-17-6625-2024, https://doi.org/10.5194/amt-17-6625-2024, 2024
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This study presents direct flux measurements in tall towers using existing slow-response analysers and adding 3D sonic anemometers. This way, we can significantly improve greenhouse gas monitoring with little extra instrumental effort. Slow-response analysers may be used here as the relevant frequency ranges depend on measuring height. Tall towers offer a large footprint, amplifying spatial coverage. The presented concept is a valuable bridge between atmospheric and ecosystem communities.
Bo Fang, Nana Wei, Weixiong Zhao, Nana Yang, Hao Zhou, Heng Zhang, Jiarong Li, Weijun Zhang, Yanyu Lu, Zhu Zhu, and Yue Liu
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-184, https://doi.org/10.5194/amt-2024-184, 2024
Revised manuscript accepted for AMT
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A portable LP-FRS instrument with dimensions of 130 cm × 40 cm × 35 cm was developed. A specific pump-probe MPC was designed to offer a high overlapping factor of 75.4 %. The precision and uncertainty of the LP-FRS instrument for measuring kOH' were 1.0 s-1 (1σ, 300 s) and within 2 s-1, respectively. The developed portable LP-FRS instrument expands the measurement capabilities for atmospheric total OH reactivity and will be employed in more field observations.
Kristen Okorn and Laura T. Iraci
Atmos. Meas. Tech., 17, 6425–6457, https://doi.org/10.5194/amt-17-6425-2024, https://doi.org/10.5194/amt-17-6425-2024, 2024
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We reviewed 60 sensor networks and 17 related efforts (sensor review papers and data accessibility projects) to better understand the landscape of stationary low-cost gas-phase sensor networks deployed in outdoor environments worldwide. Gaps in monitoring efforts include the availability of gas-phase measurements compared to particulate matter (PM) and geographic coverage gaps (the Global South, rural areas). We conclude with a summary of cross-network unification and quality control efforts.
Henning Finkenzeller, Jyri Mikkilä, Cecilia Righi, Paxton Juuti, Mikko Sipilä, Matti Rissanen, Douglas Worsnop, Aleksei Shcherbinin, Nina Sarnela, and Juha Kangasluoma
Atmos. Meas. Tech., 17, 5989–6001, https://doi.org/10.5194/amt-17-5989-2024, https://doi.org/10.5194/amt-17-5989-2024, 2024
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Chemical ionisation mass spectrometry is used in the atmospheric sciences to measure trace gas concentrations. Neutral gases require charging in inlets before the mass-to-charge ratio of the resulting ions can be analysed. This study uses multiphysics modelling to investigate how the MION2 and Eisele type inlets work and shows the effect of tuning parameters and their current limitations. The findings are helpful for inlet users and are expected to aid in developing improved inlets.
Steven A. Bailey, Reem A. Hannun, Andrew K. Swanson, and Thomas F. Hanisco
Atmos. Meas. Tech., 17, 5903–5910, https://doi.org/10.5194/amt-17-5903-2024, https://doi.org/10.5194/amt-17-5903-2024, 2024
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We have developed a portable, optically based instrument that measures NO2. It consumes less than 6 W of power, so it can easily run off a small battery. This instrument has made both balloon and UAV flights. NO2 measurement results compare favorably with other known NO2 instruments. We find this instrument to be stable with repeatable results compared with calibration sources. Material cost to build a single instrument is around USD 4000. This could be lowered with economies of scale.
Jinghui Lian, Olivier Laurent, Mali Chariot, Luc Lienhardt, Michel Ramonet, Hervé Utard, Thomas Lauvaux, François-Marie Bréon, Grégoire Broquet, Karina Cucchi, Laurent Millair, and Philippe Ciais
Atmos. Meas. Tech., 17, 5821–5839, https://doi.org/10.5194/amt-17-5821-2024, https://doi.org/10.5194/amt-17-5821-2024, 2024
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We have designed and deployed a mid-cost medium-precision CO2 sensor monitoring network in Paris since July 2020. The data are automatically calibrated by a newly implemented data processing system. The accuracies of the mid-cost instruments vary from 1.0 to 2.4 ppm for hourly afternoon measurements. Our model–data analyses highlight prospects for integrating mid-cost instrument data with high-precision measurements to improve fine-scale CO2 emission quantification in urban areas.
Abdullah Bolek, Martin Heimann, and Mathias Göckede
Atmos. Meas. Tech., 17, 5619–5636, https://doi.org/10.5194/amt-17-5619-2024, https://doi.org/10.5194/amt-17-5619-2024, 2024
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This study describes the development of a new UAV platform to measure atmospheric greenhouse gas (GHG) mole fractions, 2D wind speed, air temperature, humidity, and pressure. Understanding GHG flux processes and controls across various ecosystems is essential for estimating the current and future state of climate change. It was shown that using the UAV platform for such measurements is beneficial for improving our understanding of GHG processes over complex landscapes.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
EGUsphere, https://doi.org/10.5194/egusphere-2024-2752, https://doi.org/10.5194/egusphere-2024-2752, 2024
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Jonathan F. Dooley, Kenneth Minschwaner, Manvendra K. Dubey, Sahar H. El Abbadi, Evan D. Sherwin, Aaron G. Meyer, Emily Follansbee, and James E. Lee
Atmos. Meas. Tech., 17, 5091–5111, https://doi.org/10.5194/amt-17-5091-2024, https://doi.org/10.5194/amt-17-5091-2024, 2024
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Methane is a powerful greenhouse gas originating from both natural and human activities. We describe a new uncrewed aerial system (UAS) designed to measure methane emission rates over a wide range of scales. This system has been used for direct quantification of point sources and distributed emitters over scales of up to 1 km. The system uses simultaneous measurements of methane and ethane to distinguish between different kinds of natural and human-related emission sources.
Brice Barret, Patrice Medina, Natalie Brett, Roman Pohorsky, Kathy Law, Slimane Bekki, Gilberto J. Fochesatto, Julia Schmale, Steve Arnold, Andrea Baccarini, Mauricio Busetto, Meeta Cesler-Maloney, Barbara D'Anna, Stefano Decesari, Jingqiu Mao, Gianluca Pappaccogli, Joel Savarino, Federico Scoto, and William R. Simpson
EGUsphere, https://doi.org/10.5194/egusphere-2024-2421, https://doi.org/10.5194/egusphere-2024-2421, 2024
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The Fairbanks area experiences severe pollution episodes in winter because of enhanced emissions of pollutants trapped near the surface by strong temperature inversions. Low-cost sensors were deployed onboard a car and a tethered balloon to measure the concentrations of gaseous pollutants (CO, O3, NOx) in Fairbanks during the winter of 2022. Data calibration with reference measurements and machine learning methods enabled to document pollution at the surface and power plant plumes aloft.
John Ericksen, Tobias P. Fischer, G. Matthew Fricke, Scott Nowicki, Nemesio M. Pérez, Pedro Hernández Pérez, Eleazar Padrón González, and Melanie E. Moses
Atmos. Meas. Tech., 17, 4725–4736, https://doi.org/10.5194/amt-17-4725-2024, https://doi.org/10.5194/amt-17-4725-2024, 2024
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Volcanic eruptions emit significant quantities of carbon dioxide (CO2) to the atmosphere. We present a new method for directly determining the CO2 emission from a volcanic eruption on the island of La Palma, Spain, using an unpiloted aerial vehicle (UAV). We also collected samples of the emitted CO2 and analyzed their isotopic composition. Together with the emission rate the isotopic data provide valuable information on the state of volcanic activity and the potential evolution of the eruption.
László Haszpra
Atmos. Meas. Tech., 17, 4629–4647, https://doi.org/10.5194/amt-17-4629-2024, https://doi.org/10.5194/amt-17-4629-2024, 2024
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The paper evaluates a 30-year-long atmospheric CO2 data series from a mid-continental central European site, Hegyhátsál (HUN). It presents the site-specific features observed in the long-term evolution of the atmospheric CO2 concentration. Since the measurement data are widely used in atmospheric inverse models and budget calculations all around the world, the paper provides potentially valuable information for model tuning and interpretation of the model results.
Mathieu Casado, Amaelle Landais, Tim Stoltmann, Justin Chaillot, Mathieu Daëron, Fréderic Prié, Baptiste Bordet, and Samir Kassi
Atmos. Meas. Tech., 17, 4599–4612, https://doi.org/10.5194/amt-17-4599-2024, https://doi.org/10.5194/amt-17-4599-2024, 2024
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Measuring water isotopic composition in Antarctica is difficult because of the extremely cold temperature in winter. Here, we designed a new infrared spectrometer able to measure the vapour isotopic composition during more than 95 % of the year in the coldest locations of Antarctica, whereas current commercial instruments are only able to measure during the warm summer months in the interior.
Jean-Louis Bonne, Ludovic Donnat, Grégory Albora, Jérémie Burgalat, Nicolas Chauvin, Delphine Combaz, Julien Cousin, Thomas Decarpenterie, Olivier Duclaux, Nicolas Dumelié, Nicolas Galas, Catherine Juery, Florian Parent, Florent Pineau, Abel Maunoury, Olivier Ventre, Marie-France Bénassy, and Lilian Joly
Atmos. Meas. Tech., 17, 4471–4491, https://doi.org/10.5194/amt-17-4471-2024, https://doi.org/10.5194/amt-17-4471-2024, 2024
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We present a top-down approach to quantify CO2 and CH4 emissions at the scale of an industrial site, based on a mass balance model relying on atmospheric concentrations measurements from a new sensor embarked on board uncrewed aircraft vehicles (UAVs). We present a laboratory characterization of our sensor and a field validation of our quantification method, together with field application to the monitoring of two real-world offshore oil and gas platforms.
Rodrigo Rivera-Martinez, Pramod Kumar, Olivier Laurent, Gregoire Broquet, Christopher Caldow, Ford Cropley, Diego Santaren, Adil Shah, Cécile Mallet, Michel Ramonet, Leonard Rivier, Catherine Juery, Olivier Duclaux, Caroline Bouchet, Elisa Allegrini, Hervé Utard, and Philippe Ciais
Atmos. Meas. Tech., 17, 4257–4290, https://doi.org/10.5194/amt-17-4257-2024, https://doi.org/10.5194/amt-17-4257-2024, 2024
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We explore the use of metal oxide semiconductors (MOSs) as a low-cost alternative for detecting and measuring CH4 emissions from industrial facilities. MOSs were exposed to several controlled releases to test their accuracy in detecting and quantifying emissions. Two reconstruction models were compared, and emission estimates were computed using a Gaussian dispersion model. Findings show that MOSs can provide accurate emission estimates with a 25 % emission rate error and a 9.5 m location error.
Inge Wiekenkamp, Anna Katharina Lehmann, Alexander Bütow, Jörg Hartmann, Stefan Metzger, Thomas Ruhtz, Christian Wille, Mathias Zöllner, and Torsten Sachs
EGUsphere, https://doi.org/10.5194/egusphere-2024-1586, https://doi.org/10.5194/egusphere-2024-1586, 2024
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Airborne eddy covariance platforms are crucial, as they measure the three-dimension wind, and turbulent transport of matter and energy between the surface and the atmosphere at larger scales. In this study we introduce the new ASK-16 eddy covariance platform that is able to accurately measure turbulent fluxes and wind vectors. Data from this platform can help to build bridges between local tower measurements and regional remote sensing fluxes or inversion products.
Zihan Zhu, Javier González-Rocha, Yifan Ding, Isis Frausto-Vicencio, Sajjan Heerah, Akula Venkatram, Manvendra Dubey, Don Collins, and Francesca M. Hopkins
Atmos. Meas. Tech., 17, 3883–3895, https://doi.org/10.5194/amt-17-3883-2024, https://doi.org/10.5194/amt-17-3883-2024, 2024
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Increases in agriculture, oil and gas, and waste management activities have contributed to the increase in atmospheric methane levels and resultant climate warming. In this paper, we explore the use of small uncrewed aircraft systems (sUASs) and AirCore technology to detect and quantify methane emissions. Results from field experiments demonstrate that sUASs and AirCore technology can be effective for detecting and quantifying methane emissions in near real time.
Sebastian Diez, Stuart Lacy, Hugh Coe, Josefina Urquiza, Max Priestman, Michael Flynn, Nicholas Marsden, Nicholas A. Martin, Stefan Gillott, Thomas Bannan, and Pete M. Edwards
Atmos. Meas. Tech., 17, 3809–3827, https://doi.org/10.5194/amt-17-3809-2024, https://doi.org/10.5194/amt-17-3809-2024, 2024
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In this paper we present an overview of the QUANT project, which to our knowledge is one of the largest evaluations of commercial sensors to date. The objective was to evaluate the performance of a range of commercial products and also to nourish the different applications in which these technologies can offer relevant information.
Linda Ort, Lenard Lukas Röder, Uwe Parchatka, Rainer Königstedt, Daniel Crowley, Frank Kunz, Ralf Wittkowski, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 17, 3553–3565, https://doi.org/10.5194/amt-17-3553-2024, https://doi.org/10.5194/amt-17-3553-2024, 2024
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Airborne in situ measurements are of great importance to collect valuable data to improve our knowledge of the atmosphere but also present challenges which demand specific designs. This study presents an IR spectrometer for airborne trace-gas measurements with high data efficiency and a simple, compact design. Its in-flight performance is characterized with the help of a test flight and a comparison with another spectrometer. Moreover, results from its first campaign highlight its benefits.
Roger Curcoll, Claudia Grossi, Stefan Röttger, and Arturo Vargas
Atmos. Meas. Tech., 17, 3047–3065, https://doi.org/10.5194/amt-17-3047-2024, https://doi.org/10.5194/amt-17-3047-2024, 2024
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This paper presents a new user-friendly version of the Atmospheric Radon MONitor (ARMON). The efficiency of the instrument is of 0.0057 s-1, obtained using different techniques at Spanish and German chambers. The total calculated uncertainty of the ARMON for hourly radon concentrations above 5 Bq m-3 is lower than 10 % (k = 1). Results confirm that the ARMON is suitable to measure low-level radon activity concentrations and to be used as a transfer standard to calibrate in situ radon monitors.
Josie K. Radtke, Benjamin N. Kies, Whitney A. Mottishaw, Sydney M. Zeuli, Aidan T. H. Voon, Kelly L. Koerber, Grant W. Petty, Michael P. Vermeuel, Timothy H. Bertram, Ankur R. Desai, Joseph P. Hupy, R. Bradley Pierce, Timothy J. Wagner, and Patricia A. Cleary
Atmos. Meas. Tech., 17, 2833–2847, https://doi.org/10.5194/amt-17-2833-2024, https://doi.org/10.5194/amt-17-2833-2024, 2024
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The use of uncrewed aircraft systems (UASs) to conduct a vertical profiling of ozone and meteorological variables was evaluated using comparisons between tower or ground observations and UAS-based measurements. Changes to the UAS profiler showed an improvement in performance. The profiler was used to see the impact of Chicago pollution plumes on a shoreline area near Lake Michigan.
Takuji Sugidachi, Masatomo Fujiwara, Kensaku Shimizu, Shin-Ya Ogino, Junko Suzuki, and Ruud J. Dirksen
EGUsphere, https://doi.org/10.5194/egusphere-2024-635, https://doi.org/10.5194/egusphere-2024-635, 2024
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A Peltier-based chilled-mirror hygrometer, SKYDEW, has been developed to measure tropospheric and stratospheric water vapor. Continuous accurate measurements of water vapor are essential for climate monitoring. More than 40 soundings with SKYDEW have been conducted since 2011 to evaluate the performance. The result of soundings at tropical and mid-latitudes demonstrated that SKYDEW is able to measure up to an altitude of 20–25 km for daytime soundings and above 25 km for nighttime soundings.
Chen-Wei Liang and Chang-Hung Shen
Atmos. Meas. Tech., 17, 2671–2686, https://doi.org/10.5194/amt-17-2671-2024, https://doi.org/10.5194/amt-17-2671-2024, 2024
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In the present study, a UAV platform with sensing and sampling systems was developed for 3D air pollutant concentration measurements. The sensing system of this platform contains multiple microsensors and IoT technologies for obtaining the real-time 3D distributions of critical air pollutants. The sampling system contains gas sampling sets and a 1 L Tedlar bag instead of a canister for the 3D measurement of VOC concentrations in accordance with the TO-15 method of the US EPA.
Daniel Furuta, Bruce Wilson, Albert A. Presto, and Jiayu Li
Atmos. Meas. Tech., 17, 2103–2121, https://doi.org/10.5194/amt-17-2103-2024, https://doi.org/10.5194/amt-17-2103-2024, 2024
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Methane is an important driver of climate change and is challenging to inexpensively sense in low atmospheric concentrations. We developed a low-cost sensor to monitor methane and tested it in indoor and outdoor settings. Our device shows promise for monitoring low levels of methane. We characterize its limitations and suggest future research directions for further development.
Audrey J. Dang, Nathan M. Kreisberg, Tyler L. Cargill, Jhao-Hong Chen, Sydney Hornitschek, Remy Hutheesing, Jay R. Turner, and Brent J. Williams
Atmos. Meas. Tech., 17, 2067–2087, https://doi.org/10.5194/amt-17-2067-2024, https://doi.org/10.5194/amt-17-2067-2024, 2024
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The Multichannel Organics In situ enviRonmental Analyzer (MOIRA) is a new instrument for measuring speciated volatile organic compounds (VOCs) in the air and has been developed for mapping concentrations from a hybrid car. MOIRA is characterized in the lab and pilot field studies of indoor air in a single-family residence and outdoor air during a mobile deployment. Future applications include indoor, outdoor, and lab measurements to grasp the impact of VOCs on air quality, health, and climate.
Asher P. Mouat, Zelda A. Siegel, and Jennifer Kaiser
Atmos. Meas. Tech., 17, 1979–1994, https://doi.org/10.5194/amt-17-1979-2024, https://doi.org/10.5194/amt-17-1979-2024, 2024
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Three fast-measurement formaldehyde monitors were deployed at two field sites in Atlanta, GA, over 1 year. Four different zeroing methods were tested to develop an optimal field setup as well as procedures for instrument calibration. Observations agreed well after calibration but were much higher compared to the TO-11A monitoring method, which is the golden standard. Historical HCHO concentrations were compared with measurements in this work, showing a 22 % reduction in midday HCHO since 1999.
Da Yang, Margarita Reza, Roy Mauldin, Rainer Volkamer, and Suresh Dhaniyala
Atmos. Meas. Tech., 17, 1463–1474, https://doi.org/10.5194/amt-17-1463-2024, https://doi.org/10.5194/amt-17-1463-2024, 2024
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This paper evaluates the performance of an aircraft gas inlet. Here, we use computational fluid dynamics (CFD) and experiments to demonstrate the role of turbulence in determining sampling performance of a gas inlet and identify ideal conditions for inlet operation to minimize gas loss. Experiments conducted in a high-speed wind tunnel under near-aircraft speeds validated numerical results. We believe that the results obtained from this work will greatly inform future gas inlet studies.
Reena Macagga, Michael Asante, Geoffroy Sossa, Danica Antonijević, Maren Dubbert, and Mathias Hoffmann
Atmos. Meas. Tech., 17, 1317–1332, https://doi.org/10.5194/amt-17-1317-2024, https://doi.org/10.5194/amt-17-1317-2024, 2024
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Using only low-cost microcontrollers and sensors, we constructed a measurement device to accurately and precisely obtain atmospheric carbon dioxide and water fluxes. The device was tested against known concentration increases and high-cost, commercial sensors during a laboratory and field experiment. We additionally tested the device over a longer period in a field study in Ghana during which the net ecosystem carbon balance and water use efficiency of maize cultivation were studied.
Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Lu Xu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
Atmos. Meas. Tech., 17, 801–825, https://doi.org/10.5194/amt-17-801-2024, https://doi.org/10.5194/amt-17-801-2024, 2024
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Mass spectrometry is a tool commonly used to measure air pollutants. This study evaluates measurement artifacts produced in the proton-transfer-reaction mass spectrometer. We provide methods to correct these biases and better measure compounds that degrade air quality.
Tianran Han, Conghui Xie, Yayong Liu, Yanrong Yang, Yuheng Zhang, Yufei Huang, Xiangyu Gao, Xiaohua Zhang, Fangmin Bao, and Shao-Meng Li
Atmos. Meas. Tech., 17, 677–691, https://doi.org/10.5194/amt-17-677-2024, https://doi.org/10.5194/amt-17-677-2024, 2024
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This study reported an integrated UAV measurement platform for GHG monitoring and its application for emission quantification from a coking plant. The key element of this system is a newly designed air sampler, consisting of a 150 m long tube with remote-controlled time stamping. When comparing the top-down results to those derived from the bottom-up inventory method, the present findings indicate that the use of IPCC emission factors for emission calculations can lead to overestimation.
Yuening Li, Faqiang Zhan, Yushan Su, Ying Duan Lei, Chubashini Shunthirasingham, Zilin Zhou, Jonathan P. D. Abbatt, Hayley Hung, and Frank Wania
Atmos. Meas. Tech., 17, 715–729, https://doi.org/10.5194/amt-17-715-2024, https://doi.org/10.5194/amt-17-715-2024, 2024
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A simple device for sampling gases from the atmosphere without the help of pumps was calibrated for an important group of hazardous air pollutants called polycyclic aromatic compounds (PACs). While the sampler appeared to perform well when used for relatively short periods of up to several months, some PACs were lost from the sampler during longer deployments. Sampling rates that can be used to quantitatively interpret the quantities of PACs taken up in the device have been derived.
Jiaxin Li, Kunpeng Zang, Yi Lin, Yuanyuan Chen, Shuo Liu, Shanshan Qiu, Kai Jiang, Xuemei Qing, Haoyu Xiong, Haixiang Hong, Shuangxi Fang, Honghui Xu, and Yujun Jiang
Atmos. Meas. Tech., 16, 4757–4768, https://doi.org/10.5194/amt-16-4757-2023, https://doi.org/10.5194/amt-16-4757-2023, 2023
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Based on observed data of CO2 and CH4 and meteorological parameters over the Yellow Sea in November 2012 and June 2013, a data process and quality control method was optimized and established to filter the data influenced by multiple factors. Spatial and seasonal variations in CO2 and CH4 mixing ratios were mainly controlled by the East Asian Monsoon, while the influence of air–sea exchange was slight.
Zaneta Hamryszczak, Antonia Hartmann, Dirk Dienhart, Sascha Hafermann, Bettina Brendel, Rainer Königstedt, Uwe Parchatka, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 16, 4741–4756, https://doi.org/10.5194/amt-16-4741-2023, https://doi.org/10.5194/amt-16-4741-2023, 2023
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Hydroperoxide measurements improve the understanding of atmospheric oxidation processes. We introduce an instrumental setup for airborne measurements. The aim of the work is the characterization of the measurement method with emphasis on interferences impacting instrumental uncertainty. Technical and physical challenges do not critically impact the instrumental performance. The instrument resolves dynamic processes, such as convective transport, as shown based on the CAFE-Brazil campaign.
James F. Hurley, Alejandra Caceres, Deborah F. McGlynn, Mary E. Tovillo, Suzanne Pinar, Roger Schürch, Ksenia Onufrieva, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4681–4692, https://doi.org/10.5194/amt-16-4681-2023, https://doi.org/10.5194/amt-16-4681-2023, 2023
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Volatile organic compounds (VOCs) have a wide range of sources and impacts on environments and human health that make them spatially, temporally, and chemically varied. Current methods lack the ability to collect samples in ways that provide spatial and chemical resolution without complex, costly instrumentation. We describe and validate a low-cost, portable VOC sampler and demonstrate its utility in collecting distributed coordinated samples.
Simone Brunamonti, Manuel Graf, Tobias Bühlmann, Céline Pascale, Ivan Ilak, Lukas Emmenegger, and Béla Tuzson
Atmos. Meas. Tech., 16, 4391–4407, https://doi.org/10.5194/amt-16-4391-2023, https://doi.org/10.5194/amt-16-4391-2023, 2023
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The abundance of water vapor (H2O) in the upper atmosphere has a significant impact on the rate of global warming. We developed a new lightweight spectrometer (ALBATROSS) for H2O measurements aboard meteorological balloons. Here, we assess the accuracy and precision of ALBATROSS using metrology-grade reference gases. The results demonstrate the exceptional potential of mid-infrared laser absorption spectroscopy as a new reference method for in situ measurements of H2O in the upper atmosphere.
Roubina Papaconstantinou, Marios Demosthenous, Spyros Bezantakos, Neoclis Hadjigeorgiou, Marinos Costi, Melina Stylianou, Elli Symeou, Chrysanthos Savvides, and George Biskos
Atmos. Meas. Tech., 16, 3313–3329, https://doi.org/10.5194/amt-16-3313-2023, https://doi.org/10.5194/amt-16-3313-2023, 2023
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In this paper, we investigate the performance of low-cost electrochemical gas sensors. We carried out yearlong measurements at a traffic air quality monitoring station, where the low-cost sensors were collocated with reference instruments and exposed to highly variable environmental conditions with extremely high temperatures and low relative humidity (RH). Sensors provide measurements that exhibit increasing errors and decreasing correlations as temperature increases and RH decreases.
Jianghanyang Li, Bianca C. Baier, Fred Moore, Tim Newberger, Sonja Wolter, Jack Higgs, Geoff Dutton, Eric Hintsa, Bradley Hall, and Colm Sweeney
Atmos. Meas. Tech., 16, 2851–2863, https://doi.org/10.5194/amt-16-2851-2023, https://doi.org/10.5194/amt-16-2851-2023, 2023
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Monitoring a suite of trace gases in the stratosphere will help us better understand the stratospheric circulation and its impact on the earth's radiation balance. However, such measurements are rare and usually expensive. We developed an instrument that can measure stratospheric trace gases using a low-cost sampling platform (AirCore). The results showed expected agreement with aircraft measurements, demonstrating this technique provides a low-cost and robust way to observe the stratosphere.
Tara I. Yacovitch, Christoph Dyroff, Joseph R. Roscioli, Conner Daube, J. Barry McManus, and Scott C. Herndon
Atmos. Meas. Tech., 16, 1915–1921, https://doi.org/10.5194/amt-16-1915-2023, https://doi.org/10.5194/amt-16-1915-2023, 2023
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Ethylene oxide is a toxic, carcinogenic compound used in the medical and bulk sterilization industry. Here we describe a precise and fast laser-based ethylene oxide monitor. We report months-long concentrations at a Massachusetts site, and we show how they suggest a potential emission source 35 km away. This source, and another, is confirmed by driving the instrument downwind of the sites, where concentrations were tens to tens of thousands of times greater than background levels.
Tatsumi Nakano and Takashi Morofuji
Atmos. Meas. Tech., 16, 1583–1595, https://doi.org/10.5194/amt-16-1583-2023, https://doi.org/10.5194/amt-16-1583-2023, 2023
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We have developed a system that can automatically measure the pump efficiency of the ECC-type ozonesonde. Operational measurement for 13 years by this system revealed that the efficiency fluctuates in each and slightly increases over time. Those can affect the estimation of total ozone amount by up to 4 %. This result indicates that it is necessary to understand the tendency of the pump correction factor of each ozonesonde in order to detect the actual atmospheric change with high accuracy.
Benjamin Birner, Eric Morgan, and Ralph F. Keeling
Atmos. Meas. Tech., 16, 1551–1561, https://doi.org/10.5194/amt-16-1551-2023, https://doi.org/10.5194/amt-16-1551-2023, 2023
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Atmospheric variations of helium (He) and CO2 are strongly linked due to the co-release of both gases from natural-gas burning. This implies that atmospheric He measurements may be a potentially powerful tool for verifying reported anthropogenic natural-gas usage. Here, we present the development and initial results of a novel measurement system of atmospheric He that paves the way for establishing a global monitoring network in the future.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
Henning Finkenzeller, Denis Pöhler, Martin Horbanski, Johannes Lampel, and Ulrich Platt
Atmos. Meas. Tech., 16, 1343–1356, https://doi.org/10.5194/amt-16-1343-2023, https://doi.org/10.5194/amt-16-1343-2023, 2023
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Optical resonators enhance the light path in compact instruments, thereby improving their sensitivity. Determining the established path length in the instrument is a prerequisite for the accurate determination of trace gas concentrations but can be a significant complication in the use of such resonators. Here we show two calibration techniques which are relatively simple and free of consumables but still provide accurate calibrations. This facilitates the use of optical resonators.
Andrew W. Seidl, Harald Sodemann, and Hans Christian Steen-Larsen
Atmos. Meas. Tech., 16, 769–790, https://doi.org/10.5194/amt-16-769-2023, https://doi.org/10.5194/amt-16-769-2023, 2023
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It is challenging to make field measurements of stable water isotopes in the Arctic. To this end, we present a modular stable-water-isotope analyzer profiling system. The system operated for a 2-week field campaign on Svalbard during the Arctic winter. We evaluate the system’s performance and analyze any potential impact that the field conditions might have had on the isotopic measurements and the system's ability to resolve isotope gradients in the lowermost layer of the atmosphere.
Daan Swart, Jun Zhang, Shelley van der Graaf, Susanna Rutledge-Jonker, Arjan Hensen, Stijn Berkhout, Pascal Wintjen, René van der Hoff, Marty Haaima, Arnoud Frumau, Pim van den Bulk, Ruben Schulte, Margreet van Zanten, and Thomas van Goethem
Atmos. Meas. Tech., 16, 529–546, https://doi.org/10.5194/amt-16-529-2023, https://doi.org/10.5194/amt-16-529-2023, 2023
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During a 5-week comparison campaign, we tested two set-ups to measure half hourly ammonia fluxes. The eddy covariance and flux gradient systems showed very similar results when the upwind terrain was both homogeneous and free of obstacles. We discuss the technical performance and practical limitations of both systems. Measurements from these instruments can facilitate the study of processes behind ammonia deposition, an important contributor to eutrophication and acidificationin natural areas.
Suding Yang, Xin Li, Limin Zeng, Xuena Yu, Ying Liu, Sihua Lu, Xiaofeng Huang, Dongmei Zhang, Haibin Xu, Shuchen Lin, Hefan Liu, Miao Feng, Danlin Song, Qinwen Tan, Jinhui Cui, Lifan Wang, Ying Chen, Wenjie Wang, Haijiong Sun, Mengdi Song, Liuwei Kong, Yi Liu, Linhui Wei, Xianwu Zhu, and Yuanhang Zhang
Atmos. Meas. Tech., 16, 501–512, https://doi.org/10.5194/amt-16-501-2023, https://doi.org/10.5194/amt-16-501-2023, 2023
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Vertical observation of volatile organic compounds (VOCs) is essential to study the spatial distribution and evolution patterns of VOCs in the planetary boundary layer (PBL). This paper describes multi-channel whole-air sampling equipment onboard an unmanned aerial vehicle (UAV) for near-continuous VOC vertical observation. Vertical profiles of VOCs and trace gases during the evolution of the PBL in south-western China have been successfully obtained by deploying the newly developed UAV system.
Tobias Schuldt, Georgios I. Gkatzelis, Christian Wesolek, Franz Rohrer, Benjamin Winter, Thomas A. J. Kuhlbusch, Astrid Kiendler-Scharr, and Ralf Tillmann
Atmos. Meas. Tech., 16, 373–386, https://doi.org/10.5194/amt-16-373-2023, https://doi.org/10.5194/amt-16-373-2023, 2023
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We report in situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin NT in Germany. We highlight the in-flight evaluation of electrochemical sensors that were installed inside a hatch box located on the bottom of the Zeppelin. Results from this work emphasize the potential of these sensors for other in situ airborne applications, e.g., on board unmanned aerial vehicles (UAVs).
Leigh S. Fleming, Andrew C. Manning, Penelope A. Pickers, Grant L. Forster, and Alex J. Etchells
Atmos. Meas. Tech., 16, 387–401, https://doi.org/10.5194/amt-16-387-2023, https://doi.org/10.5194/amt-16-387-2023, 2023
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Measurements of atmospheric O2 can help constrain the carbon cycle processes and quantify fossil fuel CO2 emissions; however, measurement of atmospheric O2 is very challenging, and existing analysers are complex systems to build and maintain. We have tested a new O2 analyser (Picarro Inc. G2207-i) in the laboratory and at Weybourne Atmospheric Observatory. We have found that the G2207-i does not perform as well as an existing O2 analyser from Sable Systems Inc.
Siegfried Schobesberger, Emma L. D'Ambro, Lejish Vettikkat, Ben H. Lee, Qiaoyun Peng, David M. Bell, John E. Shilling, Manish Shrivastava, Mikhail Pekour, Jerome Fast, and Joel A. Thornton
Atmos. Meas. Tech., 16, 247–271, https://doi.org/10.5194/amt-16-247-2023, https://doi.org/10.5194/amt-16-247-2023, 2023
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We present a new, highly sensitive technique for measuring atmospheric ammonia, an important trace gas that is emitted mainly by agriculture. We deployed the instrument on an aircraft during research flights over rural Oklahoma. Due to its fast response, we could analyze correlations with turbulent winds and calculate ammonia emissions from nearby areas at 1 to 2 km resolution. We observed high spatial variability and point sources that are not resolved in the US National Emissions Inventory.
Cited articles
Birdsall, A. W., Andreoni, J. F., and Elrod, M. J.: Investigation of the
role of bicyclic peroxy radicals in the oxidation mechanism of toluene,
J. Phys. Chem. A, 114, 10655–10663, https://doi.org/10.1021/jp105467e, 2010.
Bloss, W. J., Lee, J. D., Heard, D. E., Salmon, R. A., Bauguitte, S. J.-B., Roscoe, H. K., and Jones, A. E.: Observations of OH and HO2 radicals in coastal Antarctica, Atmos. Chem. Phys., 7, 4171–4185, https://doi.org/10.5194/acp-7-4171-2007, 2007.
Boggs, P. T., Byrd, R. H., and Schnabel, R. B.: A Stable and Efficient
Algorithm for Nonlinear Orthogonal Distance Regression,
Siam J. Sci. Stat. Comp., 8, 1052–1078, https://doi.org/10.1137/0908085, 1987.
Bohn, B., Corlett, G. K., Gillmann, M., Sanghavi, S., Stange, G., Tensing, E., Vrekoussis, M., Bloss, W. J., Clapp, L. J., Kortner, M., Dorn, H.-P., Monks, P. S., Platt, U., Plass-Dülmer, C., Mihalopoulos, N., Heard, D. E., Clemitshaw, K. C., Meixner, F. X., Prevot, A. S. H., and Schmitt, R.: Photolysis frequency measurement techniques: results of a comparison within the ACCENT project, Atmos. Chem. Phys., 8, 5373–5391, https://doi.org/10.5194/acp-8-5373-2008, 2008.
Brune, W. H., Baier, B. C., Thomas, J., Ren, X., Cohen, R. C., Pusede, S.
E., Browne, E. C., Goldstein, A. H., Gentner, D. R., Keutsch, F. N.,
Thornton, J. A., Harrold, S., Lopez-Hilfiker, F. D., and Wennberg, P. O.:
Ozone production chemistry in the presence of urban plumes, Faraday
Discuss., 189, 169–189, https://doi.org/10.1039/c5fd00204d, 2016.
Carslaw, N., Creasey, D. J., Harrison, D., Heard, D. E., Hunter, M. C.,
Jacobs, P. J., Jenkin, M. E., Lee, J. D., Lewis, A. C., Pilling, M. J.,
Saunders, S. M., and Seakins, P. W.: OH and HO2 radical chemistry in a
forested region of north-western Greece, Atmos. Environ., 35,
4725–4737, https://doi.org/10.1016/S1352-2310(01)00089-9, 2001.
Cazorla, M. and Brune, W. H.: Measurement of Ozone Production Sensor, Atmos. Meas. Tech., 3, 545–555, https://doi.org/10.5194/amt-3-545-2010, 2010.
Cazorla, M., Brune, W. H., Ren, X., and Lefer, B.: Direct measurement of ozone production rates in Houston in 2009 and comparison with two estimation methods, Atmos. Chem. Phys., 12, 1203–1212, https://doi.org/10.5194/acp-12-1203-2012, 2012.
Chao, W., Hsieh, J. T., Chang, C. H., and Lin, J. J.: Atmospheric chemistry.
Direct kinetic measurement of the reaction of the simplest Criegee
intermediate with water vapor, Science, 347, 751–754,
https://doi.org/10.1126/science.1261549, 2015.
Chen, W., Tang, H. Z., and Zhao, H. M.: Diurnal, weekly and monthly spatial
variations of air pollutants and air quality of Beijing, Atmos. Environ., 119, 21–34, https://doi.org/10.1016/j.atmosenv.2015.08.040, 2015.
Creasey, D. J., HalfordMaw, P. A., Heard, D. E., Pilling, M. J., and
Whitaker, B. J.: Implementation and initial deployment of a field instrument
for measurement of OH and HO2 in the troposphere by laser-induced
fluorescence, J. Chem. Soc.-Faraday T., 93,
2907–2913, https://doi.org/10.1039/a701469d, 1997a.
Creasey, D. J., Heard, D. E., Pilling, M. J., Whitaker, B. J., Berzins, M.,
and Fairlie, R.: Visualisation of a supersonic free-jet expansion using
laser-induced fluorescence spectroscopy: Application to the measurement of
rate constants at ultralow temperatures, Appl. Phys. B, 65, 375–391, https://doi.org/10.1007/s003400050285, 1997b.
Creasey, D. J., Heard, D. E., and Lee, J. D.: OH and HO2 measurements
in a forested region of north-western Greece, Atmos. Environ., 35,
4713–4724, https://doi.org/10.1016/S1352-2310(01)00090-5, 2001.
Creasey, D. J., Evans, G. E., Heard, D. E., and Lee, J. D.: Measurements of
OH and HO2 concentrations in the Southern Ocean marine boundary layer,
J. Geophys. Res.-Atmos., 108, 4475,
10.1029/2002JD003206, 2003.
Crounse, J. D., Paulot, F., Kjaergaard, H. G., and Wennberg, P. O.: Peroxy
radical isomerization in the oxidation of isoprene,
Phys. Chem. Chem. Phys., 13, 13607–13613, https://doi.org/10.1039/c1cp21330j, 2011.
Crounse, J. D., Knap, H. C., Ornso, K. B., Jorgensen, S., Paulot, F.,
Kjaergaard, H. G., and Wennberg, P. O.: Atmospheric fate of methacrolein. 1.
Peroxy radical isomerization following addition of OH and O2, J. Phys. Chem. A, 116, 5756–5762, https://doi.org/10.1021/jp211560u, 2012.
Cryer, D. R.: Measurements of hydroxyl radical reactivity and formaldehyde
in the atmosphere, PhD thesis, School of Chemistry, University of Leeds,
2016.
da Silva, G., Graham, C., and Wang, Z. F.: Unimolecular beta-hydroxyperoxy
radical decomposition with OH recycling in the photochemical oxidation of
isoprene, Environ. Sci. Technol., 44, 250–256,
https://doi.org/10.1021/es900924d, 2010.
Dillon, T. J. and Crowley, J. N.: Direct detection of OH formation in the reactions of HO2 with CH3C(O)O2 and other substituted peroxy radicals, Atmos. Chem. Phys., 8, 4877–4889, https://doi.org/10.5194/acp-8-4877-2008, 2008.
Dubey, M. K., Hanisco, T. F., Wennberg, P. O., and Anderson, J. G.:
Monitoring potential photochemical interference in laser-induced
fluorescence measurements of atmospheric OH, Geophys. Res. Lett.,
23, 3215–3218, https://doi.org/10.1029/96gl03008, 1996.
Dusanter, S., Vimal, D., Stevens, P. S., Volkamer, R., and Molina, L. T.: Measurements of OH and HO2 concentrations during the MCMA-2006 field campaign – Part 1: Deployment of the Indiana University laser-induced fluorescence instrument, Atmos. Chem. Phys., 9, 1665–1685, https://doi.org/10.5194/acp-9-1665-2009, 2009.
Edwards, G. D., Cantrell, C. A., Stephens, S., Hill, B., Goyea, O., Shetter,
R. E., Mauldin, R. L., Kosciuch, E., Tanner, D. J., and Eisele, F. L.:
Chemical ionization mass spectrometer instrument for the measurement of
tropospheric HO2 and RO2, Anal. Chem., 75, 5317–5327,
https://doi.org/10.1021/ac034402b, 2003.
Emmerson, K. M., Carslaw, N., Carslaw, D. C., Lee, J. D., McFiggans, G., Bloss, W. J., Gravestock, T., Heard, D. E., Hopkins, J., Ingham, T., Pilling, M. J., Smith, S. C., Jacob, M., and Monks, P. S.: Free radical modelling studies during the UK TORCH Campaign in Summer 2003, Atmos. Chem. Phys., 7, 167–181, https://doi.org/10.5194/acp-7-167-2007, 2007.
Faloona, I., Tan, D., Brune, W., Hurst, J., Barket, D., Couch, T. L.,
Shepson, P., Apel, E., Riemer, D., Thornberry, T., Carroll, M. A., Sillman,
S., Keeler, G. J., Sagady, J., Hooper, D., and Paterson, K.: Nighttime
observations of anomalously high levels of hydroxyl radicals above a
deciduous forest canopy, J. Geophys. Res.-Atmos., 106,
24315–24333, https://doi.org/10.1029/2000jd900691, 2001.
Faloona, I. C., Tan, D., Lesher, R. L., Hazen, N. L., Frame, C. L., Simpas,
J. B., Harder, H., Martinez, M., Di Carlo, P., Ren, X. R., and Brune, W. H.:
A laser-induced fluorescence instrument for detecting tropospheric OH and
HO2: Characteristics and calibration, J. Atmos. Chem.,
47, 139–167, https://doi.org/10.1023/B:JOCH.0000021036.53185.0e, 2004.
Feiner, P. A., Brune, W. H., Miller, D. O., Zhang, L., Cohen, R. C., Romer,
P. S., Goldstein, A. H., Keutsch, F. N., Skog, K. M., Wennberg, P. O.,
Nguyen, T. B., Teng, A. P., DeGouw, J., Koss, A., Wild, R. J., Brown, S. S.,
Guenther, A., Edgerton, E., Baumann, K., and Fry, J. L.: Testing Atmospheric
Oxidation in an Alabama Forest, J. Atmos. Sci., 73,
4699–4710, https://doi.org/10.1175/Jas-D-16-0044.1, 2016.
Fittschen, C., Al Ajami, M., Batut, S., Ferracci, V., Archer-Nicholls, S., Archibald, A. T., and Schoemaecker, C.: ROOOH: a missing piece of the puzzle for OH measurements in low-NO environments?, Atmos. Chem. Phys., 19, 349–362, https://doi.org/10.5194/acp-19-349-2019, 2019.
Fuchs, H., Holland, F., and Hofzumahaus, A.: Measurement of tropospheric
RO2 and HO2 radicals by a laser-induced fluorescence instrument,
Rev. Sci. Instrum., 79, 084104, https://doi.org/10.1063/1.2968712, 2008.
Fuchs, H., Bohn, B., Hofzumahaus, A., Holland, F., Lu, K. D., Nehr, S., Rohrer, F., and Wahner, A.: Detection of HO2 by laser-induced fluorescence: calibration and interferences from RO2 radicals, Atmos. Meas. Tech., 4, 1209–1225, https://doi.org/10.5194/amt-4-1209-2011, 2011.
Fuchs, H., Hofzumahaus, A., Rohrer, F., Bohn, B., Brauers, T., Dorn, H. P.,
Haseler, R., Holland, F., Kaminski, M., Li, X., Lu, K., Nehr, S., Tillmann,
R., Wegener, R., and Wahner, A.: Experimental evidence for efficient
hydroxyl radical regeneration in isoprene oxidation, Nat. Geosci., 6,
1023–1026, https://doi.org/10.1038/Ngeo1964, 2013.
Fuchs, H., Acir, I.-H., Bohn, B., Brauers, T., Dorn, H.-P., Häseler, R., Hofzumahaus, A., Holland, F., Kaminski, M., Li, X., Lu, K., Lutz, A., Nehr, S., Rohrer, F., Tillmann, R., Wegener, R., and Wahner, A.: OH regeneration from methacrolein oxidation investigated in the atmosphere simulation chamber SAPHIR, Atmos. Chem. Phys., 14, 7895–7908, https://doi.org/10.5194/acp-14-7895-2014, 2014.
Fuchs, H., Tan, Z., Hofzumahaus, A., Broch, S., Dorn, H.-P., Holland, F., Künstler, C., Gomm, S., Rohrer, F., Schrade, S., Tillmann, R., and Wahner, A.: Investigation of potential interferences in the detection of atmospheric ROx radicals by laser-induced fluorescence under dark conditions, Atmos. Meas. Tech., 9, 1431–1447, https://doi.org/10.5194/amt-9-1431-2016, 2016.
Fuchs, H., Tan, Z., Lu, K., Bohn, B., Broch, S., Brown, S. S., Dong, H., Gomm, S., Häseler, R., He, L., Hofzumahaus, A., Holland, F., Li, X., Liu, Y., Lu, S., Min, K.-E., Rohrer, F., Shao, M., Wang, B., Wang, M., Wu, Y., Zeng, L., Zhang, Y., Wahner, A., and Zhang, Y.: OH reactivity at a rural site (Wangdu) in the North China Plain: contributions from OH reactants and experimental OH budget, Atmos. Chem. Phys., 17, 645–661, https://doi.org/10.5194/acp-17-645-2017, 2017.
Fuchs, H., Albrecht, S., Acir, I., Bohn, B., Breitenlechner, M., Dorn, H.-P., Gkatzelis, G. I., Hofzumahaus, A., Holland, F., Kaminski, M., Keutsch, F. N., Novelli, A., Reimer, D., Rohrer, F., Tillmann, R., Vereecken, L., Wegener, R., Zaytsev, A., Kiendler-Scharr, A., and Wahner, A.: Investigation of the oxidation of methyl vinyl ketone (MVK) by OH radicals in the atmospheric simulation chamber SAPHIR, Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, 2018.
Griffith, S. M., Hansen, R. F., Dusanter, S., Stevens, P. S., Alaghmand, M., Bertman, S. B., Carroll, M. A., Erickson, M., Galloway, M., Grossberg, N., Hottle, J., Hou, J., Jobson, B. T., Kammrath, A., Keutsch, F. N., Lefer, B. L., Mielke, L. H., O'Brien, A., Shepson, P. B., Thurlow, M., Wallace, W., Zhang, N., and Zhou, X. L.: OH and HO2 radical chemistry during PROPHET 2008 and CABINEX 2009 – Part 1: Measurements and model comparison, Atmos. Chem. Phys., 13, 5403–5423, https://doi.org/10.5194/acp-13-5403-2013, 2013.
Griffith, S. M., Hansen, R. F., Dusanter, S., Michoud, V., Gilman, J. B.,
Kuster, W. C., Veres, P. R., Graus, M., de Gouw, J. A., Roberts, J., Young,
C., Washenfelder, R., Brown, S. S., Thalman, R., Waxman, E., Volkamer, R.,
Tsai, C., Stutz, J., Flynn, J. H., Grossberg, N., Lefer, B., Alvarez, S. L.,
Rappenglueck, B., Mielke, L. H., Osthoff, H. D., and Stevens, P. S.:
Measurements of hydroxyl and hydroperoxy radicals during CalNex-LA: Model
comparisons and radical budgets, J. Geophys. Res.-Atmos., 121, 4211–4232, https://doi.org/10.1002/2015jd024358, 2016.
Hansen, R. F., Lewis, T. R., Graham, L., Whalley, L. K., Seakins, P. W.,
Heard, D. E., and Blitz, M. A.: OH production from the photolysis of
isoprene-derived peroxy radicals: cross-sections, quantum yields and
atmospheric implications, Phys. Chem. Chem. Phys., 19, 2332–2345,
https://doi.org/10.1039/c6cp06718b, 2017.
Hard, T. M., Obrien, R. J., Chan, C. Y., and Mehrabzadeh, A. A.:
Tropospheric Free-Radical Determination by fluorescence by gas expansion,
Environ. Sci. Technol., 18, 768–777, https://doi.org/10.1021/es00128a009,
1984.
Heard, D. E., Carpenter, L. J., Creasey, D. J., Hopkins, J. R., Lee, J. D.,
Lewis, A. C., Pilling, M. J., Seakins, P. W., Carslaw, N., and Emmerson, K.
M.: High levels of the hydroxyl radical in the winter urban troposphere,
Geophys. Res. Lett., 31, L18112, https://doi.org/10.1029/2004GL020544, 2004.
Hens, K., Novelli, A., Martinez, M., Auld, J., Axinte, R., Bohn, B., Fischer, H., Keronen, P., Kubistin, D., Nölscher, A. C., Oswald, R., Paasonen, P., Petäjä, T., Regelin, E., Sander, R., Sinha, V., Sipilä, M., Taraborrelli, D., Tatum Ernest, C., Williams, J., Lelieveld, J., and Harder, H.: Observation and modelling of HOx radicals in a boreal forest, Atmos. Chem. Phys., 14, 8723–8747, https://doi.org/10.5194/acp-14-8723-2014, 2014.
Hewitt, C. N., Lee, J. D., MacKenzie, A. R., Barkley, M. P., Carslaw, N., Carver, G. D., Chappell, N. A., Coe, H., Collier, C., Commane, R., Davies, F., Davison, B., DiCarlo, P., Di Marco, C. F., Dorsey, J. R., Edwards, P. M., Evans, M. J., Fowler, D., Furneaux, K. L., Gallagher, M., Guenther, A., Heard, D. E., Helfter, C., Hopkins, J., Ingham, T., Irwin, M., Jones, C., Karunaharan, A., Langford, B., Lewis, A. C., Lim, S. F., MacDonald, S. M., Mahajan, A. S., Malpass, S., McFiggans, G., Mills, G., Misztal, P., Moller, S., Monks, P. S., Nemitz, E., Nicolas-Perea, V., Oetjen, H., Oram, D. E., Palmer, P. I., Phillips, G. J., Pike, R., Plane, J. M. C., Pugh, T., Pyle, J. A., Reeves, C. E., Robinson, N. H., Stewart, D., Stone, D., Whalley, L. K., and Yin, X.: Overview: oxidant and particle photochemical processes above a south-east Asian tropical rainforest (the OP3 project): introduction, rationale, location characteristics and tools, Atmos. Chem. Phys., 10, 169–199, https://doi.org/10.5194/acp-10-169-2010, 2010.
Hofzumahaus, A. and Heard, D. E.: Assessment of Local HOx and ROx
Measurement Techniques: Achievements, Challenges, and Future Directions –
Outcomes of the 2015 International HOx Workshop, IGAG News, 55, 20–21,
2015.
Hofzumahaus, A., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C. C.,
Fuchs, H., Holland, F., Kita, K., Kondo, Y., Li, X., Lou, S., Shao, M.,
Zeng, L., Wahner, A., and Zhang, Y.: Amplified trace gas removal in the
troposphere, Science, 324, 1702–1704, https://doi.org/10.1126/science.1164566, 2009.
Lee, J. D., Whalley, L. K., Heard, D. E., Stone, D., Dunmore, R. E., Hamilton, J. F., Young, D. E., Allan, J. D., Laufs, S., and Kleffmann, J.: Detailed budget analysis of HONO in central London reveals a missing daytime source, Atmos. Chem. Phys., 16, 2747–2764, https://doi.org/10.5194/acp-16-2747-2016, 2016.
Lelieveld, J., Butler, T. M., Crowley, J. N., Dillon, T. J., Fischer, H.,
Ganzeveld, L., Harder, H., Lawrence, M. G., Martinez, M., Taraborrelli, D.,
and Williams, J.: Atmospheric oxidation capacity sustained by a tropical
forest, Nature, 452, 737–740, https://doi.org/10.1038/nature06870, 2008.
Lew, M. L., Rickly, P. S., Bottorff, B. P., Sklaveniti, S., Léonardis, T., Locoge, N., Dusanter, S., Kundu, S., Wood, E., and Stevens, P. S.: OH and HO2 radical chemistry in a midlatitude forest: Measurements and model comparisons, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2019-726, in review, 2019.
Lewis, T. R., Blitz, M. A., Heard, D. E., and Seakins, P. W.: Direct
evidence for a substantive reaction between the Criegee intermediate,
CH2OO, and the water vapour dimer, Phys. Chem. Chem. Phys., 17, 4859–4863,
https://doi.org/10.1039/c4cp04750h, 2015.
Lin, L. C., Chao, W., Chang, C. H., Takahashi, K., and Lin, J. J.:
Temperature dependence of the reaction of anti-CH3CHOO with water
vapor, Phys. Chem. Chem. Phys., 18, 28189–28197, https://doi.org/10.1039/c6cp05171e, 2016.
Lu, K. D., Rohrer, F., Holland, F., Fuchs, H., Brauers, T., Oebel, A., Dlugi, R., Hu, M., Li, X., Lou, S. R., Shao, M., Zhu, T., Wahner, A., Zhang, Y. H., and Hofzumahaus, A.: Nighttime observation and chemistry of HOx in the Pearl River Delta and Beijing in summer 2006, Atmos. Chem. Phys., 14, 4979–4999, https://doi.org/10.5194/acp-14-4979-2014, 2014.
Mallik, C., Tomsche, L., Bourtsoukidis, E., Crowley, J. N., Derstroff, B., Fischer, H., Hafermann, S., Hüser, I., Javed, U., Keßel, S., Lelieveld, J., Martinez, M., Meusel, H., Novelli, A., Phillips, G. J., Pozzer, A., Reiffs, A., Sander, R., Taraborrelli, D., Sauvage, C., Schuladen, J., Su, H., Williams, J., and Harder, H.: Oxidation processes in the eastern Mediterranean atmosphere: evidence from the modelling of HOx measurements over Cyprus, Atmos. Chem. Phys., 18, 10825–10847, https://doi.org/10.5194/acp-18-10825-2018, 2018.
Mao, J., Ren, X., Zhang, L., Van Duin, D. M., Cohen, R. C., Park, J.-H., Goldstein, A. H., Paulot, F., Beaver, M. R., Crounse, J. D., Wennberg, P. O., DiGangi, J. P., Henry, S. B., Keutsch, F. N., Park, C., Schade, G. W., Wolfe, G. M., Thornton, J. A., and Brune, W. H.: Insights into hydroxyl measurements and atmospheric oxidation in a California forest, Atmos. Chem. Phys., 12, 8009–8020, https://doi.org/10.5194/acp-12-8009-2012, 2012.
Martinez, M., Harder, H., Ren, X., Lesher, R. L., and Brune, W. H.: Measuring atmospheric naphthalene with laser-induced fluorescence, Atmos. Chem. Phys., 4, 563–569, https://doi.org/10.5194/acp-4-563-2004, 2004.
Martinez, M., Harder, H., Kubistin, D., Rudolf, M., Bozem, H., Eerdekens, G., Fischer, H., Klüpfel, T., Gurk, C., Königstedt, R., Parchatka, U., Schiller, C. L., Stickler, A., Williams, J., and Lelieveld, J.: Hydroxyl radicals in the tropical troposphere over the Suriname rainforest: airborne measurements, Atmos. Chem. Phys., 10, 3759–3773, https://doi.org/10.5194/acp-10-3759-2010, 2010.
Molteni, U., Bianchi, F., Klein, F., El Haddad, I., Frege, C., Rossi, M. J., Dommen, J., and Baltensperger, U.: Formation of highly oxygenated organic molecules from aromatic compounds, Atmos. Chem. Phys., 18, 1909–1921, https://doi.org/10.5194/acp-18-1909-2018, 2018.
Newland, M. J., Rickard, A. R., Vereecken, L., Muñoz, A., Ródenas, M., and Bloss, W. J.: Atmospheric isoprene ozonolysis: impacts of stabilised Criegee intermediate reactions with SO2, H2O and dimethyl sulfide, Atmos. Chem. Phys., 15, 9521–9536, https://doi.org/10.5194/acp-15-9521-2015, 2015.
Nguyen, T. L., Vereecken, L., and Peeters, J.: HOx regeneration in the
oxidation of isoprene III: theoretical study of the key isomerisation of the
Z-delta-hydroxy-peroxy isoprene radicals, Chemphyschem, 11, 3996–4001,
https://doi.org/10.1002/cphc.201000480, 2010.
Novelli, A., Hens, K., Tatum Ernest, C., Kubistin, D., Regelin, E., Elste, T., Plass-Dülmer, C., Martinez, M., Lelieveld, J., and Harder, H.: Characterisation of an inlet pre-injector laser-induced fluorescence instrument for the measurement of atmospheric hydroxyl radicals, Atmos. Meas. Tech., 7, 3413–3430, https://doi.org/10.5194/amt-7-3413-2014, 2014a.
Novelli, A., Vereecken, L., Lelieveld, J., and Harder, H.: Direct
observation of OH formation from stabilised Criegee intermediates, Phys. Chem.
Chem. Phys., 16, 19941–19951, https://doi.org/10.1039/c4cp02719a, 2014b.
Novelli, A., Hens, K., Tatum Ernest, C., Martinez, M., Nölscher, A. C., Sinha, V., Paasonen, P., Petäjä, T., Sipilä, M., Elste, T., Plass-Dülmer, C., Phillips, G. J., Kubistin, D., Williams, J., Vereecken, L., Lelieveld, J., and Harder, H.: Estimating the atmospheric concentration of Criegee intermediates and their possible interference in a FAGE-LIF instrument, Atmos. Chem. Phys., 17, 7807–7826, https://doi.org/10.5194/acp-17-7807-2017, 2017.
Novelli, A., Kaminski, M., Rolletter, M., Acir, I.-H., Bohn, B., Dorn, H.-P., Li, X., Lutz, A., Nehr, S., Rohrer, F., Tillmann, R., Wegener, R., Holland, F., Hofzumahaus, A., Kiendler-Scharr, A., Wahner, A., and Fuchs, H.: Evaluation of OH and HO2 concentrations and their budgets during photooxidation of 2-methyl-3-butene-2-ol (MBO) in the atmospheric simulation chamber SAPHIR, Atmos. Chem. Phys., 18, 11409–11422, https://doi.org/10.5194/acp-18-11409-2018, 2018.
Paulot, F., Crounse, J. D., Kjaergaard, H. G., Kurten, A., St Clair, J. M.,
Seinfeld, J. H., and Wennberg, P. O.: Unexpected epoxide formation in the
gas-phase photooxidation of isoprene, Science, 325, 730–733,
https://doi.org/10.1126/science.1172910, 2009.
Peeters, J. and Muller, J. F.: HO(x) radical regeneration in isoprene
oxidation via peroxy radical isomerisations. II: experimental evidence and
global impact, Phys. Chem. Chem. Phys., 12, 14227–14235,
https://doi.org/10.1039/c0cp00811g, 2010.
Peeters, J., Nguyen, T. L., and Vereecken, L.: HOx radical regeneration
in the oxidation of isoprene, Phys. Chem. Chem. Phys., 11,
5935–5939, https://doi.org/10.1039/b908511d, 2009.
Peeters, J., Muller, J. F., Stavrakou, T., and Nguyen, V. S.: Hydroxyl
radical recycling in isoprene oxidation driven by hydrogen bonding and
hydrogen tunneling: the upgraded LIM1 mechanism, J. Phys. Chem. A, 118, 8625–8643, https://doi.org/10.1021/jp5033146, 2014.
Praske, E., Crounse, J. D., Bates, K. H., Kurten, T., Kjaergaard, H. G., and
Wennberg, P. O.: Atmospheric fate of methyl vinyl ketone: peroxy radical
reactions with NO and HO2, J. Phys. Chem. A, 119,
4562–4572, https://doi.org/10.1021/jp5107058, 2015.
Ren, X. R., Harder, H., Martinez, M., Faloona, I. C., Tan, D., Lesher, R.
L., Di Carlo, P., Simpas, J. B., and Brune, W. H.: Interference testing for
atmospheric HOx measurements by laser-induced fluorescence, J.
Atmos. Chem., 47, 169–190, https://doi.org/10.1023/B:Joch.0000021037.46866.81,
2004.
Ren, X. R., Olson, J. R., Crawford, J. H., Brune, W. H., Mao, J. Q., Long,
R. B., Chen, Z., Chen, G., Avery, M. A., Sachse, G. W., Barrick, J. D.,
Diskin, G. S., Huey, L. G., Fried, A., Cohen, R. C., Heikes, B., Wennberg,
P. O., Singh, H. B., Blake, D. R., and Shetter, R. E.: HOx chemistry
during INTEX-A 2004: Observation, model calculation, and comparison with
previous studies, J. Geophys. Res.-Atmos., 113, D05310,
https://doi.org/10.1029/2007jd009166, 2008.
Ren, X. R., van Duin, D., Cazorla, M., Chen, S., Mao, J. Q., Zhang, L.,
Brune, W. H., Flynn, J. H., Grossberg, N., Lefer, B. L., Rappengluck, B.,
Wong, K. W., Tsai, C., Stutz, J., Dibb, J. E., Jobson, B. T., Luke, W. T.,
and Kelley, P.: Atmospheric oxidation chemistry and ozone production:
Results from SHARP 2009 in Houston, Texas, J. Geophys. Res.-Atmos., 118, 5770–5780, https://doi.org/10.1002/jgrd.50342, 2013.
Rickly, P. and Stevens, P. S.: Measurements of a potential interference with laser-induced fluorescence measurements of ambient OH from the ozonolysis of biogenic alkenes, Atmos. Meas. Tech., 11, 1–16, https://doi.org/10.5194/amt-11-1-2018, 2018.
Sander, S. P., Abbatt, J., Barker, J. R., Burkholder, J. B., Friedl, D. M.,
Golden, D. M., Huie, R. E., Kolb, C. E., Kurylo, M. J., Moortgat, G. K.,
Orkin, V. L., and Wine, P. H.: Chemical Kinetics and Photochemical Data for
Use in Atmospheric Studies, Evaluation No. 17, 2011.
Sheps, L., Scully, A. M., and Au, K.: UV absorption probing of the
conformer-dependent reactivity of a Criegee intermediate CH3CHOO,
Phys. Chem. Chem. Phys., 16, 26701–26706, https://doi.org/10.1039/c4cp04408h,
2014.
Shi, Z., Vu, T., Kotthaus, S., Harrison, R. M., Grimmond, S., Yue, S., Zhu, T., Lee, J., Han, Y., Demuzere, M., Dunmore, R. E., Ren, L., Liu, D., Wang, Y., Wild, O., Allan, J., Acton, W. J., Barlow, J., Barratt, B., Beddows, D., Bloss, W. J., Calzolai, G., Carruthers, D., Carslaw, D. C., Chan, Q., Chatzidiakou, L., Chen, Y., Crilley, L., Coe, H., Dai, T., Doherty, R., Duan, F., Fu, P., Ge, B., Ge, M., Guan, D., Hamilton, J. F., He, K., Heal, M., Heard, D., Hewitt, C. N., Hollaway, M., Hu, M., Ji, D., Jiang, X., Jones, R., Kalberer, M., Kelly, F. J., Kramer, L., Langford, B., Lin, C., Lewis, A. C., Li, J., Li, W., Liu, H., Liu, J., Loh, M., Lu, K., Lucarelli, F., Mann, G., McFiggans, G., Miller, M. R., Mills, G., Monk, P., Nemitz, E., O'Connor, F., Ouyang, B., Palmer, P. I., Percival, C., Popoola, O., Reeves, C., Rickard, A. R., Shao, L., Shi, G., Spracklen, D., Stevenson, D., Sun, Y., Sun, Z., Tao, S., Tong, S., Wang, Q., Wang, W., Wang, X., Wang, X., Wang, Z., Wei, L., Whalley, L., Wu, X., Wu, Z., Xie, P., Yang, F., Zhang, Q., Zhang, Y., Zhang, Y., and Zheng, M.: Introduction to the special issue “In-depth study of air pollution sources and processes within Beijing and its surrounding region (APHH-Beijing)”, Atmos. Chem. Phys., 19, 7519–7546, https://doi.org/10.5194/acp-19-7519-2019, 2019.
Smith, S. C., Lee, J. D., Bloss, W. J., Johnson, G. P., Ingham, T., and Heard, D. E.: Concentrations of OH and HO2 radicals during NAMBLEX: measurements and steady state analysis, Atmos. Chem. Phys., 6, 1435–1453, https://doi.org/10.5194/acp-6-1435-2006, 2006.
Stevens, P. S., Mather, J. H., and Brune, W. H.: Measurement of Tropospheric
OH and HO2 by Laser-Induced Fluorescence at Low-Pressure, J.
Geophys. Res.-Atmos., 99, 3543–3557, https://doi.org/10.1029/93jd03342, 1994.
Stone, D., Evans, M. J., Edwards, P. M., Commane, R., Ingham, T., Rickard, A. R., Brookes, D. M., Hopkins, J., Leigh, R. J., Lewis, A. C., Monks, P. S., Oram, D., Reeves, C. E., Stewart, D., and Heard, D. E.: Isoprene oxidation mechanisms: measurements and modelling of OH and HO2 over a South-East Asian tropical rainforest during the OP3 field campaign, Atmos. Chem. Phys., 11, 6749–6771, https://doi.org/10.5194/acp-11-6749-2011, 2011.
Stone, D., Whalley, L. K., Ingham, T., Edwards, P. M., Cryer, D. R., Brumby, C. A., Seakins, P. W., and Heard, D. E.: Measurement of OH reactivity by laser flash photolysis coupled with laser-induced fluorescence spectroscopy, Atmos. Meas. Tech., 9, 2827–2844, https://doi.org/10.5194/amt-9-2827-2016, 2016.
Taatjes, C. A., Welz, O., Eskola, A. J., Savee, J. D., Scheer, A. M.,
Shallcross, D. E., Rotavera, B., Lee, E. P., Dyke, J. M., Mok, D. K.,
Osborn, D. L., and Percival, C. J.: Direct measurements of
conformer-dependent reactivity of the Criegee intermediate CH3CHOO,
Science, 340, 177–180, https://doi.org/10.1126/science.1234689, 2013.
Tan, Z., Fuchs, H., Lu, K., Hofzumahaus, A., Bohn, B., Broch, S., Dong, H., Gomm, S., Häseler, R., He, L., Holland, F., Li, X., Liu, Y., Lu, S., Rohrer, F., Shao, M., Wang, B., Wang, M., Wu, Y., Zeng, L., Zhang, Y., Wahner, A., and Zhang, Y.: Radical chemistry at a rural site (Wangdu) in the North China Plain: observation and model calculations of OH, HO2 and RO2 radicals, Atmos. Chem. Phys., 17, 663–690, https://doi.org/10.5194/acp-17-663-2017, 2017.
Tan, Z., Rohrer, F., Lu, K., Ma, X., Bohn, B., Broch, S., Dong, H., Fuchs, H., Gkatzelis, G. I., Hofzumahaus, A., Holland, F., Li, X., Liu, Y., Liu, Y., Novelli, A., Shao, M., Wang, H., Wu, Y., Zeng, L., Hu, M., Kiendler-Scharr, A., Wahner, A., and Zhang, Y.: Wintertime photochemistry in Beijing: observations of ROx radical concentrations in the North China Plain during the BEST-ONE campaign, Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, 2018.
Tan, Z., Lu, K., Hofzumahaus, A., Fuchs, H., Bohn, B., Holland, F., Liu, Y., Rohrer, F., Shao, M., Sun, K., Wu, Y., Zeng, L., Zhang, Y., Zou, Q., Kiendler-Scharr, A., Wahner, A., and Zhang, Y.: Experimental budgets of OH, HO2, and RO2 radicals and implications for ozone formation in the Pearl River Delta in China 2014, Atmos. Chem. Phys., 19, 7129–7150, https://doi.org/10.5194/acp-19-7129-2019, 2019.
Teng, A. P., Crounse, J. D., and Wennberg, P. O.: Isoprene Peroxy Radical
Dynamics, J. Am. Chem. Soc., 139, 5367–5377,
https://doi.org/10.1021/jacs.6b12838, 2017.
Tsiligiannis, E., Hammes, J., Salvador, C. M., Mentel, T. F., and Hallquist, M.: Effect of NOx on 1,3,5-trimethylbenzene (TMB) oxidation product distribution and particle formation, Atmos. Chem. Phys., 19, 15073–15086, https://doi.org/10.5194/acp-19-15073-2019, 2019.
Wang, S., Wu, R., Berndt, T., Ehn, M., and Wang, L.: Formation of Highly
Oxidized Radicals and Multifunctional Products from the Atmospheric
Oxidation of Alkylbenzenes, Environ. Sci. Technol., 51,
8442–8449, https://doi.org/10.1021/acs.est.7b02374, 2017.
Welz, O., Savee, J. D., Osborn, D. L., Vasu, S. S., Percival, C. J.,
Shallcross, D. E., and Taatjes, C. A.: Direct kinetic measurements of
Criegee intermediate (CH2OO) formed by reaction of CH2I with
O2, Science, 335, 204–207, https://doi.org/10.1126/science.1213229, 2012.
Welz, O., Eskola, A. J., Sheps, L., Rotavera, B., Savee, J. D., Scheer, A.
M., Osborn, D. L., Lowe, D., Murray Booth, A., Xiao, P., Anwar, H. K. M.,
Percival, C. J., Shallcross, D. E., and Taatjes, C. A.: Rate coefficients of
C(1) and C(2) Criegee intermediate reactions with formic and acetic Acid
near the collision limit: direct kinetics measurements and atmospheric
implications, Angew. Chem. Int. Edit., 53,
4547–4550, https://doi.org/10.1002/anie.201400964, 2014.
Whalley, L. K., Furneaux, K. L., Goddard, A., Lee, J. D., Mahajan, A., Oetjen, H., Read, K. A., Kaaden, N., Carpenter, L. J., Lewis, A. C., Plane, J. M. C., Saltzman, E. S., Wiedensohler, A., and Heard, D. E.: The chemistry of OH and HO2 radicals in the boundary layer over the tropical Atlantic Ocean, Atmos. Chem. Phys., 10, 1555–1576, https://doi.org/10.5194/acp-10-1555-2010, 2010.
Whalley, L. K., Edwards, P. M., Furneaux, K. L., Goddard, A., Ingham, T., Evans, M. J., Stone, D., Hopkins, J. R., Jones, C. E., Karunaharan, A., Lee, J. D., Lewis, A. C., Monks, P. S., Moller, S. J., and Heard, D. E.: Quantifying the magnitude of a missing hydroxyl radical source in a tropical rainforest, Atmos. Chem. Phys., 11, 7223–7233, https://doi.org/10.5194/acp-11-7223-2011, 2011.
Whalley, L. K., Blitz, M. A., Desservettaz, M., Seakins, P. W., and Heard, D. E.: Reporting the sensitivity of laser-induced fluorescence instruments used for HO2 detection to an interference from RO2 radicals and introducing a novel approach that enables HO2 and certain RO2 types to be selectively measured, Atmos. Meas. Tech., 6, 3425–3440, https://doi.org/10.5194/amt-6-3425-2013, 2013.
Whalley, L. K., Stone, D., Bandy, B., Dunmore, R., Hamilton, J. F., Hopkins, J., Lee, J. D., Lewis, A. C., and Heard, D. E.: Atmospheric OH reactivity in central London: observations, model predictions and estimates of in situ ozone production, Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, 2016.
Whalley, L. K., Stone, D., Dunmore, R., Hamilton, J., Hopkins, J. R., Lee, J. D., Lewis, A. C., Williams, P., Kleffmann, J., Laufs, S., Woodward-Massey, R., and Heard, D. E.: Understanding in situ ozone production in the summertime through radical observations and modelling studies during the Clean air for London project (ClearfLo), Atmos. Chem. Phys., 18, 2547–2571, https://doi.org/10.5194/acp-18-2547-2018, 2018.
Winiberg, F. A. F., Smith, S. C., Bejan, I., Brumby, C. A., Ingham, T., Malkin, T. L., Orr, S. C., Heard, D. E., and Seakins, P. W.: Pressure-dependent calibration of the OH and HO2 channels of a FAGE HOx instrument using the Highly Instrumented Reactor for Atmospheric Chemistry (HIRAC), Atmos. Meas. Tech., 8, 523–540, https://doi.org/10.5194/amt-8-523-2015, 2015.
Wolfe, G. M., Thornton, J. A., Bouvier-Brown, N. C., Goldstein, A. H., Park, J.-H., McKay, M., Matross, D. M., Mao, J., Brune, W. H., LaFranchi, B. W., Browne, E. C., Min, K.-E., Wooldridge, P. J., Cohen, R. C., Crounse, J. D., Faloona, I. C., Gilman, J. B., Kuster, W. C., de Gouw, J. A., Huisman, A., and Keutsch, F. N.: The Chemistry of Atmosphere-Forest Exchange (CAFE) Model – Part 2: Application to BEARPEX-2007 observations, Atmos. Chem. Phys., 11, 1269–1294, https://doi.org/10.5194/acp-11-1269-2011, 2011.
Wolfe, G. M., Crounse, J. D., Parrish, J. D., St Clair, J. M., Beaver, M.
R., Paulot, F., Yoon, T. P., Wennberg, P. O., and Keutsch, F. N.:
Photolysis, OH reactivity and ozone reactivity of a proxy for
isoprene-derived hydroperoxyenals (HPALDs), Phys. Chem. Chem. Phys., 14, 7276–7286, https://doi.org/10.1039/c2cp40388a, 2012.
Short summary
The OH radical is known as nature’s detergent, removing most trace gases from the atmosphere. Hence, an accurate measurement of its concentration is very important. We present measurements of OH in several field locations using a laser-based fluorescence method equipped with an OH scavenger. By determining the background signal in two different ways, we show that the instrument does not suffer any significant interferences that could result in an overestimation of OH concentrations.
The OH radical is known as nature’s detergent, removing most trace gases from the atmosphere....
