Articles | Volume 13, issue 9
Research article 18 Sep 2020
Research article | 18 Sep 2020
A new approach for measuring the carbon and oxygen content of atmospherically relevant compounds and mixtures
James F. Hurley et al.
No articles found.
Gabriel Isaacman-VanWertz and Bernard Aumont
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
There are tens of thousands of different chemical compounds in the atmosphere. To tackle this complexity, there are a wide range of different methods to estimate their physical and chemical properties. We use these methods to understand how much the detailed structure of a molecule impacts its properties, and the extent to which properties can be estimated without knowing this level of detail. We find that structure matters, but methods lacking that level of detail still perform reasonably well.
Chenyang Bi, Jordan E. Krechmer, Graham O. Frazier, Wen Xu, Andrew T. Lambe, Megan S. Claflin, Brian M. Lerner, John T. Jayne, Douglas R. Worsnop, Manjula R. Canagaratna, and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech. Discuss.,
Preprint under review for AMTShort summary
Measurement techniques that can achieve molecular characterizations are necessary to understand the differences of fate and transport within isomers produced in the atmospheric oxidation process. In this work, we develop an instrument to conduct isomer-resolved measurements of particle-phase organics. We assess the number of isomers per chemical formula in atmospherically-relevant samples and examine the feasibility of extending the use of an existing instrument to a broader range of analytes.
Sanna Saarikoski, Leah R. Williams, Steven R. Spielman, Gregory S. Lewis, Arantzazu Eiguren-Fernandez, Minna Aurela, Susanne V. Hering, Kimmo Teinilä, Philip Croteau, John T. Jayne, Thorsten Hohaus, Douglas R. Worsnop, and Hilkka Timonen
Atmos. Meas. Tech., 12, 3907–3920,Short summary
An air-to-air ultrafine particle concentrator (Aerosol Dynamics Inc. concentrator; ADIc) has been tailored for the low (~ 0.08 L min−1) inlet flow of aerosol mass spectrometers, and it provides a factor of 8–21 enrichment in the concentration of particles. The ADIc was evaluated in laboratory and field measurements. The results showed that the concentration factor depends primarily on the ratio between the sample flow and the output flow and is independent of particle size above about 10 nm.
Suzane S. de Sá, Luciana V. Rizzo, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Joel Brito, Samara Carbone, Yingjun J. Liu, Arthur Sedlacek, Stephen Springston, Allen H. Goldstein, Henrique M. J. Barbosa, M. Lizabeth Alexander, Paulo Artaxo, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 19, 7973–8001,Short summary
This study investigates the impacts of urban and fire emissions on the concentration, composition, and optical properties of submicron particulate matter (PM1) in central Amazonia during the dry season. Biomass-burning and urban emissions appeared to contribute at least 80 % of brown carbon absorption while accounting for 30 % to 40 % of the organic PM1 mass concentration. Only a fraction of the 9-fold increase in mass concentration relative to the wet season was due to biomass burning.
Coty N. Jen, Lindsay E. Hatch, Vanessa Selimovic, Robert J. Yokelson, Robert Weber, Arantza E. Fernandez, Nathan M. Kreisberg, Kelley C. Barsanti, and Allen H. Goldstein
Atmos. Chem. Phys., 19, 1013–1026,Short summary
Wildfires in the western US are occurring more frequently and burning larger land areas. Smoke from these fires will play a greater role in regional air quality and atmospheric chemistry than in the past. To help fire and climate modelers and atmospheric experimentalists better understand how smoke impacts the environment, we have separated, identified, classified, and quantified the thousands of organic compounds found in smoke and related their amounts emitted to fire conditions.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Joel Brito, Samara Carbone, Igor O. Ribeiro, Glauber G. Cirino, Yingjun Liu, Ryan Thalman, Arthur Sedlacek, Aaron Funk, Courtney Schumacher, John E. Shilling, Johannes Schneider, Paulo Artaxo, Allen H. Goldstein, Rodrigo A. F. Souza, Jian Wang, Karena A. McKinney, Henrique Barbosa, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 18, 12185–12206,Short summary
This study aimed at understanding and quantifying the changes in mass concentration and composition of submicron airborne particulate matter (PM) in Amazonia due to urban pollution. Downwind of Manaus, PM concentrations increased by up to 200 % under polluted compared with background conditions. The observed changes included contributions from both primary and secondary processes. The differences in organic PM composition suggested a shift in the pathways of secondary production with pollution.
Lindsay D. Yee, Gabriel Isaacman-VanWertz, Rebecca A. Wernis, Meng Meng, Ventura Rivera, Nathan M. Kreisberg, Susanne V. Hering, Mads S. Bering, Marianne Glasius, Mary Alice Upshur, Ariana Gray Bé, Regan J. Thomson, Franz M. Geiger, John H. Offenberg, Michael Lewandowski, Ivan Kourtchev, Markus Kalberer, Suzane de Sá, Scot T. Martin, M. Lizabeth Alexander, Brett B. Palm, Weiwei Hu, Pedro Campuzano-Jost, Douglas A. Day, Jose L. Jimenez, Yingjun Liu, Karena A. McKinney, Paulo Artaxo, Juarez Viegas, Antonio Manzi, Maria B. Oliveira, Rodrigo de Souza, Luiz A. T. Machado, Karla Longo, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 10433–10457,Short summary
Biogenic volatile organic compounds react in the atmosphere to form secondary organic aerosol, yet the chemical pathways remain unclear. We collected filter samples and deployed a semi-volatile thermal desorption aerosol gas chromatograph in the central Amazon. We measured 30 sesquiterpenes and 4 diterpenes and find them to be important for reactive ozone loss. We estimate that sesquiterpene oxidation contributes at least 0.4–5 % (median 1 %) of observed submicron organic aerosol mass.
Brett B. Palm, Suzane S. de Sá, Douglas A. Day, Pedro Campuzano-Jost, Weiwei Hu, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Joel Brito, Florian Wurm, Paulo Artaxo, Ryan Thalman, Jian Wang, Lindsay D. Yee, Rebecca Wernis, Gabriel Isaacman-VanWertz, Allen H. Goldstein, Yingjun Liu, Stephen R. Springston, Rodrigo Souza, Matt K. Newburn, M. Lizabeth Alexander, Scot T. Martin, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 467–493,Short summary
Ambient air was oxidized by OH or O3 in an oxidation flow reactor during both wet and dry seasons in the GoAmazon2014/5 campaign to study secondary organic aerosol (SOA) formation. We investigated how much biogenic, urban, and biomass burning sources contributed to the ambient concentrations of SOA precursor gases and how their contributions changed diurnally and seasonally. SOA yields and hygroscopicity of organic aerosol in the oxidation flow reactor were also studied.
David H. Hagan, Gabriel Isaacman-VanWertz, Jonathan P. Franklin, Lisa M. M. Wallace, Benjamin D. Kocar, Colette L. Heald, and Jesse H. Kroll
Atmos. Meas. Tech., 11, 315–328,Short summary
The use of low-cost sensors for air pollution research has outpaced our understanding of their capabilities and limitations under real-world conditions. Here we describe the deployment, calibration and evaluation of electrochemical sensors on the Island of Hawai‘i. We obtain excellent performance (RMSE < 7 ppb, r2 = 0.997) across a wide dynamic range (1 ppb–2 ppm). We introduce a hybrid regression algorithm which works across a large dynamic range and shows little decay in sensitivity over time.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370,Short summary
Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Tamara Pinterich, Steven R. Spielman, Yang Wang, Susanne V. Hering, and Jian Wang
Atmos. Meas. Tech., 10, 4915–4925,Short summary
The ability of atmospheric particles to uptake water (particle hygroscopicity) is a key parameter in determining their impact on global climate. We present a humidity-controlled fast integrated mobility spectrometer (HFIMS) for rapid measurement of particle hygroscopicity. The HFIMS' performance evaluation shows that it is about an order of magnitude faster than traditional systems, greatly improving our capability to study particle hygroscopicity especially for rapidly evolving aerosols.
Juha Kangasluoma, Susanne Hering, David Picard, Gregory Lewis, Joonas Enroth, Frans Korhonen, Markku Kulmala, Karine Sellegri, Michel Attoui, and Tuukka Petäjä
Atmos. Meas. Tech., 10, 2271–2281,Short summary
The manuscript presents a characterization of three new particle counters able to detect airborne nanoparticles smaller than 3 nm in diameter. We explored some of the parameters affecting the smallest detectable particle size, such as sample flow relative humidity, the particle chemical composition and the electrical charging state. The characterization results help one to select a suitable particle counter for a given application.
Suzane S. de Sá, Brett B. Palm, Pedro Campuzano-Jost, Douglas A. Day, Matthew K. Newburn, Weiwei Hu, Gabriel Isaacman-VanWertz, Lindsay D. Yee, Ryan Thalman, Joel Brito, Samara Carbone, Paulo Artaxo, Allen H. Goldstein, Antonio O. Manzi, Rodrigo A. F. Souza, Fan Mei, John E. Shilling, Stephen R. Springston, Jian Wang, Jason D. Surratt, M. Lizabeth Alexander, Jose L. Jimenez, and Scot T. Martin
Atmos. Chem. Phys., 17, 6611–6629,
Arantzazu Eiguren-Fernandez, Nathan Kreisberg, and Susanne Hering
Atmos. Meas. Tech., 10, 633–644,Short summary
The capacity of airborne particles to generate reactive oxygen species has been correlated with the generation of oxidative stress, which may lead to the development of common diseases such as asthma and Alzheimer’s. As the oxidative potential of particles varies significantly by location and time of day, there is a need for monitoring this property in a comprehensive manner. Thus, we are developing a field-deployable system for time-resolved assessment of the oxidative capacity of particles.
Brian M. Lerner, Jessica B. Gilman, Kenneth C. Aikin, Elliot L. Atlas, Paul D. Goldan, Martin Graus, Roger Hendershot, Gabriel A. Isaacman-VanWertz, Abigail Koss, William C. Kuster, Richard A. Lueb, Richard J. McLaughlin, Jeff Peischl, Donna Sueper, Thomas B. Ryerson, Travis W. Tokarek, Carsten Warneke, Bin Yuan, and Joost A. de Gouw
Atmos. Meas. Tech., 10, 291–313,Short summary
Whole air sampling followed by analysis by gas chromatography is a common technique for characterization of trace volatile organic compounds in the atmosphere. We describe a new automated gas chromatograph–mass spectrograph which uses a Stirling cooler for sample preconcentration at −165 °C without the need for a cryogen such as liquid nitrogen. We also discuss potential sources of artifacts from our electropolished stainless steel sampling system and present results from two field campaigns.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369,Short summary
We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Brent J. Williams, Yaping Zhang, Xiaochen Zuo, Raul E. Martinez, Michael J. Walker, Nathan M. Kreisberg, Allen H. Goldstein, Kenneth S. Docherty, and Jose L. Jimenez
Atmos. Meas. Tech., 9, 1569–1586,Short summary
The thermal desorption aerosol gas chromatograph (TAG) has been used for in situ measurements of organic marker compounds to identify atmospheric particle sources and transformation processes. Here we identify that inorganic aerosol components (e.g., nitrate and sulfate) and highly oxygenated organic components experience thermal decomposition upon sample heating. This thermal decomposition signal in the TAG system is investigated through laboratory and field data.
A. Hecobian, A. Evanoski-Cole, A. Eiguren-Fernandez, A. P. Sullivan, G. S. Lewis, S. V. Hering, and J. L. Collett Jr.
Atmos. Meas. Tech., 9, 525–533,Short summary
A newly developed instrument, the Sequential Spot Sampler (S3) was evaluated in the laboratory and field for the hourly measurement of ambient PM2.5 nitrate and sulfate concentrations. The results from the comparison of two S3s and the S3s with other well-established methods show that this instrument is suitable for deployment; provides high-resolution aerosol nitrate and sulfate concentrations while requiring minimal operator involvement and low power input; and has a small footprint.
W. W. Hu, P. Campuzano-Jost, B. B. Palm, D. A. Day, A. M. Ortega, P. L. Hayes, J. E. Krechmer, Q. Chen, M. Kuwata, Y. J. Liu, S. S. de Sá, K. McKinney, S. T. Martin, M. Hu, S. H. Budisulistiorini, M. Riva, J. D. Surratt, J. M. St. Clair, G. Isaacman-Van Wertz, L. D. Yee, A. H. Goldstein, S. Carbone, J. Brito, P. Artaxo, J. A. de Gouw, A. Koss, A. Wisthaler, T. Mikoviny, T. Karl, L. Kaser, W. Jud, A. Hansel, K. S. Docherty, M. L. Alexander, N. H. Robinson, H. Coe, J. D. Allan, M. R. Canagaratna, F. Paulot, and J. L. Jimenez
Atmos. Chem. Phys., 15, 11807–11833,Short summary
This work summarized all the studies reporting isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) measured globally by aerosol mass spectrometer and compare them with modeled gas-phase IEPOX, with results suggestive of the importance of IEPOX-SOA for regional and global OA budgets. A real-time tracer of IEPOX-SOA is thoroughly evaluated for the first time by combing multiple field and chamber studies. A quick and easy empirical method on IEPOX-SOA estimation is also presented.
G. Isaacman, N. M. Kreisberg, L. D. Yee, D. R. Worton, A. W. H. Chan, J. A. Moss, S. V. Hering, and A. H. Goldstein
Atmos. Meas. Tech., 7, 4417–4429,Short summary
We present here a new in situ instrument for ambient measurements of highly polar organic semi-volatile and low-volatility compounds in both the gas and particle phase by gas chromatography. Compounds previously measured only through filter collection and offline analysis can now be measured hourly with, in most cases, less than 20% uncertainty. This instrument provides unprecedented time resolution and the first ever observations of gas-particle partitioning for most of these compounds.
N. M. Kreisberg, D. R. Worton, Y. Zhao, G. Isaacman, A. H. Goldstein, and S. V. Hering
Atmos. Meas. Tech., 7, 4431–4444,
Related subject area
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learning techniques and spark emission spectroscopyAn experimental study on light scattering matrices for Chinese loess dust with different particle size distributionsCounting on chemistry: laboratory evaluation of seed-material-dependent detection efficiencies of ultrafine condensation particle countersPhotophoretic spectroscopy in atmospheric chemistry – high-sensitivity measurements of light absorption by a single particleLaboratory evaluation of particle-size selectivity of optical low-cost particulate matter sensorsMapping ice formation to mineral-surface topography using a micro mixing chamber with video and atomic-force microscopyHigh-humidity tandem differential mobility analyzer for accurate determination of aerosol hygroscopic growth, microstructure, and activity coefficients over a wide range of relative humidityDevelopment of an improved two-sphere integration technique for quantifying black carbon concentrations in the atmosphere and seasonal snowDevelopment of the DRoplet 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Arttu Ylisirniö, Luis M. F. Barreira, Iida Pullinen, Angela Buchholz, John Jayne, Jordan E. Krechmer, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Meas. Tech., 14, 355–367,Short summary
FIGAERO-ToF-CIMS enables online volatility measurements of chemical compounds in ambient aerosols. Previously published volatility calibration results however differ from each other significantly. In this study we investigate the reason for this discrepancy. We found a major source of error in the widely used syringe deposition method and propose a new method for volatility calibration by using atomized calibration compounds.
Bradley Visser, Jannis Röhrbein, Peter Steigmeier, Luka Drinovec, Griša Močnik, and Ernest Weingartner
Atmos. Meas. Tech., 13, 7097–7111,Short summary
Here we report on the development of a novel single-beam photothermal interferometer and its use in the measurement of aerosol light absorption. We demonstrate how light-absorbing gases can be used to calibrate the instrument and how this absorption is automatically subtracted during normal operation. The performance of the instrument is compared to a standard filter-based instrument using a black carbon test aerosol. The 60 s detection limit is found to be less than 10 Mm-1.
Michael Rösch and Daniel J. Cziczo
Atmos. Meas. Tech., 13, 6807–6812,Short summary
The need for a simple atomizer with a high-output stability combined with the capabilities of CAD software and high-resolution 3D printing has allowed for the design, production and testing of the PRinted drOpleT Generator (PROTeGE) to generate liquid particles from solutions. The size and number concentrations of the generated particles have been characterized with different ammonium sulfate and PSL solutions. PROTeGE is easy to operate, requires minimal maintenance and is cost-effective.
Gourihar Kulkarni, Naruki Hiranuma, Ottmar Möhler, Kristina Höhler, Swarup China, Daniel J. Cziczo, and Paul J. DeMott
Atmos. Meas. Tech., 13, 6631–6643,Short summary
This study presents a new continuous-flow-diffusion-chamber-style operated ice chamber (Modified Compact Ice Chamber, MCIC) to measure the immersion-freezing efficiency of atmospheric particles. MCIC allowed us to obtain maximum droplet-freezing efficiency at higher time resolution without droplet breakthrough ambiguity. Its evaluation was performed by reproducing published data from the recent ice nucleation workshop and past laboratory data for standard and airborne ice-nucleating particles.
Christian Tauber, David Schmoll, Johannes Gruenwald, Sophia Brilke, Peter Josef Wlasits, Paul Martin Winkler, and Daniela Wimmer
Atmos. Meas. Tech., 13, 5993–6006,Short summary
In this paper we show that a commercially available plasma charger with nitrogen as the working gas can enhance the charging probability for sub-12 nm particles. In addition, the charger ion mobilities and the chemical composition have been examined using an atmospheric pressure interface time-of-flight mass spectrometer (APi-TOF MS), and comparison of the experimental results revealed that the generated neutralizer ions are not dependent on the charging mechanism.
Marcel Weloe and Thorsten Hoffmann
Atmos. Meas. Tech., 13, 5725–5738,Short summary
Aerosol mass spectrometers (AMSs) are frequently applied in atmospheric aerosol research in connection with climate, environmental or health-related projects. The paper describes a new real-time technique for the measurement of organic peroxides, which play an important role in new particle formation and as
reactive oxygen speciesin aerosol–health-related aspects of atmospheric aerosols.
Ting Lei, Nan Ma, Juan Hong, Thomas Tuch, Xin Wang, Zhibin Wang, Mira Pöhlker, Maofa Ge, Weigang Wang, Eugene Mikhailov, Thorsten Hoffmann, Ulrich Pöschl, Hang Su, Alfred Wiedensohler, and Yafang Cheng
Atmos. Meas. Tech., 13, 5551–5567,Short summary
We present the design of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. We further introduce comprehensive methods for system calibration and validation of the performance of the system. We then study the size dependence of the deliquescence and the efflorescence of aerosol nanoparticles for sizes down to 6 nm.
Seyyed Ali Davari and Anthony S. Wexler
Atmos. Meas. Tech., 13, 5369–5377,Short summary
Traditional instruments for detection and quantification of toxic metals in the atmosphere are expensive. In this study, we have designed, fabricated, and tested a low-cost instrument, which employs cheap components to detect and quantify toxic metals. Advanced machine learning (ML) techniques have been used to improve the instrument's performance. This study demonstrates how the combination of low-cost sensors with ML can address problems that traditionally have been too expensive to be solved.
Jia Liu, Qixing Zhang, Yinuo Huo, Jinjun Wang, and Yongming Zhang
Atmos. Meas. Tech., 13, 4097–4109,Short summary
Angular behaviors of light scattering properties for loess dust sampled from the Chinese Loess Plateau were investigated using a self-developed apparatus. Two samples with different size distributions were used to represent dust that can or cannot be transported over long ranges. Analyses of optical simulation results showed that differences of measurements are mainly caused by different sizes. This study is useful for the development of optical models of loess dust during transportation.
Peter Josef Wlasits, Dominik Stolzenburg, Christian Tauber, Sophia Brilke, Sebastian Harald Schmitt, Paul Martin Winkler, and Daniela Wimmer
Atmos. Meas. Tech., 13, 3787–3798,Short summary
In this paper we show that chemical similarities between the seed particle material and the working fluid have an impact on the detection efficiency of commonly used CPCs. A remarkable set of CPCs, including the newly developed V-WCPC 3789, was tested. Among others, reproducibly generated organic seeds based on beta-caryophyllene were used. Theoretical simulations of supersaturation profiles were successfully linked to measured data.
Nir Bluvshtein, Ulrich K. Krieger, and Thomas Peter
Atmos. Meas. Tech., 13, 3191–3203,Short summary
Light-absorbing organic particles undergo transformations during their exposure in the atmosphere. The role these particles play in the global radiative balance is uncertain. This study describes high-sensitivity and high-precision measurements of light absorption by a single particle levitated in an electrodynamic balance. This high level of sensitivity enables future studies to explore the major processes responsible for changes to the particle's light absorptivity.
Joel Kuula, Timo Mäkelä, Minna Aurela, Kimmo Teinilä, Samu Varjonen, Óscar González, and Hilkka Timonen
Atmos. Meas. Tech., 13, 2413–2423,Short summary
Particle-size-dependent detection ranges of low-cost particulate matter sensors were evaluated in a laboratory experiment. Six different sensor models were evaluated altogether. The results showed that none of the sensor models adhered to the technical specifications provided by the manufacturers, and thus a high risk of sensor misuse is posed. It is paramount that the limitations regarding the particle size discrimination of low-cost sensors are acknowledged properly.
Raymond W. Friddle and Konrad Thürmer
Atmos. Meas. Tech., 13, 2209–2218,Short summary
An obstacle to predicting ice content in mixed-phase clouds is the inability to directly view atmospheric ice nucleation at the nanoscale, where this process occurs. Here we show how a cloud-like environment can be created in a small atomic-force microscopy (AFM) sample cell. By colocating video microscopy of ice formation with high-resolution AFM images, we quantitatively show how the surface topography, down to nanometer-length scales, can determine the preferential locations of ice formation.
Eugene F. Mikhailov and Sergey S. Vlasenko
Atmos. Meas. Tech., 13, 2035–2056,Short summary
Here we present the high-humidity tandem differential hygroscopicity analyzer (HHTDMA) and a new method to measure the hygroscopic growth of aerosol particles with in situ restructuring to minimize the influence of particle shape. Our results demonstrate that the HHTDMA system described in this work allows us to determine the thermodynamic characteristics of aqueous solutions with an accuracy close to that obtained by bulk methods.
Xin Wang, Xueying Zhang, and Wenjing Di
Atmos. Meas. Tech., 13, 39–52,Short summary
We developed an improved two-sphere integration (TSI) technique to quantify black carbon (BC) concentrations in the atmosphere and seasonal snow. The major advantage of this system is that it combines two distinct integrated spheres to reduce the scattering effect due to light-absorbing particles and thus provides accurate determinations of total light absorption from BC collected on Nuclepore filters.
Robert O. David, Maria Cascajo-Castresana, Killian P. Brennan, Michael Rösch, Nora Els, Julia Werz, Vera Weichlinger, Lin S. Boynton, Sophie Bogler, Nadine Borduas-Dedekind, Claudia Marcolli, and Zamin A. Kanji
Atmos. Meas. Tech., 12, 6865–6888,Short summary
Here we present the development and applicability of the DRoplet Ice Nuclei Counter Zurich (DRINCZ). DRINCZ allows for ice nuclei in the immersion mode to be quantified between 0 and -25 °C with an uncertainty of ±0.9 °C. Furthermore, we present a new method for assessing biases in drop-freezing apparatuses and cumulative ice-nucleating-particle concentrations from snow samples collected in the Austrian Alps at the Sonnblick Observatory.
Jonas Svensson, Johan Ström, and Aki Virkkula
Atmos. Meas. Tech., 12, 5913–5925,Short summary
Collection of particles onto filters can be a valuable tool in several research disciplines. Here we experiment with quartz filters and their response to soot particles in an airborne and liquid state in order to better understand the sampling procedure. Soot particles in a liquid phase showed absorption of light nearly double that of airborne sampled particles.
Sebastian Düsing, Birgit Wehner, Thomas Müller, Almond Stöcker, and Alfred Wiedensohler
Atmos. Meas. Tech., 12, 5879–5895,Short summary
This study examines the effect of changes in relative humidity on measurements made by two different filter-based absorption photometers. Different filter loads, loading materials, and filter types are considered. It was found that both instruments react opposingly and with different magnitudes. One of the devices showed a variation in the dependence on the loading material. For each of the two devices, a correction approach is provided. Recommendations based on the findings are given.
Alberto Sanchez-Marroquin, Duncan H. P. Hedges, Matthew Hiscock, Simon T. Parker, Philip D. Rosenberg, Jamie Trembath, Richard Walshaw, Ian T. Burke, James B. McQuaid, and Benjamin J. Murray
Atmos. Meas. Tech., 12, 5741–5763,Short summary
Sampling coarse-mode aerosol from a fast-moving research aircraft is challenging and can be subject to substantial losses and enhancements. We characterise these losses and enhancements for an inlet system designed to collect aerosol onto filters. We go on to present an application of this inlet system where we use electron microscopy to study the size and composition of the collected aerosol particles.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545,Short summary
We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Judith C. Chow, Junji Cao, L.-W. Antony Chen, Xiaoliang Wang, Qiyuan Wang, Jie Tian, Steven Sai Hang Ho, Adam C. Watts, Tessa B. Carlson, Steven D. Kohl, and John G. Watson
Atmos. Meas. Tech., 12, 5475–5501,Short summary
Source profiles that allow peat fire contributions to be distinguished from other source contributions using receptor models are lacking for a wide variety of peat fuels and burning conditions. These profiles change with photochemical aging during transport. Fresh and aged profiles for a variety of peat fuels are measured with an oxidation flow reactor to improve source attributions at distant receptors.
Alexandra J. Boris, Satoshi Takahama, Andrew T. Weakley, Bruno M. Debus, Carley D. Fredrickson, Martin Esparza-Sanchez, Charlotte Burki, Matteo Reggente, Stephanie L. Shaw, Eric S. Edgerton, and Ann M. Dillner
Atmos. Meas. Tech., 12, 5391–5415,Short summary
Organic species are abundant in atmospheric particle-phase (aerosol) pollution and originate from a variety of biogenic and anthropogenic sources. Infrared spectrometry of filter-based atmospheric particle samples can afford a direct measurement of the particulate organic matter concentration and a characterization of its composition. This work discusses recent method improvements and compositions measured in samples from the SouthEastern Aerosol Research and Characterization (SEARCH) network.
Seong-Jae Yoo, Hong-Beom Kwon, Ui-Seon Hong, Dong-Hyun Kang, Sang-Myun Lee, Jangseop Han, Jungho Hwang, and Yong-Jun Kim
Atmos. Meas. Tech., 12, 5335–5345,Short summary
We present a portable, inexpensive, and accurate microelectromechanical-system-based (MEMS-based) condensation particle counter (CPC) for the sensitive and precise monitoring of airborne ultrafine particles (UFPs). The CPC is miniaturized by utilizing MEMS technology and 3-D printing. Thus, the proposed system can potentially be used for UFP monitoring in various environments.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315,Short summary
Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Carmen Dameto de España, Gerhard Steiner, Harald Schuh, Constantinos Sioutas, and Regina Hitzenberger
Atmos. Meas. Tech., 12, 4733–4744,
Kelly L. Pereira, Grazia Rovelli, Young C. Song, Alfred W. Mayhew, Jonathan P. Reid, and Jacqueline F. Hamilton
Atmos. Meas. Tech., 12, 4519–4541,Short summary
We present the design and operation of a newly built continuous-flow reactor (CFR), which can be used as a tool to gain considerable insights into the composition and physical state of secondary organic aerosol (SOA). The CFR was used to generate large quantities of SOA mass, allowing the use of highly accurate techniques that are not usually accessible. We demonstrate how this unique approach can be used to investigate the relationship between SOA formation and physiochemical properties.
Alberto Baldelli and Steven Nicholas Rogak
Atmos. Meas. Tech., 12, 4339–4346,Short summary
Raman spectra and soot primary particle size change with the impactor sampling stage even though the soot source is a steady laboratory flame. This is of potential interest to atmospheric researchers because past work on aerodynamically separated samples was interpreted in terms of distinct particle sources producing particles of different sizes and chemical structures.
Daisy N. Grace, Melissa B. Sebold, and Melissa M. Galloway
Atmos. Meas. Tech., 12, 3841–3851,Short summary
The identification and quantification of compounds within an atmospheric particle can be difficult to achieve. We present a supercritical fluid chromatography method to separate these compounds prior to mass spectrometry analysis. The aqueous methylglyoxal–ammonium sulfate system was used as a proxy for atmospheric aerosol; polar columns combined with a carbon dioxide and methanol mobile phase provided the most efficient separation. This method can be extended to other atmospheric systems.
Christian Tauber, Sophia Brilke, Peter Josef Wlasits, Paulus Salomon Bauer, Gerald Köberl, Gerhard Steiner, and Paul Martin Winkler
Atmos. Meas. Tech., 12, 3659–3671,Short summary
In this paper we show that sodium chloride particles with a mobility diameter below 10 nm indicate different activation regimes. The results of our studies reveal that with increasing humidity the activation of NaCl particles with a standard butanol-based CPC can be enhanced. For Ag this humidity dependence could not be observed – an indicator for the importance of molecular interactions between seed and vapor molecules.
Theresa Haller, Christian Rentenberger, Jannik C. Meyer, Laura Felgitsch, Hinrich Grothe, and Regina Hitzenberger
Atmos. Meas. Tech., 12, 3503–3519,Short summary
In thermal–optical measurement techniques – widely used techniques to separate organic and elemental carbon – a filter sample is heated stepwise first in He and then in He+O2. Pyrolysis of organic material occurring during heating in He influences the results but is not fully understood. In this study, structural changes of carbonaceous material during a thermal–optical heating procedure are analyzed with Raman spectroscopy, TEM, UV–VIS and the integrating-sphere method.
Joseph L. Woo, Neha Sareen, Allison N. Schwier, and V. Faye McNeill
Atmos. Meas. Tech., 12, 3395–3402,Short summary
We present a proof-of-concept method of concentrating aerosols in a continuous stream using an applied electric field. Potential enrichment was estimated using a trajectory model, predicting values of up to 65 % for 75–200 nm aerosol, using voltages of up to 30 kV. Experimental results using similar geometry yielded up to 15 % observed enrichment for the same conditions. These results imply that aerosol enrichment using an applied electric field can be achieved in continuous-flow applications.
Dario Massabò, Alessandro Altomari, Virginia Vernocchi, and Paolo Prati
Atmos. Meas. Tech., 12, 3173–3182,
Christos Kaltsonoudis, Spiro D. Jorga, Evangelos Louvaris, Kalliopi Florou, and Spyros N. Pandis
Atmos. Meas. Tech., 12, 2733–2743,Short summary
A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers surrounded by UV lamps. The system has been designed to use ambient air as the starting point of the experiments. It can be easily disassembled and transported, enabling the study of various atmospheric environments and it can be used with natural sunlight. The results of test experiments using ambient air are discussed as examples of applications of this system.
Franz Friebel and Amewu A. Mensah
Atmos. Meas. Tech., 12, 2647–2663,Short summary
Simulating atmospheric aging processes in the laboratory under atmospheric conditions is a challenging task. The main obstacle is achieving long observation times with a reasonable amount of technical and financial input. We adapted the concept of the continuous-flow stirred tank reactor in order to achieve long observation times (up to 16 h) in small chamber volumes (3m3). We successfully tested this concept by oxidation of soot particles with ozone.
Michael I. Cotterell, Andrew J. Orr-Ewing, Kate Szpek, Jim M. Haywood, and Justin M. Langridge
Atmos. Meas. Tech., 12, 2371–2385,Short summary
Photoacoustic spectroscopy provides measurements of absorption coefficient for aerosol and gas samples but requires careful calibration, and researchers often use concentrations of ozone. Recent work has shown that the bath gas composition impacts the accuracy of this calibration at visible wavelengths. We explore further the role of bath gas, demonstrating that the calibration accuracy is optimal for a bath gas composed of 20 % oxygen and 80 % nitrogen at wavelengths of 405, 514 and 658 nm.
Rachel E. O'Brien, Kelsey J. Ridley, Manjula R. Canagaratna, John T. Jayne, Philip L. Croteau, Douglas R. Worsnop, Sri Hapsari Budisulistiorini, Jason D. Surratt, Christopher L. Follett, Daniel J. Repeta, and Jesse H. Kroll
Atmos. Meas. Tech., 12, 1659–1671,Short summary
Analysis of the elemental composition of organic mixtures can provide insights into the sources and aging of environmental samples. Here we describe a method that allows characterization of this type of material using micrograms of material by a combination of a small-volume ultrasonic nebulizer and an aerosol mass spectrometer. This technique enables rapid analysis of complex organic mixtures using approximately an order of magnitude less sample than standard analyses.
Jessica A. Mirrielees and Sarah D. Brooks
Atmos. Meas. Tech., 11, 6389–6407,Short summary
Particles in the air, called aerosols, can participate in cloud formation and affect cloud properties. One way to study these particles is by determining their ability to uptake water, called hygroscopicity. Apparent hygroscopicity is one such measurement. This study evaluates how errors can arise in determining apparent hygroscopicity and how to avoid or minimize them when collecting data.
Anna T. Kunert, Mark Lamneck, Frank Helleis, Ulrich Pöschl, Mira L. Pöhlker, and Janine Fröhlich-Nowoisky
Atmos. Meas. Tech., 11, 6327–6337,Short summary
The new Twin-plate Ice Nucleation Assay with infrared detection for high-throughput droplet freezing experiments in microliter-sized droplets is introduced, which was tested and characterized with bacterial and fungal ice nuclei. It was applied to investigate the influence of chemical processing on the activity of biological ice nuclei, and aqueous extracts of atmospheric aerosols were studied for ice nuclei activity.
Dario Massabò, Silvia Giulia Danelli, Paolo Brotto, Antonio Comite, Camilla Costa, Andrea Di Cesare, Jean François Doussin, Federico Ferraro, Paola Formenti, Elena Gatta, Laura Negretti, Maddalena Oliva, Franco Parodi, Luigi Vezzulli, and Paolo Prati
Atmos. Meas. Tech., 11, 5885–5900,
Alexander D. Harrison, Thomas F. Whale, Rupert Rutledge, Stephen Lamb, Mark D. Tarn, Grace C. E. Porter, Michael P. Adams, James B. McQuaid, George J. Morris, and Benjamin J. Murray
Atmos. Meas. Tech., 11, 5629–5641,Short summary
The detection of low concentrations of ice-nucleating particles (INPs) is challenging. Here we present a new technique (IR-NIPI) that is sensitive to low concentrations of INPs (> 0.01 L−1) and uses an infrared camera with a novel calibration to detect the freezing of experimental suspensions. IR-NIPI temperature measurements prove to be robust with a series of comparisons to thermocouple measurements. Experimental comparisons to other freezing assay instruments are also in agreement.
Andrea C. Wagner, Anton Bergen, Sophia Brilke, Claudia Fuchs, Markus Ernst, Jesica Hoker, Martin Heinritzi, Mario Simon, Bertram Bühner, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 11, 5489–5506,Short summary
Chemical analysis of sub-30 nm aerosol particles is important for understanding aerosol nucleation and early growth, yet it is still an experimental challenge. In this study, we present a novel device for size resolved chemical analysis of nucleation and Aitken mode particles (from ~10 to ~30 nm) while allowing gas phase measurements with the same detector. Particles are charged, size selected, electrostatically collected and then thermally desorbed in a carrier gas.
Michael Polen, Thomas Brubaker, Joshua Somers, and Ryan C. Sullivan
Atmos. Meas. Tech., 11, 5315–5334,Short summary
Ice nucleation commonly studied using droplet freezing measurements suffers from artifacts caused by water impurities or substrate effects. We evaluate a series of substrates and water sources to find methods that reduce the background freezing temperature limit. The best performance was obtained from our new microfluidic device and hydrophobic glass surfaces, using filtered HPLC bottled water. We conclude with recommendations for best practices in droplet freezing experiments and data analysis.
Ta-Chih Hsiao, Li-Hao Young, Yu-Chun Tai, and Po-Kai Chang
Atmos. Meas. Tech., 11, 4617–4626,Short summary
Ambient pressure and temperature can vary with location, which implies that classifying aerosol particle mass using APM might be influenced at high-altitude sites. On the other hand, when using the APM as a particle classifier coupled with inductively coupled plasma mass spectrometry, argon would be required as the carrier gas. Therefore, air, oxygen and carbon dioxide were selected as carrier gases to evaluate the effect of gas viscosity and the mean free path on the performance of APM.
Ramakrishna Ramisetty, Ahmed Abdelmonem, Xiaoli Shen, Harald Saathoff, Thomas Leisner, and Claudia Mohr
Atmos. Meas. Tech., 11, 4345–4360,Short summary
In this study we coupled a laser ablation aerosol time-of-flight (LAAPTOF) single-particle mass spectrometer, originally equipped with an excimer laser, to a femtosecond laser. The objective was to assess the influence of the higher laser power density of the femtosecond laser on ablation–ionization of atmospheric particles, ion signal, and ultimately quantitative abilities of the single-particle mass spectrometer.
Yue Zhang, Shachi Katira, Andrew Lee, Andrew T. Lambe, Timothy B. Onasch, Wen Xu, William A. Brooks, Manjula R. Canagaratna, Andrew Freedman, John T. Jayne, Doug R. Worsnop, Paul Davidovits, David Chandler, and Charles E. Kolb
Atmos. Meas. Tech., 11, 3479–3490,Short summary
We have adopted a new technique for measuring glass-forming properties of atmospherically relevant organic aerosols at submicron sizes and relatively low mass concentrations. Aerosol particles are deposited in the form of a thin film with interdigitated electrodes using electrostatic precipitation. Broadband dielectric spectroscopy is used to measure the kinetically controlled glass transition temperatures of glycerol and citric acid aerosols with three atmospheric relevant cooling rates.
Shouming Zhou, Jean C. Rivera-Rios, Frank N. Keutsch, and Jonathan P. D. Abbatt
Atmos. Meas. Tech., 11, 3081–3089,
Xiaoli Shen, Ramakrishna Ramisetty, Claudia Mohr, Wei Huang, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 11, 2325–2343,Short summary
This paper presents performance data and reference spectra from the commercially available single-particle mass spectrometer LAAPTOF. The main characteristics of the instrument, like its detection efficiency, are given for a wide particle size range. Furthermore, reference mass spectra for 32 well-defined different particle types relevant for atmospheric aerosol compounds are presented. It is shown that these reference mass spectra are very useful in analysis of atmospheric aerosol particles.
Agnieszka Kupc, Christina Williamson, Nicholas L. Wagner, Mathews Richardson, and Charles A. Brock
Atmos. Meas. Tech., 11, 369–383,
Naama Reicher, Lior Segev, and Yinon Rudich
Atmos. Meas. Tech., 11, 233–248,Short summary
Ice nucleating particles (INPs) affect the clouds' ice properties and can influence Earth’s hydrological cycle and climate. Here we present a detailed validation of WISDOM, a setup for the study of heterogeneous ice nucleation in an array of micron-sized droplets, and a demonstration of how it can be applied for the study of ice nucleation properties of ambient particles collected during dust storm events in Israel.
Nicholas A. Marsden, Michael J. Flynn, James D. Allan, and Hugh Coe
Atmos. Meas. Tech., 11, 195–213,Short summary
Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is lost. We introduce a novel technique that enables the online differentiation of mineral phase in silicate particles by single-particle mass spectrometry.
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The chemical composition of aerosols has implications for human and ecosystem health. Current methods for determining chemical composition are expensive and require highly trained personnel. Our method is promising for moderate-cost, low-maintenance measurements of oxygen / carbon ratios, a key chemical parameter, and other elements may also be studied. In this work, we coupled two commonly used detectors to assess O / C ratios in a variety of compounds and mixtures within an acceptable error.
The chemical composition of aerosols has implications for human and ecosystem health. Current...