Articles | Volume 14, issue 6
https://doi.org/10.5194/amt-14-4355-2021
© Author(s) 2021. 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-14-4355-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Quantifying organic matter and functional groups in particulate matter filter samples from the southeastern United States – Part 2: Spatiotemporal trends
Air Quality Research Center, University of California, Davis, Davis, CA 95616, USA
Satoshi Takahama
Ecole Polytechnique Federale de Lausanne, Lausanne, Switzerland
Andrew T. Weakley
Air Quality Research Center, University of California, Davis, Davis, CA 95616, USA
Bruno M. Debus
Air Quality Research Center, University of California, Davis, Davis, CA 95616, USA
Stephanie L. Shaw
Electric Power Research Institute, Palo Alto, CA 94304, USA
Eric S. Edgerton
Atmospheric Research & Analysis, Inc., Cary, NC 27513, USA
Taekyu Joo
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA
Nga L. Ng
School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA 30332, USA
School of Chemical and Bimolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA
School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA
Ann M. Dillner
Air Quality Research Center, University of California, Davis, Davis, CA 95616, USA
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Wendell W. Walters, Masayuki Takeuchi, Danielle E. Blum, Gamze Eris, David Tanner, Weiqi Xu, Jean Rivera-Rios, Fobang Liu, Tianchang Xu, Greg Huey, Justin B. Min, Rodney Weber, Nga L. Ng, and Meredith G. Hastings
Atmos. Chem. Phys., 25, 10707–10730, https://doi.org/10.5194/acp-25-10707-2025, https://doi.org/10.5194/acp-25-10707-2025, 2025
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We studied how chemicals released from plants and pollution interact in the atmosphere, affecting air quality and climate. By combining laboratory experiments and chemistry models, we tracked unique chemical fingerprints to understand how nitrogen compounds transform to form particles in the air. Our findings help explain the role of these reactions in pollution and provide tools to improve predictions for cleaner air and better climate policies.
Yuting Lyu, Taekyu Joo, Ruihan Ma, Mark Kristan Espejo Cabello, Tianye Zhou, Shun Yeung, Cheuk Ki Wong, Yifang Gu, Yiming Qin, and Theodora Nah
Atmos. Chem. Phys., 25, 10731–10745, https://doi.org/10.5194/acp-25-10731-2025, https://doi.org/10.5194/acp-25-10731-2025, 2025
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We investigated the aqueous nitrate-mediated photooxidation of four green leaf volatiles (GLVs). The aqueous reaction medium conditions, dilute cloud/fog vs. concentrated aqueous aerosol conditions, governed the effects that pH, ionic strength, and sulfate have on the GLV degradation rates and aqueous secondary organic aerosol (aqSOA) mass yields. Most notably, reactions initiated by sulfate photolysis have significant effects in aqueous aerosols but not in cloud/fog droplets.
Yuchen Wang, Xiang Zhang, Yuanlong Huang, Yutong Liang, and Nga L. Ng
Atmos. Chem. Phys., 25, 5215–5231, https://doi.org/10.5194/acp-25-5215-2025, https://doi.org/10.5194/acp-25-5215-2025, 2025
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This work provides the first fundamental laboratory data to evaluate SOA (secondary organic aerosol) production from styrene and NO3 chemistry. Additionally, the formation mechanisms of aromatic organic nitrates (ONs) are reported, highlighting that previously identified nitroaromatics in ambient field campaigns can be aromatic ONs. Finally, the hydrolysis lifetimes observed for ONs generated from styrene and NO3 oxidation can serve as experimentally constrained parameters for modeling hydrolysis of aromatic ONs in general.
Nagendra Raparthi, Anthony S. Wexler, and Ann M. Dillner
Atmos. Meas. Tech., 18, 603–618, https://doi.org/10.5194/amt-18-603-2025, https://doi.org/10.5194/amt-18-603-2025, 2025
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Quantifying the composition-dependent hygroscopicity of aerosol particles is essential for advancing our understanding of atmospheric processes. Existing methods do not integrate chemical composition with hygroscopicity. We developed a novel method to assess the water uptake of particles sampled on aerosol filters at relative humidity levels up to 97 % and link it with their composition. This approach allows for the separation of total water uptake into inorganic and organic components.
Wendell W. Walters, Masayuki Takeuchi, Nga L. Ng, and Meredith G. Hastings
Geosci. Model Dev., 17, 4673–4687, https://doi.org/10.5194/gmd-17-4673-2024, https://doi.org/10.5194/gmd-17-4673-2024, 2024
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The study introduces a novel chemical mechanism for explicitly tracking oxygen isotope transfer in oxidized reactive nitrogen and odd oxygen using the Regional Atmospheric Chemistry Mechanism, version 2. This model enhances our ability to simulate and compare oxygen isotope compositions of reactive nitrogen, revealing insights into oxidation chemistry. The approach shows promise for improving atmospheric chemistry models and tropospheric oxidation capacity predictions.
Emily Y. Li, Amir Yazdani, Ann M. Dillner, Guofeng Shen, Wyatt M. Champion, James J. Jetter, William T. Preston, Lynn M. Russell, Michael D. Hays, and Satoshi Takahama
Atmos. Meas. Tech., 17, 2401–2413, https://doi.org/10.5194/amt-17-2401-2024, https://doi.org/10.5194/amt-17-2401-2024, 2024
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Infrared spectroscopy is a cost-effective measurement technique to characterize the chemical composition of organic aerosol emissions. This technique differentiates the organic matter emission factor from different fuel sources by their characteristic functional groups. Comparison with collocated measurements suggests that polycyclic aromatic hydrocarbon concentrations in emissions estimated by conventional chromatography may be substantially underestimated.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Yutong Liang, Rebecca A. Wernis, Kasper Kristensen, Nathan M. Kreisberg, Philip L. Croteau, Scott C. Herndon, Arthur W. H. Chan, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12441–12454, https://doi.org/10.5194/acp-23-12441-2023, https://doi.org/10.5194/acp-23-12441-2023, 2023
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We measured the gas–particle partitioning behaviors of biomass burning markers and examined the effect of wildfire organic aerosol on the partitioning of semivolatile organic compounds. Most compounds measured are less volatile than model predictions. Wildfire aerosol enhanced the condensation of polar compounds and caused some nonpolar (e.g., polycyclic aromatic hydrocarbons) compounds to partition into the gas phase, thus affecting their lifetimes in the atmosphere and the mode of exposure.
Marife B. Anunciado, Miranda De Boskey, Laura Haines, Katarina Lindskog, Tracy Dombek, Satoshi Takahama, and Ann M. Dillner
Atmos. Meas. Tech., 16, 3515–3529, https://doi.org/10.5194/amt-16-3515-2023, https://doi.org/10.5194/amt-16-3515-2023, 2023
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Organic sulfur compounds are used to identify sources and atmospheric processing of aerosol. Our paper evaluates the potential of using a non-destructive measurement technique to measure organic sulfur compounds in filter samples by assessing their chemical stability over time. Some were stable, but some evaporated or changed chemically. Future work includes evaluating the stability and potential interference of multiple organic sulfur compounds in laboratory mixtures and ambient aerosol.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
Nikunj Dudani and Satoshi Takahama
Atmos. Meas. Tech., 15, 4693–4707, https://doi.org/10.5194/amt-15-4693-2022, https://doi.org/10.5194/amt-15-4693-2022, 2022
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We designed and fabricated an aerosol collector with high collection efficiency that enables quantitative infrared spectroscopy analysis. By collecting particles on optical windows, typical substrate interferences are eliminated. New methods for fabricating aerosol devices using 3D printing with post-treatment to reduce the time and cost of prototyping are described.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Bruno Debus, Andrew T. Weakley, Satoshi Takahama, Kathryn M. George, Anahita Amiri-Farahani, Bret Schichtel, Scott Copeland, Anthony S. Wexler, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2685–2702, https://doi.org/10.5194/amt-15-2685-2022, https://doi.org/10.5194/amt-15-2685-2022, 2022
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In the US, routine particulate matter composition is measured on samples collected on three types of filter media and analyzed using several techniques. We propose an alternate approach that uses one analytical technique, Fourier transform-infrared spectroscopy (FT-IR), and one filter type to measure the chemical composition of particulate matter in a major US monitoring network. This method could be used to add low-cost sites to the network, fill-in missing data, or for quality control.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
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Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
Amir Yazdani, Ann M. Dillner, and Satoshi Takahama
Atmos. Meas. Tech., 14, 4805–4827, https://doi.org/10.5194/amt-14-4805-2021, https://doi.org/10.5194/amt-14-4805-2021, 2021
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We propose a spectroscopic method for estimating several mixture-averaged molecular properties (carbon number and molecular weight) in particulate matter relevant for understanding its chemical origins. This estimation is enabled by calibration models built and tested using laboratory standards containing molecules with known structure, and can be applied to filter samples of PM2.5 currently collected in existing air pollution monitoring networks and field campaigns.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Weiqi Xu, Masayuki Takeuchi, Chun Chen, Yanmei Qiu, Conghui Xie, Wanyun Xu, Nan Ma, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Meas. Tech., 14, 3693–3705, https://doi.org/10.5194/amt-14-3693-2021, https://doi.org/10.5194/amt-14-3693-2021, 2021
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Here we developed a method for estimation of particulate organic nitrates (pON) from the measurements of a high-resolution aerosol mass spectrometer coupled with a thermodenuder based on the volatility differences between inorganic nitrate and pON. The results generally had improvements in reducing negative values due to the influences of a high concentration of inorganic nitrate and a constant ratio of NO+ to NO2+ of organic nitrates (RON).
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Thomas Berkemeier, Masayuki Takeuchi, Gamze Eris, and Nga L. Ng
Atmos. Chem. Phys., 20, 15513–15535, https://doi.org/10.5194/acp-20-15513-2020, https://doi.org/10.5194/acp-20-15513-2020, 2020
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This paper presents how environmental chamber data of secondary organic aerosol (SOA) formation can be interpreted using kinetic modeling techniques. Utilizing pure and mixed precursor experiments, we show that SOA formation and evaporation can be understood by explicitly treating gas-phase chemistry, gas–particle partitioning, and, notably, particle-phase oligomerization, but some of the non-linear, non-equilibrium effects must be accredited to diffusion limitations in the particle phase.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
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Short summary
Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give comprehensive characterization of the organic material by bond rather than species. Using this technique, the concentrations of particle organic material were found to decrease 2011–2016 in the southeastern US, driven by a decline in highly aged material, concurrent with declining anthropogenic emissions. However, an increase was observed in the fraction of more moderately aged organic matter.
Infrared spectrometry can be applied in routine monitoring of atmospheric particles to give...