Tight Coupling of Surface and In-Plant Biochemistry and Convection Governs Key Fine Particulate Components over the Amazon Rainforest

Shrivastava, ManishKumar B.; Quazi Ziaur Rasool, Fnu; Zhao, Bin; Octaviani, Mega; Zaveri, Rahul A.; Zelenyuk-Imre, Alla; Gaudet, Brian J.; Liu, Ying; Shilling, John E.; Schneider, Johannes; Schulz, Christiane; Zoeger, Martin; Martin, Scot T.; Ye, Jianhuai; Guenther, Alex B.; Souza, Rodrigo A.; Wendisch, Manfred; Poschl, Ulrich

doi:10.1021/acsearthspacechem.1c00356

Tight Coupling of Surface and In-Plant Biochemistry and Convection Governs Key Fine Particulate Components over the Amazon Rainforest

Journal Article · Wed Jan 12 04:00:00 EST 2022 · ACS Earth and Space Chemistry

DOI:https://doi.org/10.1021/acsearthspacechem.1c00356· OSTI ID:1855401

^[1]; ^[1]; Zhao, Bin ^[2]; Octaviani, Mega ^[3]; ^[1]; ^[1]; ^[1]; ^[1]; Shilling, John E. ^[1]; Schneider, Johannes ^[4]; Schulz, Christiane ^[4]; Zoeger, Martin ^[5]; Martin, Scot T. ^[6]; Ye, Jianhuai ^[7]; Guenther, Alex B. ^[8]; Souza, Rodrigo A. ^[9]; Wendisch, Manfred ^[10]; Poschl, Ulrich ^[4]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Tsinghua Univ., Beijing (China)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Karlsruhe Inst. of Technology (KIT) (Germany)
Max Planck Institute for Chemistry, Mainz (Germany)
German Aerospace Center (DLR), Oberpfaffenhofen (Germany)
Harvard Univ., Cambridge, MA (United States)
Harvard Univ., Cambridge, MA (United States); Southern University of Science and Technology (SUSTech), Shenzhen (China)
Univ. of California, Irvine, CA (United States)
Amazonas State Univ., Manaus (Brazil)
Univ. of Leipzig (Germany)

We report that throughout the troposphere over the Amazon rainforest, isoprene epoxydiol-secondary organic aerosols (IEPOX-SOA) are key components of submicrometer particle mass. IEPOX-SOA is thought to form by multiphase chemical pathways in the atmosphere, but using detailed model simulations, we show that these pathways are strongly inhibited by the solid particle phase state prevailing in the upper troposphere. We find that 2-methyltetrol gases formed by in-plant biochemical oxidation pathways, their partitioning to fine particles, and dissolution in cloud droplets can explain over 90% of IEPOX-SOA mass concentrations in the upper troposphere. In agreement with previous PM10 chiral measurements, our simulations indicate that plant biochemical processes are the dominant source of particulate 2-methyltetrols in the lower troposphere as well (>70%). Our results imply that in-plant biochemistry plays a central but previously unidentified role in aerosol processes and atmosphere-biosphere-climate interactions over the rainforest.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); Sao Paulo Research Foundation

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1855401

Report Number(s):: PNNL-SA-163479

Journal Information:: ACS Earth and Space Chemistry, Journal Name: ACS Earth and Space Chemistry Journal Issue: 2 Vol. 6; ISSN 2472-3452

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (46)

Recent advances in understanding secondary organic aerosol: Implications for global climate forcing: Advances in Secondary Organic Aerosol Shrivastava, Manish; Cappa, Christopher D.; Fan, Jiwen Reviews of Geophysics, Vol. 55, Issue 2 https://doi.org/10.1002/2016rg000540	journal	June 2017
Fully coupled “online” chemistry within the WRF model Grell, Georg A.; Peckham, Steven E.; Schmitz, Rainer Atmospheric Environment, Vol. 39, Issue 37 https://doi.org/10.1016/j.atmosenv.2005.04.027	journal	December 2005
Impact of Urban Pollution on Organic-Mediated New-Particle Formation and Particle Number Concentration in the Amazon Rainforest Zhao, Bin; Fast, Jerome D.; Donahue, Neil M. Environmental Science & Technology, Vol. 55, Issue 8 https://doi.org/10.1021/acs.est.0c07465	journal	March 2021
Ambient Gas-Particle Partitioning of Tracers for Biogenic Oxidation Isaacman-VanWertz, Gabriel; Yee, Lindsay D.; Kreisberg, Nathan M. Environmental Science & Technology, Vol. 50, Issue 18 https://doi.org/10.1021/acs.est.6b01674	journal	September 2016
The Cooling Rate- and Volatility-Dependent Glass-Forming Properties of Organic Aerosols Measured by Broadband Dielectric Spectroscopy Zhang, Yue; Nichman, Leonid; Spencer, Peyton Environmental Science & Technology, Vol. 53, Issue 21 https://doi.org/10.1021/acs.est.9b03317	journal	September 2019
A Near-Explicit Mechanistic Evaluation of Isoprene Photochemical Secondary Organic Aerosol Formation and Evolution: Simulations of Multiple Chamber Experiments with and without Added NO _x Thornton, Joel A.; Shilling, John E.; Shrivastava, Manish ACS Earth and Space Chemistry, Vol. 4, Issue 7 https://doi.org/10.1021/acsearthspacechem.0c00118	journal	June 2020
Modeling Volatility-Based Aerosol Phase State Predictions in the Amazon Rainforest Rasool, Quazi Z.; Shrivastava, Manish; Octaviani, Mega ACS Earth and Space Chemistry, Vol. 5, Issue 10 https://doi.org/10.1021/acsearthspacechem.1c00255	journal	September 2021
Modeling the Size Distribution and Chemical Composition of Secondary Organic Aerosols during the Reactive Uptake of Isoprene-Derived Epoxydiols under Low-Humidity Condition Octaviani, Mega; Shrivastava, Manish; Zaveri, Rahul A. ACS Earth and Space Chemistry, Vol. 5, Issue 11 https://doi.org/10.1021/acsearthspacechem.1c00303	journal	November 2021
Joint Impacts of Acidity and Viscosity on the Formation of Secondary Organic Aerosol from Isoprene Epoxydiols (IEPOX) in Phase Separated Particles Zhang, Yue; Chen, Yuzhi; Lei, Ziying ACS Earth and Space Chemistry, Vol. 3, Issue 12 https://doi.org/10.1021/acsearthspacechem.9b00209	journal	October 2019
Reactive Uptake of an Isoprene-Derived Epoxydiol to Submicron Aerosol Particles Gaston, Cassandra J.; Riedel, Theran P.; Zhang, Zhenfa Environmental Science & Technology, Vol. 48, Issue 19 https://doi.org/10.1021/es5034266	journal	September 2014
On the Reactive Uptake of Gaseous Compounds by Organic-Coated Aqueous Aerosols: Theoretical Analysis and Application to the Heterogeneous Hydrolysis of N ₂ O ₅ Anttila, Tatu; Kiendler-Scharr, Astrid; Tillmann, Ralf The Journal of Physical Chemistry A, Vol. 110, Issue 35 https://doi.org/10.1021/jp062403c	journal	September 2006
A computationally efficient Multicomponent Equilibrium Solver for Aerosols (MESA) Zaveri, Rahul A.; Easter, Richard C.; Peters, Leonard K. Journal of Geophysical Research, Vol. 110, Issue D24 https://doi.org/10.1029/2004jd005618	journal	January 2005
Evolution of ozone, particulates, and aerosol direct radiative forcing in the vicinity of Houston using a fully coupled meteorology-chemistry-aerosol model Fast, Jerome D.; Gustafson, William I.; Easter, Richard C. Journal of Geophysical Research, Vol. 111, Issue D21 https://doi.org/10.1029/2005jd006721	journal	January 2006
Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) Zaveri, Rahul A.; Easter, Richard C.; Fast, Jerome D. Journal of Geophysical Research, Vol. 113, Issue D13 https://doi.org/10.1029/2007jd008782	journal	January 2008
Temperature- and Humidity-Dependent Phase States of Secondary Organic Aerosols Petters, Sarah S.; Kreidenweis, Sonia M.; Grieshop, Andrew P. Geophysical Research Letters, Vol. 46, Issue 2 https://doi.org/10.1029/2018gl080563	journal	January 2019
Global distribution of particle phase state in atmospheric secondary organic aerosols Shiraiwa, Manabu; Li, Ying; Tsimpidi, Alexandra P. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15002	journal	April 2017
Urban pollution greatly enhances formation of natural aerosols over the Amazon rainforest Shrivastava, Manish; Andreae, Meinrat O.; Artaxo, Paulo Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08909-4	journal	March 2019
Glass transition and phase state of organic compounds: dependency on molecular properties and implications for secondary organic aerosols in the atmosphere Koop, Thomas; Bookhold, Johannes; Shiraiwa, Manabu Physical Chemistry Chemical Physics, Vol. 13, Issue 43 https://doi.org/10.1039/c1cp22617g	journal	January 2011
Primary and secondary organics in the tropical Amazonian rainforest aerosols: chiral analysis of 2-methyltetraols González, N. J. D.; Borg-Karlson, A. -K.; Artaxo, P. Environmental Science: Processes & Impacts, Vol. 16, Issue 6 https://doi.org/10.1039/c4em00102h	journal	January 2014
Near-canopy horizontal concentration heterogeneity of semivolatile oxygenated organic compounds and implications for 2-methyltetrols primary emissions Ye, Jianhuai; Batista, Carla E.; Guimarães, Patricia C. Environmental Science: Atmospheres, Vol. 1, Issue 1 https://doi.org/10.1039/d0ea00006j	journal	January 2021
Reactive intermediates revealed in secondary organic aerosol formation from isoprene Surratt, J. D.; Chan, A. W. H.; Eddingsaas, N. C. Proceedings of the National Academy of Sciences, Vol. 107, Issue 15 https://doi.org/10.1073/pnas.0911114107	journal	December 2009
Viscosity of -pinene secondary organic material and implications for particle growth and reactivity Renbaum-Wolff, L.; Grayson, J. W.; Bateman, A. P. Proceedings of the National Academy of Sciences, Vol. 110, Issue 20 https://doi.org/10.1073/pnas.1219548110	journal	April 2013
Integrating phase and composition of secondary organic aerosol from the ozonolysis of -pinene Kidd, C.; Perraud, V.; Wingen, L. M. Proceedings of the National Academy of Sciences, Vol. 111, Issue 21 https://doi.org/10.1073/pnas.1322558111	journal	May 2014
Rapid deposition of oxidized biogenic compounds to a temperate forest Nguyen, Tran B.; Crounse, John D.; Teng, Alex P. Proceedings of the National Academy of Sciences, Vol. 112, Issue 5 https://doi.org/10.1073/pnas.1418702112	journal	January 2015
Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru Proceedings of the National Academy of Sciences, Vol. 113, Issue 43 https://doi.org/10.1073/pnas.1602360113	journal	October 2016
High concentration of ultrafine particles in the Amazon free troposphere produced by organic new particle formation Zhao, Bin; Shrivastava, Manish; Donahue, Neil M. Proceedings of the National Academy of Sciences, Vol. 117, Issue 41 https://doi.org/10.1073/pnas.2006716117	journal	September 2020
Within‐plant isoprene oxidation confirmed by direct emissions of oxidation products methyl vinyl ketone and methacrolein Jardine, Kolby J.; Monson, Russell K.; Abrell, Leif Global Change Biology, Vol. 18, Issue 3 https://doi.org/10.1111/j.1365-2486.2011.02610.x	journal	November 2011
Formation of Secondary Organic Aerosols Through Photooxidation of Isoprene Claeys, M. Science, Vol. 303, Issue 5661 https://doi.org/10.1126/science.1092805	journal	February 2004
A Comprehensive Mass Flux Scheme for Cumulus Parameterization in Large-Scale Models Tiedtke, M. Monthly Weather Review, Vol. 117, Issue 8 https://doi.org/10.1175/1520-0493(1989)117<1779:acmfsf>2.0.co;2	journal	August 1989
ACRIDICON–CHUVA Campaign: Studying Tropical Deep Convective Clouds and Precipitation over Amazonia Using the New German Research Aircraft HALO Wendisch, Manfred; Pöschl, Ulrich; Andreae, Meinrat O. Bulletin of the American Meteorological Society, Vol. 97, Issue 10 https://doi.org/10.1175/bams-d-14-00255.1	journal	October 2016
Impact of Aerosol-Cloud Cycling on Aqueous Secondary Organic Aerosol Formation Tsui, William G.; Woo, Joseph L.; McNeill, V. Faye Atmosphere, Vol. 10, Issue 11 https://doi.org/10.3390/atmos10110666	journal	October 2019
Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): a review of laboratory, field and model studies Ervens, B.; Turpin, B. J.; Weber, R. J. Atmospheric Chemistry and Physics, Vol. 11, Issue 21 https://doi.org/10.5194/acp-11-11069-2011	journal	January 2011
Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements Hu, W. W.; Campuzano-Jost, P.; Palm, B. B. Atmospheric Chemistry and Physics, Vol. 15, Issue 20 https://doi.org/10.5194/acp-15-11807-2015	journal	January 2015
Observation of viscosity transition in α -pinene secondary organic aerosol Järvinen, Emma; Ignatius, Karoliina; Nichman, Leonid Atmospheric Chemistry and Physics, Vol. 16, Issue 7 https://doi.org/10.5194/acp-16-4423-2016	journal	January 2016
Introduction: Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) Martin, S. T.; Artaxo, P.; Machado, L. A. T. Atmospheric Chemistry and Physics, Vol. 16, Issue 8 https://doi.org/10.5194/acp-16-4785-2016	journal	January 2016
Aircraft observations of the chemical composition and aging of aerosol in the Manaus urban plume during GoAmazon 2014/5 Shilling, John E.; Pekour, Mikhail S.; Fortner, Edward C. Atmospheric Chemistry and Physics, Vol. 18, Issue 14 https://doi.org/10.5194/acp-18-10773-2018	journal	January 2018
Aircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region Schulz, Christiane; Schneider, Johannes; Amorim Holanda, Bruna Atmospheric Chemistry and Physics, Vol. 18, Issue 20 https://doi.org/10.5194/acp-18-14979-2018	journal	January 2018
Aerosol characteristics and particle production in the upper troposphere over the Amazon Basin Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel Atmospheric Chemistry and Physics, Vol. 18, Issue 2 https://doi.org/10.5194/acp-18-921-2018	journal	January 2018
Chamber-based insights into the factors controlling epoxydiol (IEPOX) secondary organic aerosol (SOA) yield, composition, and volatility D'Ambro, Emma L.; Schobesberger, Siegfried; Gaston, Cassandra J. Atmospheric Chemistry and Physics, Vol. 19, Issue 17 https://doi.org/10.5194/acp-19-11253-2019	journal	January 2019
A new model mechanism for atmospheric oxidation of isoprene: global effects on oxidants, nitrogen oxides, organic products, and secondary organic aerosol Bates, Kelvin H.; Jacob, Daniel J. Atmospheric Chemistry and Physics, Vol. 19, Issue 14 https://doi.org/10.5194/acp-19-9613-2019	journal	January 2019
An evaluation of global organic aerosol schemes using airborne observations Pai, Sidhant J.; Heald, Colette L.; Pierce, Jeffrey R. Atmospheric Chemistry and Physics, Vol. 20, Issue 5 https://doi.org/10.5194/acp-20-2637-2020	journal	January 2020
Future changes in isoprene-epoxydiol-derived secondary organic aerosol (IEPOX SOA) under the Shared Socioeconomic Pathways: the importance of physicochemical dependency Jo, Duseong S.; Hodzic, Alma; Emmons, Louisa K. Atmospheric Chemistry and Physics, Vol. 21, Issue 5 https://doi.org/10.5194/acp-21-3395-2021	journal	January 2021
A review of Secondary Organic Aerosol (SOA) formation from isoprene Carlton, A. G.; Wiedinmyer, C.; Kroll, J. H. Atmospheric Chemistry and Physics, Vol. 9, Issue 14 https://doi.org/10.5194/acp-9-4987-2009	journal	January 2009
Comparison of aircraft measurements during GoAmazon2014/5 and ACRIDICON-CHUVA Mei, Fan; Wang, Jian; Comstock, Jennifer M. Atmospheric Measurement Techniques, Vol. 13, Issue 2 https://doi.org/10.5194/amt-13-661-2020	journal	January 2020
Isoprene-derived secondary organic aerosol in the global aerosol–chemistry–climate model ECHAM6.3.0–HAM2.3–MOZ1.0 Stadtler, Scarlet; Kühn, Thomas; Schröder, Sabine Geoscientific Model Development, Vol. 11, Issue 8 https://doi.org/10.5194/gmd-11-3235-2018	journal	January 2018
The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions Guenther, A. B.; Jiang, X.; Heald, C. L. Geoscientific Model Development, Vol. 5, Issue 6 https://doi.org/10.5194/gmd-5-1471-2012	journal	January 2012

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Tight Coupling of Surface and In-Plant Biochemistry and Convection Governs Key Fine Particulate Components over the Amazon Rainforest

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