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

Author(s):Show less -

Shrivastava, Manish ^[1] ; Rasool, Quazi Z. ^[1] ; Zhao, Bin ^{[1, 2]} ; Octaviani, Mega ^{[1, 3]} ; Zaveri, Rahul A. ^[1] ; Zelenyuk, Alla ^[1] ; Gaudet, Brian ^[1] ; Liu, Ying ^[1] ; Shilling, John E. ^[1] ; Schneider, Johannes ^[4] ; Schulz, Christiane ^{[4, 5, 6]} ; Zoeger, Martin ^[7] ; Martin, Scot T. ^{[8, 9]} ; Ye, Jianhuai ^{[8, 9, 10]} ; Guenther, Alex ^[11] ; Souza, Rodrigo F. ^[12] ; Wendisch, Manfred ^[13] ; Poeschl, Ulrich ^[14]

Affiliation:Show less -

^[1] Pacific Northwest Natl Lab, Richland, WA 99352 - USA

^[2] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084 - Peoples R China

^[3] Karlsruhe Inst Technol, Inst Meteorol & Climate Res, Dept Troposphere Res, D-76344 Eggenstein Leopoldshafen - Germany

^[4] Max Planck Inst Chem, Particle Chem Dept, D-55128 Mainz - Germany

^[5] Leibniz Inst Tropospher Res, Expt Aerosol & Cloud Microphys Dept, D-04318 Leipzig - Germany

^[6] Leibniz Ctr Agr Landscape Res, D-15374 Muncheberg - Germany

^[7] German Aerosp Ctr DLR, Flight Expt, D-82234 Oberpfaffenhofen - Germany

^[8] Harvard Univ, Sch Engn & Appl Sci, Cambridge, MA 02138 - USA

^[9] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 - USA

^[10] Southern Univ Sci & Technol, Sch Environm Sci & Engn, Shenzhen 518055, Guangdong - Peoples R China

^[11] Univ Calif Irvine, Dept Earth Syst Sci, Irvine, CA 92697 - USA

^[12] Amazonas State Univ, Super Sch Technol, BR-69050020 Manaus, Amazonas - Brazil

^[13] Univ Leipzig, Leipzig Inst Meteorol, D-04103 Leipzig - Germany

^[14] Max Planck Inst Chem, Multiphase Chem Dept, D-55128 Mainz - Germany

• Document type: Journal article
• Source: ACS EARTH AND SPACE CHEMISTRY; v. 6, n. 2, p. 380-390, FEB 17 2022.
• Web of Science Citations: 0

Abstract

Combining unique high-altitude aircraft measurements and detailed regional model simulations, we show that inplant biochemistry plays a central but previously unidentified role in fine particulate-forming processes and atmosphere-biosphere- climate interactions over the Amazon rainforest. Isoprene epoxydiol secondary organic aerosols (IEPOX-SOA) are key components of sub-micrometer aerosol particle mass throughout the troposphere over the Amazon rainforest and are traditionally thought to form by multiphase chemical pathways. Here, we show that these pathways are strongly inhibited by the solid thermodynamic phase state of aerosol particles and lack of particle and cloud liquid water in the upper troposphere. Strong diffusion limitations within organic aerosol coatings prevailing at low temperatures and low relative humidity in the upper troposphere strongly inhibit the reactive uptake of IEPOX to inorganic aerosols. We find that direct emissions of 2-methyltetrol gases formed by in-plant biochemical oxidation and/or oxidation of deposited IEPOX gases on the surfaces of soils and leaves and their transport by cloud updrafts followed by their condensation at low temperatures could explain over 90% of the IEPOX-SOA mass concentrations in the upper troposphere. Our simulations indicate that even near the surface, direct emissions of 2-methyltetrol gases represent a ubiquitous, but previously unaccounted for, source of IEPOX-SOA. Our results provide compelling evidence for new pathways related to land surface-aerosol-cloud interactions that have not been considered previously. (AU)

• FAPESP's process: 13/05014-0 - GoAmazon: interactions of the urban plume of Manaus with biogenic forest emissions in Amazonia
• Grantee: Paulo Eduardo Artaxo Netto
• Support Opportunities: Research Program on Global Climate Change - Thematic Grants
• FAPESP's process: 09/15235-8 - Cloud processes of the main precipitation systems in Brazil: a contribution to cloud resolving modeling and to the GPM (Global Precipitation Measurement)
• Grantee: Luiz Augusto Toledo Machado
• Support Opportunities: Research Projects - Thematic Grants