A Molecular-to-Regional Scale Understanding of Secondary Organic Aerosol Formation
EMSL Project ID
49297
Abstract
Our hypothesis is that a better understanding of fast-reacting processes is needed to make a breakthrough in parameterizing secondary organic aerosols (SOA) for the next generation climate models. To investigate this hypothesis, we propose to analyze unique EMSL data sets to be collected in the vicinity of the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in Oklahoma during the summer of 2016 as part of the Holistic Interactions of Shallow Clouds, Aerosol, and Land-Ecosystems (HI-SCALE) field campaign. Extensive measurements of size, chemical composition, volatility, viscosity, and mixing state of ambient non-refractory and refractory atmospheric aerosols will be obtained through on-line mass spectrometry, using EMSL's HR-ToF-AMS, miniSPLAT, and SPLAT II instruments. The EMSL datasets will also be used to evaluate SOA predicted by Large-Eddy-Simulation (LES, delta-x = 10 - 100 m) and regional-scale (delta-x ~ 1 - 10 km) models that use both state-of-the-science and new parameterizations of SOA. Since it is computationally prohibitive for climate models to explicitly account for thousands of chemical reactions likely associated with SOA formation and transformation, the new insights obtained from the field measurements will instead be used to better constrain model parameterizations of SOA. We expect that analyses of HI-SCALE data and the model simulations of the conditions observed during HI-SCALE will enable new insights into the molecular-level understanding of gas-to-particle partitioning, aerosol mixing state, and aging over multiple time scales associated with coupling turbulent mixing within convective eddies (seconds to minutes), diurnal photochemistry and emission rates, and multi-day chemical processing associated with variable meteorological conditions. Understanding SOA is particularly important for climate models when coupled with the uncertainties in cloud predictions. In the SGP and in many other regions of the world, cumulus convection is an important component in the atmospheric radiation budget and hydrologic cycle - particularly during the summertime growing season when intense turbulence induced by surface radiation couples the land surface to clouds. Regional and global climate models cannot explicitly resolve shallow and deep convective clouds; consequently, parameterizations are required to represent the vertical mixing of atmospheric constituents, precipitation, and radiative effects associated with convective clouds. Nor do they adequately represent aerosols, particularly the properties of SOA, which subsequently influences the radiation budget through the direct and indirect effects. SOA has also been shown to be a large fraction of the total aerosol burden in many places of the world and the fraction of SOA associated with the enhancement of biogenic SOA by anthropogenic emissions still remains highly uncertain. Current models rely on crude assumptions regarding SOA formation processes, volatility, phase, and mixing state that lead to uncertainties in their ability to act CCN. In addition, the relatively coarse spatial resolution of these models ignores fast chemical processes that control the initial stages of SOA formation and growth. Therefore, errors in representing SOA microphysical and chemical properties in formation regions could eventually result in larger errors in cloud properties and the radiation budget further downwind.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2019-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Berg L.K., J.D. Fast, W.I. Gustafson, H. Xiao, Z. Feng, H.C. Barnes, and J. Kleiss, et al. 04/09/2018. "Large Eddy Simulation of Shallow to Deep Convective Cloud Transitions during HI-SCALE." Presented by Larry K Berg at EGU, Vienna, Austria. PNNL-SA-133441.
Chen J., S.M. Hagos, H. Xiao, J.D. Fast, and Z. Feng. 01/15/2020. "Characteristics of Surface Heterogeneity Induced Convection." Presented by J. Chen at Wayne Schubert Symposium in conjunction with the 100th Annual American Meteorological Society Meeting, Boston, Massachusetts. PNNL-SA-150366.
Chen J., S.M. Hagos, H. Xiao, R.A. Houze, J.D. Fast, and Z. Feng. 06/10/2019. "Investigating the Mechanisms of Shallow Precipitating Clouds Formation during the HI-SCALE Field Campaign." Bethesda, Maryland. PNNL-SA-144262.
Fast J D,Berg L K,Alexander L ,D'Ambro E ,Bell D M,Brown E ,Eiguren A ,Hubbe J M,Kuang C ,Lindenmaier R ,Liu J ,Matthews A A,Mei F ,Pekour M S,Pinterich T ,Schmid B ,Schobesberger S ,Shilling J E,Smith J N,Springston S ,Stark H ,Suski K J,Thornton J A,Wang J ,Zelenyuk-Imre A 2016. "The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Campaign: Measurement Strategy and Preliminary Findings"
Fast J D,Berg L K,Schmid B ,Alexander L ,Bell D M,D'Ambro E ,Hubbe J M,Liu J ,Mei F ,Pekour M S,Pinterich T ,Schobesberger S ,Shilling J E,Springston S R,Thornton J A,Tomlinson J M,Wang J ,Zelenyuk-Imre A 2016. "The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems Campaign: Measurement Strategy and Preliminary Findings "
Fast J.D., H. Xiao, J. Chen, M.B. Shrivastava, and R.A. Scanza. 08/09/2018. "WRF-LES-Chem Over the Southern Great Plains." Presented by J.D. Fast at Future Role of Large-Eddy Simulations (LES) models for Air Quality Workshop, Boulder, Colorado. PNNL-SA-137107.
Fast J.D., L.A. Berg, R.K. Newsom, H. Xiao, S. Tai, and J.D. Tagestad. 06/12/2018. "Observed and Simulated Heterogeneity in Boundary Layer Turbulence and Shallow Convective Clouds during the HI-SCALE Campaign." Presented by Jerome D Fast at 23 Symposium on Boundar Layers and Turbulence, Oklahoma City, Oklahoma. PNNL-SA-135769.
Fast JD, LK Berg, B Schmid, L Alexander, DM Bell, E D'Ambro, JM Hubbe, J Liu, F Mei, MS Pekour, T Pinterich, S Schobesberger, JE Shilling, SR Springston, JA Thornton, JM Tomlinson, J Wang, and A Zelenyuk-Imre. 2016. "Improving the Understanding and Model Representation of Processes that Couple Shallow Clouds, Aerosols, and Land-Ecosystems ." Abstract submitted to American Geophysical Union Fall Meeting, SAN FRANCISCO, CA. PNNL-SA-119981.
Fast JD, LK Berg, B Schmid, LJ Alexander, E D'Ambro, DM Bell, A Eiguren, JM Hubbe, C Kuang, R Lindenmaier, J Liu, AA Matthews, F Mei, MS Pekour, T Pinterich, S Schobesberger, JE Shilling, JN Smith, S Springston, H Stark, KJ Suski, JA Thornton, J Wang, and A Zelenyuk-Imre. 2017. "The Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) Campaign: Measurement Strategy and Preliminary Findings." Presented by Jerome D Fast at ARM/ASR PI Meeting, FAIRFAX, VA on March 14, 2017. PNNL-SA-124558.
Fast J.D., L.K. Berg, D.M. Bell, B.H. Lee, J. Liu, F. Mei, and J.E. Shilling, et al. 01/10/2018. "Aerosol-Cloud Interactions Observed during the Holistic Interactions of Shallow Clouds, Aerosols, and Land Ecosystems (HI-SCALE) Campaign." Abstract submitted to American Meteorological Society, Austin, Texas. PNNL-SA-131625.
Fast J.D., L.K. Berg, H.C. Barnes, Z. Feng, W.I. Gustafson, and H. Xiao. 12/13/2018. "Comparison of LES Methodologies in the Representation of Shallow Convective Cloud Populations Observed during the HI-SCALE Campaign." Presented by J.D. Fast at AGU Fall Meeting, Washington, District Of Columbia. PNNL-SA-140040.
Fast J.D., L.K. Berg, J. Chen, R.K. Newsom, M.S. Pekour, J.D. Tagestad, and S. Tai, et al. 12/11/2018. "Observed and Simulated Coupling of Land-Atmosphere Interactions, Boundary Layer Turbulence, and Shallow Convective Clouds during HI-SCALE." Abstract submitted to American Geophysical Union, Washington, District Of Columbia. PNNL-SA-136824.
Fast J.D., L.K. Berg, W.I. Gustafson, H. Xiao, S. Endo, Z. Feng, and H.C. Barnes, et al. 03/20/2018. "Large Eddy Simulations of Shallow to Deep Convective Cloud Transitions during HI-SCALE." Presented by Jerome D Fast at 2018 ARM/ASR Principal Investigator Meeting, Vienna, Virginia. PNNL-SA-135573.
Fast, J., L. Berg, L. Alexander, D. Bell, E. D’Ambro, J. Hubbe, C. Kuang, J. Liu, C. Long, A. Matthews, F. Mei, R. Newsom, M. Pekour, T. Pinterich, B. Schmid, S. Schobesberger, J. Shilling, J. Smith, S. Springston, K. Suski, J. Thornton, J. Tomlinson, J. Wang, H. Xiao, and A. Zelenyuk, 2018: Overview of the HI-SCALE Field Campaign: A New Perspective on Shallow Convective Clouds. Bull. Amer. Meteor. Soc. doi:10.1175/BAMS-D-18-0030.1, in press.
Shrivastava, M., A. Zelenyuk-Imre, D. Bell, J. Fast, J. Thornton, D. Imre, K. Suski, L. Berg, J. Shilling, J. Liu, F. Mei, J. Tomlinson, and J. Wang, 2018: Insights into isoprene-epoxydiol (IEPOX-SOA) chemistry in cloud droplets using WRF-Chem and HI-SCALE field observations. Poster. ARM/ASR Principal Investigator Meeting, Vienna, VA, March 19 - 23. PNNL-SA-131946.
Shrivastava M.B., A. Zelenyuk-Imre, D.M. Bell, J.D. Fast, J.A. Thornton, D.g. Imre, and K.J. Suski, et al. 09/04/2018. "Insights into Isoprene-Epoxydiol (IEPOX-SOA) chemistry in Cloud Droplets using WRF-Chem and HI-SCALE field observations." Abstract submitted to International Aerosol Conference 2018, St. Louis, Moscow. PNNL-SA-132081.
Wang H. C.D. Burleyson P. Ma J.D. Fast and P.J. Rasch. 2018. Using the Atmospheric Radiation Measurement (ARM) Datasets to Evaluate Climate Models in Simulating Diurnal and Seasonal Variations of Tropical Clouds." Journal of Climate 31 no. 8:3301–3325. PNNL-SA-125329. doi:10.1175/JCLI-D-17-0362.1
Zelenyuk-Imre, A., D. Bell, M. Shrivastava, J. Fast, J. Thornton, K. Suski, D. Imre, L. Berg, J. Shilling, J. Liu, F. Mei, J. Tomlinson, J. Wang, and M. Pekour, 2018: Direct observations of the formation of isoprene-derived secondary organic aerosol in ambient cloud droplets. Poster. ARM/ASR Principal Investigator Meeting, Vienna, VA, March 19 - 23.
Zelenyuk-Imre A., D.M. Bell, M.B. Shrivastava, J.D. Fast, J.A. Thornton, D. Imre, and K.J. Suski, et al. 09/04/2018. "Direct Observations of the Formation of Isoprene-derived Secondary Organic Aerosol in Ambient Cloud Droplets." Abstract submitted to 2018 International Aerosol Conference, St Louis, Mississippi. PNNL-SA-135148.