Abstract
Aerosols significantly influence atmospheric processes such as cloud nucleation, heterogeneous chemistry, and heavy-metal transport in the troposphere. The chemical and physical complexity of atmospheric aerosols results in large uncertainties in their climate and health effects. In this article, we review recent advances in scientific understanding of aerosol processes achieved by the application of quantum chemical calculations. In particular, we emphasize recent work in two areas: new particle formation and heterogeneous processes. Details in quantum chemical methods are provided, elaborating on computational models for prenucleation, secondary organic aerosol formation, and aerosol interface phenomena. Modeling of relative humidity effects, aerosol surfaces, and chemical kinetics of reaction pathways is discussed. Because of their relevance, quantum chemical calculations and field and laboratory experiments are compared. In addition to describing the atmospheric relevance of the computational models, this article also presents future challenges in quantum chemical calculations applied to aerosols.
| Original language | English |
|---|---|
| Article number | e26350 |
| Journal | International Journal of Quantum Chemistry |
| Volume | 120 |
| Issue number | 20 |
| DOIs | |
| State | Published - Oct 15 2020 |
| Externally published | Yes |
Funding
This work was supported by National Science Foundation grants CHE‐1229354, CHE‐1662030, CHE‐1721511, CHE‐1903871 (GCS), NSF Center for Aerosol Impacts on Chemistry of the Environment (CAICE), CHE‐1801971, and DBI‐1828508 (JGN), the Arnold and Mabel Beckman Foundation Beckman Scholar Award (AGG), the Barry M. Goldwater Scholarship (AGG), and the Schupf Scholar Program (AL). High‐performance computing resources of the MERCURY Consortium ( http://www.mercuryconsortium.org ) were used. Authors are grateful for the sea‐spray micrograph image from the Vicki H. Grassian group at University of California‐San Diego. [ 180,181 ] This work was supported by National Science Foundation grants CHE-1229354, CHE-1662030, CHE-1721511, CHE-1903871 (GCS), NSF Center for Aerosol Impacts on Chemistry of the Environment (CAICE), CHE-1801971, and DBI-1828508 (JGN), the Arnold and Mabel Beckman Foundation Beckman Scholar Award (AGG), the Barry M. Goldwater Scholarship (AGG), and the Schupf Scholar Program (AL). High-performance computing resources of the MERCURY Consortium (http://www.mercuryconsortium.org) were used.[180,181] Authors are grateful for the sea-spray micrograph image from the Vicki H. Grassian group at University of California-San Diego. National Science Foundation, Grant/Award Numbers: CHE‐1229354, CHE‐1662030, CHE‐1721511, CHE‐1903871; Schupf Scholar Program (AL); Barry M. Goldwater Scholarship (AGG); Arnold and Mabel Beckman Foundation Beckman Scholar Award (AGG); NSF Center for Aerosol Impacts on Chemistry of the Environment (CAICE), Grant/Award Numbers: DBI‐1828508, CHE‐1801971 Funding information
Keywords
- adsorption
- heterogeneous chemistry
- prenucleation
- secondary organic aerosol
- surface