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Dry deposition of ozone is an important sink of ozone in near surface air. When dry deposition occurs through plant stomata, ozone can injure the plant, altering water and carbon cycling and reducing crop yields. Quantifying both stomatal and nonstomatal uptake accurately is relevant for understanding ozone's impact on human health as an air pollutant and on climate as a potent short-lived greenhouse gas and primary control on the removal of several reactive greenhouse gases and air pollutants. Robust ozone dry deposition estimates require knowledge of the relative importance of individual deposition pathways, but spatiotemporal variability in nonstomatal deposition is poorly understood. Here we integrate understanding of ozone deposition processes by synthesizing research from fields such as atmospheric chemistry, ecology, and meteorology. We critically review methods for measurements and modeling, highlighting the empiricism that underpins modeling and thus the interpretation of observations. Our unprecedented synthesis of knowledge on deposition pathways, particularly soil and leaf cuticles, reveals process understanding not yet included in widely-used models. If coordinated with short-term field intensives, laboratory studies, and mechanistic modeling, measurements from a few long-term sites would bridge the molecular to ecosystem scales necessary to establish the relative importance of individual deposition pathways and the extent to which they vary in space and time. Our recommended approaches seek to close knowledge gaps that currently limit quantifying the impact of ozone dry deposition on air quality, ecosystems, and climate.

Robust estimates of historical changes in aerosols are key for accurate constraints on climate sensitivity. Dry deposition is a primary sink of aerosols from the atmosphere. However, most global climate models do not accurately represent observed strong dependencies of dry deposition following turbulent transport on aerosol size. It is unclear whether there is a substantial impact of mischaracterized aerosol deposition velocities on historical aerosol changes. Here we describe improved mechanistic representation of aerosol dry deposition in the NASA Goddard Institute for Space Studies (GISS) global climate model, ModelE, and illustrate the impact on 1850–2000 changes in global aerosol burdens as well as aerosol direct and cloud albedo effects using a set of 1850 and 2000 time slice simulations. We employ two aerosol configurations of ModelE (a "bulk" mass‐based configuration and a configuration that more explicitly represents aerosol size distributions, internal mixing, and microphysics) to explore how model structural differences in aerosol representation alter the response to representation of dry deposition. Both configurations show larger historical increases in the global burdens of non‐dust aerosols with the new dry deposition scheme, by 11% in the simpler mass‐based configuration and 23% in the more complex microphysical configuration. Historical radiative forcing responses, which vary in magnitude from 5% to 12% as well as sign, depend on the aerosol configuration. Plain Language Summary: Numerical models representing the Earth system are important tools for understanding the drivers of climate change and variability. Particles (also known as aerosols) in the atmosphere can influence climate by scattering or absorbing solar radiation and influencing clouds. How the amount of particles in the atmosphere has changed since preindustrial times is very uncertain. Many processes impact particle spatial distributions and changes with time, as well as how particles influence climate. Sources and sinks of particles need to be represented well in order to have confidence in estimates of changes in particles. Here we more accurately simulate dry deposition, which is a sink of particles, in a numerical model that represents the Earth system, and examine impacts on changes in the amount of particles in the atmosphere from preindustrial times to present day and the particles' influence on climate. Key Points: ModelE now has process‐based representation of aerosol dry deposition, and captures strong observed dependencies on particle sizeIncreases from 1850 to 2000 in the global non‐dust aerosol annual burdens are 11%–23% larger with more mechanistic dry depositionHistorical radiative forcing responses (−12% to +6%) depend on aerosol representation (e.g., microphysics and mixing state) [ABSTRACT FROM AUTHOR]

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes. [ABSTRACT FROM AUTHOR]

Peroxy acetyl nitrate (PAN) is the most important reservoir species for nitrogen oxides (NOx) in the remote troposphere. Upon decomposition in remote regions, PAN promotes efficient ozone production. We evaluate monthly mean PAN abundances from global chemical transport model simulations (HTAP1) for 2001 with measurements from five northern mid-latitude mountain sites (four European and one North American). The multi-model mean generally captures the observed monthly mean PAN but individual models simulate a factor of ~ 4–8 range in monthly abundances. We quantify PAN source-receptor relationships at the measurement sites with sensitivity simulations that decrease regional anthropogenic emissions of PAN (and ozone) precursors by 20 % from North America (NA), Europe (EU), and East Asia (EA). The HTAP1 models attribute more of the observed PAN at Jungfraujoch (Switzerland) to emissions in NA and EA, and less to EU, than a prior trajectory-based estimate. The trajectory-based and modeling approaches agree that EU emissions play a role in the observed springtime PAN maximum at Jungfraujoch. The signal from anthropogenic emissions on PAN is strongest at Jungfraujoch and Mount Bachelor (Oregon, U.S.A.) during April. In this month, PAN source-receptor relationships correlate both with model differences in regional anthropogenic volatile organic compound (AVOC) emissions and with ozone source-receptor relationships. PAN observations at mountaintop sites can thus provide key information for evaluating models, including links between PAN and ozone production and source-receptor relationships. Establishing routine, long-term, mountaintop measurements is essential given the large observed interannual variability in PAN. [ABSTRACT FROM AUTHOR]