Rate of atmospheric brown carbon whitening governed by environmental conditions.

Biomass burning organic aerosol (BBOA) in the atmosphere contains many compounds that absorb solar radiation, called brown carbon (BrC). While BBOA is in the atmosphere, BrC can undergo reactions with oxidants such as ozone which decrease absorbance, or whiten. The effect of temperature and relative humidity (RH) on whitening has not been well constrained, leading to uncertainties when predicting the direct radiative effect of BrC on climate. Using an aerosol flow-tube reactor, we show that the whitening of BBOA by oxidation with ozone is strongly dependent on RH and temperature. Using a poke-flow technique, we show that the viscosity of BBOA also depends strongly on these conditions. The measured whitening rate of BrC is described well with the viscosity data, assuming that the whitening is due to oxidation occurring in the bulk of the BBOA, within a thin shell beneath the surface. Using our combined datasets, we developed a kinetic model of this whitening process, and we show that the lifetime of BrC is 1 d or less below ∼1 km in altitude in the atmosphere but is often much longer than 1 d above this altitude. Including this altitude dependence of the whitening rate in a chemical transport model causes a large change in the predicted warming effect of BBOA on climate. Overall, the results illustrate that RH and temperature need to be considered to understand the role of BBOA in the atmosphere.

Updated World Health Organization Air Quality Guidelines Highlight the Importance of Non-anthropogenic PM2.5.

The World Health Organization recently updated their air quality guideline for annual fine particulate matter (PM2.5) exposure from 10 to 5 µg m-3, citing global health considerations. We explore if this guideline is attainable across different regions of the world using a series of model sensitivity simulations for 2019. Our results indicate that >90% of the global population is exposed to PM2.5 concentrations that exceed the 5 µg m-3 guideline and that only a few sparsely populated regions (largely in boreal North America and Asia) experience annual average concentrations of <5 µg m-3. We find that even under an extreme abatement scenario, with no anthropogenic emissions, more than half of the world's population would still experience annual PM2.5 exposures above the 5 µg m-3 guideline (including >70% and >60% of the African and Asian populations, respectively), largely due to fires and natural dust. Our simulations demonstrate the large heterogeneity in PM2.5 composition across different regions and highlight how PM2.5 composition is sensitive to reductions in anthropogenic emissions. We thus suggest the use of speciated aerosol exposure guidelines to help facilitate region-specific air quality management decisions and improve health-burden estimates of fine aerosol exposure.

Mechanisms of nitrogen deposition effects on temperate forest lichens and trees.

We review the mechanisms of deleterious nitrogen (N) deposition impacts on temperate forests, with a particular focus on trees and lichens. Elevated anthropogenic N deposition to forests has varied effects on individual organisms depending on characteristics both of the N inputs (form, timing, amount) and of the organisms (ecology, physiology) involved. Improved mechanistic knowledge of these effects can aid in developing robust predictions of how organisms respond to either increases or decreases in N deposition. Rising N levels affect forests in micro- and macroscopic ways from physiological responses at the cellular, tissue, and organism levels to influencing individual species and entire communities and ecosystems. A synthesis of these processes forms the basis for the overarching themes of this paper, which focuses on N effects at different levels of biological organization in temperate forests. For lichens, the mechanisms of direct effects of N are relatively well known at cellular, organismal, and community levels, though interactions of N with other stressors merit further research. For trees, effects of N deposition are better understood for N as an acidifying agent than as a nutrient; in both cases, the impacts can reflect direct effects on short time scales and indirect effects mediated through long-term soil and belowground changes. There are many gaps on fundamental N use and cycling in ecosystems, and we highlight the most critical gaps for understanding potential deleterious effects of N deposition. For lichens, these gaps include both how N affects specific metabolic pathways and how N is metabolized. For trees, these gaps include understanding the direct effects of N deposition onto forest canopies, the sensitivity of different tree species and mycorrhizal symbionts to N, the influence of soil properties, and the reversibility of N and acidification effects on plants and soils. Continued study of how these N response mechanisms interact with one another, and with other dimensions of global change, remains essential for predicting ongoing changes in lichen and tree populations across North American temperate forests.