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Mauzerall, D. L.

Publications and source records attributed to Mauzerall, D. L..

Quantifying PM2.5-Meteorology Sensitivities in a Global Climate Model

Climate change can influence fine particulate matter concentrations (PM2.5) through changes in air pollution meteorology. Knowledge of the extent to which climate change can exacerbate or alleviate air pollution in the future is needed for robust climate and air pollution policy decision-making. To examine the influence of climate on PM2.5, we use the Geophysical Fluid Dynamics Laboratory Coupled Model version 3 (GFDL CM3), a fully-coupled chemistry-climate model, combined with future emissions and concentrations provided by the four Representative Concentration Pathways (RCPs). For each of the RCPs, we conduct future simulations in which emissions of aerosols and their precursors are held at 2005 levels while other climate forcing agents evolve in time, such that only climate (and thus meteorology) can influence PM2.5 surface concentrations. We find a small increase in global, annual mean PM2.5 of about 0.21 micro-g/cu m3 (5%) for RCP8.5, a scenario with maximum warming. Changes in global mean PM2.5 are at a maximum in the fall and are mainly controlled by sulfate followed by organic aerosol with minimal influence of black carbon. RCP2.6 is the only scenario that projects a decrease in global PM2.5 with future climate changes, albeit only by -0.06 micro-g/cu m (1.5%) by the end of the 21st century. Regional and local changes in PM2.5 are larger, reaching upwards of 2 micro-g/cu m for polluted (eastern China) and dusty (western Africa) locations on an annually averaged basis in RCP8.5. Using multiple linear regression, we find that future PM2.5 concentrations are most sensitive to local temperature, followed by surface wind and precipitation. PM2.5 concentrations are robustly positively associated with temperature, while negatively related with precipitation and wind speed. Present-day (2006-2015) modeled sensitivities of PM2.5 to meteorological variables are evaluated against observations and found to agree reasonably well with observed sensitivities (within 10e50% over the eastern United States for several variables), although the modeled PM2.5 is less sensitive to precipitation than in the observations due to weaker convective scavenging. We conclude that the hypothesized "climate penalty" of future increases in PM2.5 is relatively minor on a global scale compared to the influence of emissions on PM2.5 concentrations.

PM2.5↗

Origin of Ozone NO(x) in the Tropical Troposphere: A Photochemical Analysis of Aircraft Observations Over the South Atlantic Basin

The photochemistry of the troposphere over the South Atlantic basin is examined by modeling of aircraft observations up to 12-km altitude taken during the TRACE A expedition in September-October 1992. A close balance is found in the 0 to 12-km column between photochemical production and loss Of O3, with net production at high altitudes compensating for weak net loss at low altitudes. This balance implies that O3 concentrations in the 0-12 km column can be explained solely by in situ photochemistry; influx from the stratosphere is negligible. Simulation of H2O2, CH3OOH, and CH2O concentrations measured aboard the aircraft lends confidence in the computations of O3 production and loss rates, although there appears to be a major gap in current understanding of CH2O chemistry in the marine boundary layer. The primary sources of NO(x) over the South Atlantic Basin appear to be continental (biomass burning, lightning, soils). There is evidence that NO(x) throughout the 0 to 12-km column is recycled from its oxidation products rather than directly transported from its primary sources. There is also evidence for rapid conversion of HNO3 to NO(x) in the upper troposphere by a mechanism not included in current models. A general representation of the O3 budget in the tropical troposphere is proposed that couples the large scale Walker circulation and in situ photochemistry. Deep convection in the rising branches of the Walker circulation injects NO(x) from combustion, soils, and lightning to the upper troposphere, leading to O3 production; eventually, the air subsides and net O3 loss takes place in the lower troposphere, closing the O3 cycle. This scheme implies a great sensitivity of the oxidizing power of the atmosphere to NO(x) emissions in the tropics.

Jacob, D. J.↗

Origin of tropospheric NO(x) over subarctic eastern Canada in summer

The original of NO(X) in the summertime troposphere over subarctic eastern Canada is investigated by photochemical modeling of aircraft and ground-based measurements from the Arctic Boundary Layer Expedition (ABLE 3B). It is found that decomposition of peroxyacetyl nitrate (PAN) can account for most of the NO(X) observed between the surface and 6.2 km altitude (aircraft ceiling). Forest fires represent the principal source of PAN in the region, implying the same origin for NO(X). There is, however, evidence for an unidentified source of NO(X) in occasional air masses subsiding from the upper troposphere. Isoprene emissions from boreal forests maintain high NO(X) concentrations in the continental boundary layer over eastern Canada by scavenging OH and NO3, thus slowing down conversion of NO(X) to HNO3, both in the daytime and at night. This effect is partly compensated by the production of CH3CO3 radicals during isoprene oxidation, which slows down the decomposition of PAN subsiding from the free troposphere. The peroxy radical concentrations estimated from concurrent measurements of NO and NO2 concentrations during ABLE 3B are consistent with values computed from our photochemical model below 4 km, but model values are low at higher altitudes. The discrepancy may reflect either a missing radical source in the model or interferences in the NO2 measurement.

Fan, S.-M↗