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Mickley, Loretta J.

Publications and source records attributed to Mickley, Loretta J..

Southeast Atmosphere Studies: Learning from Model-Observation Syntheses

Concentrations of atmospheric trace species in the United States have changed dramatically over the past several decades in response to pollution control strategies, shifts in domestic energy policy and economics, and economic development (and resulting emission changes) elsewhere in the world. Reliable projections of the future atmosphere require models to not only accurately describe current atmospheric concentrations, but to do so by representing chemical, physical and biological processes with conceptual and quantitative fidelity. Only through incorporation of the processes controlling emissions and chemical mechanisms that represent the key transformations among reactive molecules can models reliably project the impacts of future policy, energy and climate scenarios. Efforts to properly identify and implement the fundamental and controlling mechanisms in atmospheric models benefit from intensive observation periods, during which collocated measurements of diverse, speciated chemicals in both the gas and condensed phases are obtained. The Southeast Atmosphere Studies (SAS, including SENEX, SOAS, NOMADSS and SEAC4RS) conducted during the summer of 2013 provided an unprecedented opportunity for the atmospheric modeling community to come together to evaluate, diagnose and improve the representation of fundamental climate and air quality processes in models of varying temporal and spatial scales. This paper is aimed at discussing progress in evaluating, diagnosing and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models. The effort focused primarily on model representation of fundamental atmospheric processes that are essential to the formation of ozone, secondary organic aerosol (SOA) and other trace species in the troposphere, with the ultimate goal of understanding the radiative impacts of these species in the southeast and elsewhere. Here we address questions surrounding four key themes: gas-phase chemistry, aerosol chemistry, regional climate and chemistry interactions, and natural and anthropogenic emissions. We expect this review to serve as a guidance for future modeling efforts.

atmospheric chemistry↗

Seasonal Impact of Regional Outdoor Biomass Burning on Air Pollution in Three Indian Cities: Delhi, Bengaluru, and Pune

Air pollution in many of India's cities exceeds national and international standards, and effective pollution control strategies require knowledge of the sources that contribute to air pollution and their spatiotemporal variability. In this study, we examine the influence of a single pollution source, outdoor biomass burning, on particulate matter (PM) concentrations, surface visibility, and aerosol optical depth (AOD) from 2007 to 2013 in three of the most populous Indian cities. We define the upwind regions, or "airsheds," for the cities by using atmospheric back trajectories from the HYSPLIT model. Using satellite fire radiative power (FRP) observations as a measure of fire activity, we target pre-monsoon and post-monsoon fires upwind of the Delhi National Capital Region and pre-monsoon fires surrounding Bengaluru and Pune. We find varying contributions of outdoor fires to different air quality metrics. For the post-monsoon burning season, we find that a subset of local meteorological variables (air temperature, humidity, sea level pressure, wind speed and direction) and FRP as the only pollution source explained 39% of variance in Delhi station PM(sub 10) anomalies, 77% in visibility, and 30% in satellite AOD; additionally, per unit increase in FRP within the daily airshed (1000 MW), PM(sub 10) increases by 16.34 micrograms per cubic meter, visibility decreases by 0.097 km, and satellite AOD increases by 0.07. In contrast, for the pre-monsoon burning season, we find less significant contributions from FRP to air quality in all three cities. Further, we attribute 99% of FRP from post-monsoon outdoor fires within Delhi's average airshed to agricultural burning. Our work suggests that although outdoor fires are not the dominant air pollution source in India throughout the year, post-monsoon fires contribute substantially to regional air pollution and high levels of population exposure around Delhi. During 3-day blocks of extreme PM(sub 2.5) in the 2013 post-monsoon burning season, which coincided with statistically significant high fire activity, concentrations in Delhi averaged 304 micrograms per cubic meter, or more than 1000% above the 24-h PM(sub 2.5) guideline (25 micrograms per cubic meter) of the World Health Organization. These results suggest that providing viable alternatives to agricultural residue burning could help improve post-monsoon air quality for a growing population of 63 million (39% in urban areas) within Delhi's airshed.

Air quality; Outdoor fires; Crop residue burning; ↗

Global Radiative Forcing of Coupled Tropospheric Ozone and Aerosols in a Unified General Circulation Model

Global simulations of sea salt and mineral dust aerosols are integrated into a previously developed unified general circulation model (GCM), the Goddard Institute for Space Studies (GISS) GCM II', that simulates coupled tropospheric ozone-NOx-hydrocarbon chemistry and sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon aerosols. The fully coupled gas-aerosol unified GCM allows one to evaluate the extent to which global burdens, radiative forcing, and eventually climate feedbacks of ozone and aerosols are influenced by gas-aerosol chemical interactions. Estimated present-day global burdens of sea salt and mineral dust are 6.93 and 18.1 Tg with lifetimes of 0.4 and 3.9 days, respectively. The GCM is applied to estimate current top of atmosphere (TOA) and surface radiative forcing by tropospheric ozone and all natural and anthropogenic aerosol components. The global annual mean value of the radiative forcing by tropospheric ozone is estimated to be +0.53 W m(sup -2) at TOA and +0.07 W m(sup -2) at the Earth's surface. Global, annual average TOA and surface radiative forcing by all aerosols are estimated as -0.72 and -4.04 W m(sup -2), respectively. While the predicted highest aerosol cooling and heating at TOA are -10 and +12 W m(sup -2) respectively, surface forcing can reach values as high as -30 W m(sup -2), mainly caused by the absorption by black carbon, mineral dust, and OC. We also estimate the effects of chemistry-aerosol coupling on forcing estimates based on currently available understanding of heterogeneous reactions on aerosols. Through altering the burdens of sulfate, nitrate, and ozone, heterogeneous reactions are predicted to change the global mean TOA forcing of aerosols by 17% and influence global mean TOA forcing of tropospheric ozone by 15%.

Liao, Hong↗

Global Modeling of Tropospheric Chemistry with Assimilated Meteorology: Model Description and Evaluation

We present a first description and evaluation of GEOS-CHEM, a global three-dimensional (3-D) model of tropospheric chemistry driven by assimilated meteorological observations from the Goddard Earth Observing System (GEOS) of the NASA Data Assimilation Office (DAO). The model is applied to a 1-year simulation of tropospheric ozone-NOx-hydrocarbon chemistry for 1994, and is evaluated with observations both for 1994 and for other years. It reproduces usually to within 10 ppb the concentrations of ozone observed from the worldwide ozonesonde data network. It simulates correctly the seasonal phases and amplitudes of ozone concentrations for different regions and altitudes, but tends to underestimate the seasonal amplitude at northern midlatitudes. Observed concentrations of NO and peroxyacetylnitrate (PAN) observed in aircraft campaigns are generally reproduced to within a factor of 2 and often much better. Concentrations of HNO3 in the remote troposphere are overestimated typically by a factor of 2-3, a common problem in global models that may reflect a combination of insufficient precipitation scavenging and gas-aerosol partitioning not resolved by the model. The model yields an atmospheric lifetime of methylchloroform (proxy for global OH) of 5.1 years, as compared to a best estimate from observations of 5.5 plus or minus 0.8 years, and simulates H2O2 concentrations observed from aircraft with significant regional disagreements but no global bias. The OH concentrations are approximately 20% higher than in our previous global 3-D model which included an UV-absorbing aerosol. Concentrations of CO tend to be underestimated by the model, often by 10-30 ppb, which could reflect a combination of excessive OH (a 20% decrease in model OH could be accommodated by the methylchloroform constraint) and an underestimate of CO sources (particularly biogenic). The model underestimates observed acetone concentrations over the South Pacific in fall by a factor of 3; a missing source from the ocean may be implicated.

Bey, Isabelle↗