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Ridley, David A.

Publications and source records attributed to Ridley, David A..

Exploring the Constraints on Simulated Aerosol Sources and Transport across the North Atlantic with Island-Based Sun Photometers

Atmospheric aerosol over the North Atlantic Ocean impact regional clouds and climate. In this work, we use a set of sun photometer observations of Aerosol Optical Depth (AOD) located on the Graciosa and Cape Verde islands, along with the GEOS-Chem chemical transport model to investigate the sources of these aerosol and their transport over the North Atlantic Ocean. At both locations, the largest simulated contributor to aerosol extinction is the local source of sea-salt aerosol. In addition to this large source, we find that signatures consistent with long-range transport of anthropogenic, biomass burning, and dust emissions are apparent throughout the year at both locations. Model simulations suggest that this signal of long-range transport in AOD is more apparent at higher elevation locations; the influence of anthropogenic and biomass burning aerosol extinction is particularly pronounced at the height of Pico Mountain, near the Graciosa Island site. Using a machine learning approach, we further show that simulated observations at these three sites (near Graciosa, Pico Mountain, and Cape Verde) can be used to predict the simulated background aerosol imported into cities on the European mainland, particularly during the local winter months, highlighting the utility of background AOD monitoring for understanding downwind air quality.

54 ENVIRONMENTAL SCIENCES↗

Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with in situ Data from ARCTAS 2008

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9- 02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 percent, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GCRT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Alvarado, Matthew J.↗

Interpreting the Ultraviolet Aerosol Index Observed with the OMI Satellite Instrument to Understand Absorption by Organic Aerosols: Implications for Atmospheric Oxidation and Direct Radiative Effects

Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOSChem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (-0.32 to -0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from -0.57 to -0.09 over West Africa in January, from -0.32 to +0.0002 over South Asia in April, from -0.97 to -0.22 over southern Africa in July, and from -0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Angstrom exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30% over South America in September, up to 20% over southern Africa in July, and up to 15% over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing more strongly absorbing BrC changes the global annual mean all-sky top of atmosphere (TOA) DRE by +0.03Wm(exp -2) and all-sky surface DRE by -0.08Wm(exp -2). Regional changes of up to +0.3Wm(exp -2) at TOA and down to -1.5Wm(exp -2) at the surface are found over major biomass burning regions.

Air Pollution↗