Scientific Publications 2001
2001. "A Physically-Based Estimate of Radiative Forcing by Anthropogenic Sulfate Aerosol." Journal of Geophysical Research. D. (Atmospheres) 106(D6):5279-5293. Abstract Estimates of direct and indirect radiative forcing by anthropogenic sulfate aerosols from an integrated global aerosol and climate modeling system are presented. A detailed global tropospheric chemistry and aerosol model that predicts concentrations of oxidants as well as aerosols and aerosol precursors, is coupled to a general circulation model that predicts both cloud water mass and cloud droplet number. Both number and mass of several externally-mixed aerosol size modes are predicted, with internal mixing assumed for the different aerosol components within each mode. Predicted aerosol species include sulfate, organic and black carbon, soil dust, and sea salt. The models use physically-based treatments of aerosol radiative properties (including dependence on relative humidity) and aerosol activation as cloud condensation nuclei. Parallel simulations with and without anthropogenic sulfate aerosol are performed for a global domain. The global and annual mean direct and indirect radiative forcing due to anthropogenic sulfate are estimated to be -0.3 to -0.5 and -1.5 to -3.0 W m-2, respectively. The radiative forcing is sensitive to the model's horizontal resolution, the use of predicted vs. analyzed relative humidity, the prediction vs. diagnosis of aerosol number and droplet number, and the parameterization of droplet collision/coalescence. About half of the indirect radiative forcing is due to changes in droplet radius and half to increased cloud liquid water.
2001. "Evaluation of Aerosol Direct Radiative Forcing in MIRAGE." Journal of Geophysical Research. D. (Atmospheres) 106(D6):5295-5316. Abstract A variety of measurements have been used to evaluate the treatment of aerosol radiative properties and radiative impacts of aerosols simulated by the Model for Integrated Research on Atmospheric Global Exchanges (MIRAGE). The treatment of water uptake in MIRAGE agrees with laboratory measurements for the aerosol components that have been measured. The simulated frequency of relative humidity near 100% is about twice that of European Center for Medium-range Weather Forecasts analyzed relative humidity. When the analyzed relative humidity is used to calculate aerosol water uptake in MIRAGE, the simulated aerosol optical depth agrees with most surface measurements after cloudy conditions are filtered out and differences between model and station elevations are accounted for. Simulated optical depths are low over sites in Brazil during the biomass burning season and over sites in central Canada during the wildfire season, which can be attributed to limitations in the organic and black carbon emissions data used by MIRAGE. The simulated aerosol optical depths are mostly within a factor of two of satellite estimates, but MIRAGE simulates excessively high aerosol optical depths off the east coast of the US and China, and too little dust off the coast of West Africa and in the Arabian Sea. The simulated distribution of single-scatter albedo is consistent with the available in situ surface measurements. The simulated sensitivity of radiative forcing to aerosol optical depth is consistent with estimates from measurements where available. The simulated spatial distribution of aerosol radiance is broadly consistent with estimates from satellite measurements, but with the same errors as the aerosol optical depth. The simulated direct forcing is within the uncertainty of estimates from measurements in the North Atlantic.
2001. "Evaluation of Aerosol Indirect Radiative Forcing in MIRAGE." Journal of Geophysical Research. D. (Atmospheres) 106(D6):5317-5334. Abstract We evaluate aerosol indirect radiative forcing simulated by the Model for Integrated Research on Atmospheric Global Exchanges (MIRAGE). Although explicit measurements of aerosol indirect radiative forcing do not exist, measurements of many of the links between aerosols and indirect radiative forcing are available and can be used for evaluation. These links include the cloud condensation nuclei concentration, the ratio of droplet number to aerosol number, the droplet number concentration, the column droplet number, the column cloud water, the droplet effective radius, the cloud optical depth, the correlation between cloud albedo and droplet effective radius, and the cloud radiative forcing. The CCN concentration simulated by MIRAGE agrees with measurements for supersaturations larger than 0.1%, but not for smaller supersaturations. Simulated droplet number concentrations are too low in most, but not all, locations with available measurements, even when normalized by aerosol number. MIRAGE correctly simulates the higher droplet numbers and smaller droplet sizes over continents and in the Northern Hemisphere. Biases in column cloud water, cloud optical depth, and shortwave cloud radiative forcing are evident in the Intertropical Convergence Zone and in the subtropical oceans. MIRAGE correctly simulates a negative correlation between cloud albedo and droplet size over remote oceans for cloud optical depths greater than 15 and a positive correlation for cloud optical depths less than 15, but fails to simulate a negative correlation over land.
2001. "Activation of the C-H Bond of Methane by Intermediate Q of Methane Monoozygenase: A Theoretical Study." Journal of the American Chemical Society 123(16):3836-3837. Abstract The dydroxylase component (MMOH) of the multicomponent soluable methane monooxygenase (MMO) system catalyzes the oxidation of methane by dioxygen to form methanol and water at non-heme, dinuclear iron active sites.
2001. "Strategies for Multiscale Modeling and Simulation of Organic Materials: Polymers and Biopolymers." Computational and Theoretical Polymer Science 11(5):329-343. Abstract Advances in theory and methods are making it practical to consider fully first principles (de novo) predictions of structures, properties, and processes for organic materials. However, dispite the progress there remains an enormous challenge in bridging the vast range of distances and time scales between de novo atomistic simulations and the quantitative continuum models for the macroscopic systems essential in industrial design and operations. Recent advances relevant to such developments include: quantum chemistry including continuum solvation and force field embedding, de novo force fields to describe phase transitions, molecular dynamics (MD) including continuum solvent, non equilibrium MD for rheology and thermal conductivity and mesoscale simulations.