Adjoint sensitivity of global cloud droplet number to aerosol and dynamical parameters

We present the development of the adjoint of a comprehensive cloud droplet formation parameterization for use in aerosol-cloud-climate interaction studies. The adjoint efficiently and accurately calculates the sensitivity of cloud droplet number concentration (CDNC) to all parameterization inputs (e.g., updraft velocity, water uptake coefficient, aerosol number and hygroscopicity) with a single execution. The adjoint is then integrated within three dimensional (3-D) aerosol modeling frameworks to quantify the sensitivity of CDNC formation globally to each parameter. Sensitivities are computed for year-long executions of the NASA Global Modeling Initiative (GMI) Chemical Transport Model (CTM), using wind fields computed with the Goddard Institute for Space Studies (GISS) Global Circulation Model (GCM) II', and the GEOS-Chem CTM, driven by meteorological input from the Goddard Earth Observing System (GEOS) of the NASA Global Modeling and Assimilation Office (GMAO). We find that over polluted (pristine) areas, CDNC is more sensitive to updraft velocity and uptake coefficient (aerosol number and hygroscopicity). Over the oceans of the Northern Hemisphere, addition of anthropogenic or biomass burning aerosol is predicted to increase CDNC in contrast to coarse-mode sea salt which tends to decrease CDNC. Over the Southern Oceans, CDNC is most sensitive to sea salt, which is the main aerosol component of the region. Globally, CDNC is predicted to be less sensitive to changes in the hygroscopicity of the aerosols than in their concentration with the exception of dust where CDNC is very sensitive to particle hydrophilicity over arid areas. Regionally, the sensitivities differ considerably between the two frameworks and quantitatively reveal why the models differ considerably in their indirect forcing estimates

On the Effect of Dust Particles on Global Cloud Condensation Nuclei and Cloud Droplet Number

Aerosol-cloud interaction studies to date consider aerosol with a substantial fraction of soluble material as the sole source of cloud condensation nuclei (CCN). Emerging evidence suggests that mineral dust can act as good CCN through water adsorption onto the surface of particles. This study provides a first assessment of the contribution of insoluble dust to global CCN and cloud droplet number concentration (CDNC). Simulations are carried out with the NASA Global Modeling Initiative chemical transport model with an online aerosol simulation, considering emissions from fossil fuel, biomass burning, marine, and dust sources. CDNC is calculated online and explicitly considers the competition of soluble and insoluble CCN for water vapor. The predicted annual average contribution of insoluble mineral dust to CCN and CDNC in cloud-forming areas is up to 40 and 23.8%, respectively. Sensitivity tests suggest that uncertainties in dust size distribution and water adsorption parameters modulate the contribution of mineral dust to CDNC by 23 and 56%, respectively. Coating of dust by hygroscopic salts during the atmospheric aging causes a twofold enhancement of the dust contribution to CCN; the aged dust, however, can substantially deplete in-cloud supersaturation during the initial stages of cloud formation and can eventually reduce CDNC. Considering the hydrophilicity from adsorption and hygroscopicity from solute is required to comprehensively capture the dust-warm cloud interactions. The framework presented here addresses this need and can be easily integrated in atmospheric models

The impact of local sources and long-range transport on aerosol properties over the northeast U.S. region during INTEX-NA

We use data collected aboard the NASA DC-8 aircraft during the summer 2004, Intercontinental Transport and Chemical Evolution Experiment over North America (INTEX-NA) field campaign to examine the origin, composition, physical and optical properties of aerosols within air masses sampled over and downwind of the northeastern U.S. We note that aerosol concentrations within the region exhibited steep vertical gradients and significant variability in both time and space. An examination of air mass chemical signatures and backward trajectories indicates that transport from four, significantly different source regions contributed to the variability: the subtropical Atlantic Ocean (AO); the U.S. west coast and eastern Pacific (WCP); the U.S. east coast and Midwestern states (EC); and northwest Canada and Alaska (CA). AO air masses were typically confined to below 2 km altitude, exhibited low pollutant contents, contained enhanced levels of sea salt, and were typically observed when the Bermuda High strengthened. The most common air mass present in the upper troposphere, WCP air often contained weak dust and aged pollution enhances from convective input occurring over the central part of the continent. CA air exhibited enhancements in anthropogenic pollution tracers below 2 km and contained some black-carbon rich haze layers between 3 and 5 km that could be traced to forest fires burning in western Canada and Alaska. EC air was prevalent at lower elevations throughout the study area and exhibited enhanced scattering along with elevated levels of sulfate aerosols and combustion tracers. There is an overall balance between the observed cations and anions for all cases, except EC air mass below 4 km

Integrated approach towards understanding interactions of mineral dust aerosol with warm clouds

Mineral dust is ubiquitous in the atmosphere and represents a dominant type of particulate matter by mass. Despite its well-recognized importance, assessments of dust impacts on clouds and climate remain highly uncertain. This thesis addresses the role of dust as cloud condensation nuclei (CCN) and giant CCN (GCCN) with the goal of improving our understanding of dust-warm cloud interactions and their representation in climate models. We investigate the CCN-relevant properties of mineral dust samples representative of major regional dust sources experimentally in the laboratory conditions to determine their respective affinity to water. Based on the experimental exponent derived from the dependence of critical supersaturation with particle dry diameter, we determine the dominant physics of activation (i.e., adsorption activation theory (AT) or traditional Köhler theory (KT)) for dust particles from different global regions. Results from experimental measurements are used to support the development of a new parameterization of cloud droplet formation from dust CCN for climate models based on adsorption activation mechanism. The potential role of dust GCCN activating by AT within warm stratocumulus and convective clouds is also evaluated.Ph.D.Committee Chair: Nenes, Athanasios; Committee Co-Chair: Sokolik, Irina N.; Committee Member: Meredith, Carson; Committee Member: Teja, Amyn; Committee Member: Weber, Rodne

Indian Ocean Experiment: An integrated analysis of the climate forcing and effects of the great Indo-Asian haze

Every year, from December to April, anthropogenic haze spreads over most of the North Indian Ocean, and South and Southeast Asia. The Indian Ocean Experiment (INDOEX) documented this Indo-Asian haze at scales ranging from individual particles to its contribution to the regional climate forcing. This study integrates the multiplatform observations (satellites, aircraft, ships, surface stations, and balloons) with one- and four-dimensional models to derive the regional aerosol forcing resulting from the direct, the semidirect and the two indirect effects. The haze particles consisted of several inorganic and carbonaceous species, including absorbing black carbon clusters, fly ash, and mineral dust. The most striking result was the large loading of aerosols over most of the South Asian region and the North Indian Ocean. The January to March 1999 visible optical depths were about 0.5 over most of the continent and reached values as large as 0.2 over the equatorial Indian ocean due to long-range transport. The aerosol layer extended as high as 3 km. Black carbon contributed about 14% to the fine particle mass and 11% to the visible optical depth. The single-scattering albedo estimated by several independent methods was consistently around 0.9 both inland and over the open ocean. Anthropogenic sources contributed as much as 80% (±10%) to the aerosol loading and the optical depth. The in situ data, which clearly support the existence of the first indirect effect (increased aerosol concentration producing more cloud drops with smaller effective radii), are used to develop a composite indirect effect scheme. The Indo-Asian aerosols impact the radiative forcing through a complex set of heating (positive forcing) and cooling (negative forcing) processes. Clouds and black carbon emerge as the major players. The dominant factor, however, is the large negative forcing (-20±4 W m^(−2)) at the surface and the comparably large atmospheric heating. Regionally, the absorbing haze decreased the surface solar radiation by an amount comparable to 50% of the total ocean heat flux and nearly doubled the lower tropospheric solar heating. We demonstrate with a general circulation model how this additional heating significantly perturbs the tropical rainfall patterns and the hydrological cycle with implications to global climate

Fire and ice: analyzing ice nucleating particle emissions from western U.S. wildfires

2019 Fall.Includes bibliographical references.Wildfires in the western U.S. can have impacts on health and air quality and are forecasted to increase in the future. Some of the particles released from wildfires can affect cloud formation through serving as ice nucleating particles (INPs). INPs are necessary for heterogenous ice formation in mixed-phase clouds at temperatures warmer than about -38 °C and can have climate implications from radiative impacts on cloud phase and by affecting cloud lifetime. Wildfires have been shown to be a potential source of INPs from previous ground-based measurement studies, but almost no data exist at the free tropospheric level that is relevant for cloud formation. The Western Wildfire Experiment for Cloud Chemistry, Aerosol Absorption, and Nitrogen (WE-CAN) campaign that was conducted in summer 2018 utilized the NSF/NCAR C-130 to sample many smoke plumes of various ages in the free troposphere and aged smoke in the boundary layer. INP measurements were made with the CSU Continuous Flow Diffusion Chamber (CFDC) and with aerosol filter collections to analyze offline with the CSU Ice Spectrometer (IS). The results presented in this thesis indicate a contribution of smoke to the INP number concentration budget over the plume-background air, but much variability exists in concentrations and in INP composition among fires. Treatments of the filter suspensions show a dominant organic influence in all plume filters analyzed while a biological INP population is evident in several cases. For the South Sugarloaf fire, which had a primary fuel of sagebrush shrubland, the highest INP concentrations of the campaign were measured, and the unique INP temperature spectrum suggests lofting of material from uncombusted plant material. Normalization of INP concentrations measured in WE-CAN confirms that smoke is not an especially efficient source of ice nucleating particles, however emissions impacts may still occur regionally. The determination of a Normalized Excess Mixing Ratio (NEMR) of INP emissions for the first time will permit modeling of such impacts, and possible INP in-plume production will be explored in future research

Global distribution and climate forcing of carbonaceous aerosols

The global distribution of carbonaceous aerosols is simulated online in the Goddard Institute for Space Studies General Circulation Model II-prime (GISS GCM II-prime). Prognostic tracers include black carbon (BC), primary organic aerosol (POA), five groups of biogenic volatile organic compounds (BVOCs), and 14 semivolatile products of BVOC oxidation by O_3, OH, and NO_3, which condense to form secondary organic aerosols (SOA) based on an equilibrium partitioning model and experimental observations. Estimated global burdens of BC, organic carbon (OC), and SOA are 0.22, 1.2, and 0.19 Tg with lifetimes of 6.4, 5.3, and 6.2 days, respectively. The predicted global production of SOA is 11.2 Tg yr^(−1), with 91% due to O_3 and OH oxidation. Globally averaged, top of the atmosphere (TOA) radiative forcing by anthropogenic BC is predicted as +0.51 to +0.8 W m^(−2), the former being for BC in an external mixture and the latter for BC in an internal mixture of sulfate, OC, and BC. Globally averaged, anthropogenic BC, OC, and sulfate are predicted to exert a TOA radiative forcing of −0.39 to −0.78 W m^(−2), depending on the exact assumptions of aerosol mixing and water uptake by OC. Forcing estimates are compared with those published previously