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NASA NTRS2013

Bounding the Role of Black Carbon in the Climate System: a Scientific Assessment

Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg/yr in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W/sq m with 90% uncertainty bounds of (+0.08, +1.27)W/sq m. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W/sq m. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W/sq m with 90% uncertainty bounds of +0.17 to +2.1 W/sq m. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W/sq m, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (0.50 to +1.08) W/sq m during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (0.06 W/sq m with 90% uncertainty bounds of 1.45 to +1.29 W/sq m). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

black carbon↗

NASA NTRS2012

A FIRE-ACE/SHEBA Case Study of Mixed-Phase Arctic Boundary Layer Clouds: Entrainment Rate Limitations on Rapid Primary Ice Nucleation Processes

Observations of long-lived mixed-phase Arctic boundary layer clouds on 7 May 1998 during the First International Satellite Cloud Climatology Project (ISCCP) Regional Experiment (FIRE)Arctic Cloud Experiment (ACE)Surface Heat Budget of the Arctic Ocean (SHEBA) campaign provide a unique opportunity to test understanding of cloud ice formation. Under the microphysically simple conditions observed (apparently negligible ice aggregation, sublimation, and multiplication), the only expected source of new ice crystals is activation of heterogeneous ice nuclei (IN) and the only sink is sedimentation. Large-eddy simulations with size-resolved microphysics are initialized with IN number concentration N(sub IN) measured above cloud top, but details of IN activation behavior are unknown. If activated rapidly (in deposition, condensation, or immersion modes), as commonly assumed, IN are depleted from the well-mixed boundary layer within minutes. Quasi-equilibrium ice number concentration N(sub i) is then limited to a small fraction of overlying N(sub IN) that is determined by the cloud-top entrainment rate w(sub e) divided by the number-weighted ice fall speed at the surface v(sub f). Because w(sub c)< 1 cm/s and v(sub f)> 10 cm/s, N(sub i)/N(sub IN)<< 1. Such conditions may be common for this cloud type, which has implications for modeling IN diagnostically, interpreting measurements, and quantifying sensitivity to increasing N(sub IN) (when w(sub e)/v(sub f)< 1, entrainment rate limitations serve to buffer cloud system response). To reproduce observed ice crystal size distributions and cloud radar reflectivities with rapidly consumed IN in this case, the measured above-cloud N(sub IN) must be multiplied by approximately 30. However, results are sensitive to assumed ice crystal properties not constrained by measurements. In addition, simulations do not reproduce the pronounced mesoscale heterogeneity in radar reflectivity that is observed.

Fridlin, Ann↗

NASA NTRS2001

Responses of Precipitation and Hydrologic Processes to Tropical SST

The goal of the research is to identify the mechanisms in the response of tropical precipitation and atmospheric hydrologic cycle to sea surface temperature (SST) variability at seasonal-to-interannual time scales, and to utilize the knowledge for better understanding of climate feedback processes relevant to global change. As a first step to achieve the goal, we characterize the inter-relationship among convective/stratiform rain, ice/water clouds water vapor, and SST using TRMM satellite data and a cloud-resolving model. We examined the daily hydrologic variables [column water vapor (PW), cloud liquid water (CW), rainfall rates (RR)] as a function of SST using high-resolution data (0.25 x 0.25, daily) derived from TRMM satellite measurements. Comparing the winter of 97/98 (El Nino condition) against the winter of 99/00 (La Nina condition), area-mean values of all four hydrologic variables in cloudy areas within the tropical Pacific are higher in the El Nino winter than in the La Nina winter. This is consistent with previous observational analyses and SST warming experiments (idealized or ENSO-like) that showed the interaction between hydrologic cyclic and radiation at the seasonal to interannual time scales leads to intensified tropical circulation and hydrologic cycle. However, there is evidence that the enhanced hydrologic cycle over the warm pool is accompanied by an expansion of radiatively -driven subsidence in response to a stronger SST gradient between warm pool and surrounding cold pool. The expanding subsidence effectively reduces cloud amounts over the warm pool. Our analysis of daily variability further indicates a more vigorous water cycle characterized by higher PW, CW, and RR in response to overall warming. This is expected from the Clausius Clapeyron relation as a thermodynamic response to warming. However cloudy areas decrease in response to overall warming. This may be due to factors that are fundamentally different. One possibility is that in a warmer climate, there may be alteration in the microphysical processes in clouds, e.g., increased coalescence of cloud size droplets and increased entrainment of dry air from above due to the invigorated convective motions in response to overall warming. As a result, cloud amounts are less. Another interpretation is that, in colder air masses, more ice particles will be produced and, because of their lower densities, are less likely to precipitate, hence the higher cloud amount. This suggests that, when averaged over a sufficiently large area covering both the rising and sinking branches of the tropical circulation, there maybe an increase in the precipitation efficiency in stratiform clouds, in conjunction with increased subsidence in an enhanced water cycle. This is supported by the residence time at different rainrates.

Sui, C.-H.↗

NASA NTRS2004

Tropical Convective Responses to Microphysical and Radiative Processes: A Sensitivity Study With a 2D Cloud Resolving Model

Prognostic cloud schemes are increasingly used in weather and climate models in order to better treat cloud-radiation processes. Simplifications are often made in such schemes for computational efficiency, like the scheme being used in the National Centers for Environment Prediction models that excludes some microphysical processes and precipitation-radiation interaction. In this study, sensitivity tests with a 2D cloud resolving model are carried out to examine effects of the excluded microphysical processes and precipitation-radiation interaction on tropical thermodynamics and cloud properties. The model is integrated for 10 days with the imposed vertical velocity derived from the Tropical Ocean Global Atmosphere Coupled Ocean-Atmosphere Response Experiment. The experiment excluding the depositional growth of snow from cloud ice shows anomalous growth of cloud ice and more than 20% increase of fractional cloud cover, indicating that the lack of the depositional snow growth causes unrealistically large mixing ratio of cloud ice. The experiment excluding the precipitation-radiation interaction displays a significant cooling and drying bias. The analysis of heat and moisture budgets shows that the simulation without the interaction produces more stable upper troposphere and more unstable mid and lower troposphere than does the simulation with the interaction. Thus, the suppressed growth of ice clouds in upper troposphere and stronger radiative cooling in mid and lower troposphere are responsible for the cooling bias, and less evaporation of rain associated with the large-scale subsidence induces the drying in mid and lower troposphere.

Li, Xiao-Fan↗

NASA NTRS1988

Radiative processes in upper tropospheric mixed-phase clouds

The diffusional mass evolution of hydrometeors in upper tropospheric clouds for various radiative conditions in the cloud and for varying ambient moisture supply is simulated using a time dependent microphysical model. Radiation can play an important role in this mass evolution when only one phase is present. When both liquid droplets and ice crystals are situated in a typical upper tropospheric environment and the moisture supply is limited, radiation produces only a minor effect on the mass evolution of the hydrometeors. In these cases ice crystals grow quickly at the expense of the droplets and the droplets evaporate within several minutes, even under water supersaturation conditions. Radiation does not significantly influence the evaporation rates of the droplets in the coexisting cases. In the absence of ice crystals and under certain radiative conditions, the droplets can survive when the environment is subsaturated. For other radiative conditiions, the droplets can evaporate when the environment is supersaturated.

Wesley, Douglas A.↗

NASA NTRS1997

Cirrus Cloud Radiative and Microphysical Properties from Ground Observations and In Situ Measurements During FIRE 1991 and Their Application to Exhibit Problems in Cirrus Solar Radiative Transfer Modeling

Measurements from the FIRE 1991 cirrus cloud field experiment in the central United States are presented and analyzed. The first part focuses on cirrus microphysical properties. Aircraft 2D-probe in situ data at different cloud altitudes were evaluated for cirrus cases on four different days. Also presented are simultaneous data samples from balloonborne videosondes. Only these balloonsondes could detect the smaller crystals. Their data suggest (at least for midlatitude altitudes below 10 km) that ice crystals smaller than 15 microns in size are rare and that small ice crystals not detected by 2D-probe measurements are radiatively of minor importance, as overlooked 2D-probe crystals account for about 10% of the total extinction. The second part focuses on the link between cirrus cloud properties and radiation. With cloud macrophysical properties from surface remote sensing added to the microphysical data and additional radiation measurements at the surface, testbeds for radiative transfer models were created. To focus on scattering processes, model evaluations were limited to the solar radiative transfer by comparing calculated and measured transmissions of sunlight at the surface. Comparisons under cloud-free conditions already reveal a model bias of about +45 W/sq m for the hemispheric solar downward broadband flux. This discrepancy, which is (at least in part) difficult to explain, has to be accounted for in comparisons involving clouds. Comparisons under cirrus cloud conditions identify as the major obstacle in cirrus solar radiative transfer modeling the inability of one-dimensional radiative transfer models to account for horizontal inhomogeneities. The successful incorporation of multidimensional radiative transfer effects will depend not only on better models but critically on the ability to measure and to define characteristic inhomogeneity scales of cloud fields. The relative minor error related to the microphysical treatment is in part a reflection of the improved understanding on solar scattering on ice crystals over the last decade and of the available wealth on ice-crystal size and shape data for this study. In absence of this information, uncertainties from microphysical cirrus model assumptions will remain high.

Kinne, Stefan↗

NASA NTRS2017

Updates on Modeling the Water Cycle with the NASA Ames Mars Global Climate Model

Global Circulation Models (GCMs) have made steady progress in simulating the current Mars water cycle. It is now widely recognized that clouds are a critical component that can significantly affect the nature of the simulated water cycle. Two processes in particular are key to implementing clouds in a GCM: the microphysical processes of formation and dissipation, and their radiative effects on heating/ cooling rates. Together, these processes alter the thermal structure, change the dynamics, and regulate inter-hemispheric transport. We have made considerable progress representing these processes in the NASA Ames GCM, particularly in the presence of radiatively active water ice clouds. We present the current state of our group's water cycle modeling efforts, show results from selected simulations, highlight some of the issues, and discuss avenues for further investigation.

Global Circulation Models (GCMs)↗

NASA NTRSDate not supplied

Single-Scattering Properties of Melting Precipitation for GPM Passive Microwave and Radar Remote Sensing Applications

Over the past two decades, detailed computational simulations of the intricate three dimensional structures of ice-phase crystals and aggregates of those crystals have been developed. The microwave single-scattering properties of these simulated ice particles have been computed and used to improve quantitative estimates of snow rates and to better deRne the vertical structure of snow water contents in deep convective systems, as derived from satellite-borne passive microwave and/or radar remote sensing measurements. The same icephase particles have more recently been used as the starting point for simulations of melting precipitation using computational melting methods. In the current study, a heuristic melting method, as well as a physically-based melting procedure based on smoothed-particle hydrodynamics, are applied to ice particle models to describe the full evolution of the particles from dry snow to liquid drops. The discrete dipole approximation is utilized to calculate the single-scattering properties of the mixed-phase particles throughout the melting process. Then, the properties of the particles are “mapped” into simpliRed microphysical simulations of particle size spectra in the melting layers of stratiform, precipitating clouds. The bulk single-scattering properties of the melting layers and the sensitivity of their properties to modeling assumptions are explored, and the implications for combined radar-radiometer precipitation remote sensing from GPM are discussed.

William S Olson↗

NASA NTRS1990

Denitrification mechanisms in the polar stratospheres

Microphysical simulations suggest that the time required for nitric acid particles to sediment from the stratosphere is comparable to the time required for falling ice particles to incorporate nitric acid vapor from the vapor phase. Since nitric acid particles form earlier in the winter than ice particles, these simulations favor denitrification being a separate process from dehydration, with denitrification being due to nitric acid particles and dehydration due to ice particles. In the simulations, the column abundance of nitric acid is only depleted if temperatures low enough for nitric acid particles to exist extend to the altitude above which the column is measured. Such low temperatures are infrequent in the Arctic lower stratosphere, which may be the main reason that the Arctic stratospheric column shows little loss of nitric acid during winter, while the colder Antarctic stratospheric column shows a substantial loss of nitric acid.

Toon, Owen B.↗

NASA NTRS1999

Statistics of Cirrus Horizontal Inhomogeneity in the Southern Great Plains

Variability of cloud properties on scales smaller than that of a GCM grid is potentially important both for realistic parameterizations of microphysical processes and for the prediction of the large-scale radiative effects of clouds, have suggested that a simple model of marine stratocumulus variability, based on the assumption of Gaussian variation statistics of cloud depth, can explain the liquid water path histogram shapes observed in Landsat data. In advance of ARM SGP MMCR ice water path climatologies, we have examined aircraft ice water content statistics for cirrus clouds observed over Coffeyville, Kansas during FIRE 2. We find similar associations of histogram shape and cloud cover for these clouds, and we show that a simple modification of the model for cirrus combined with observed mean cloud depths, their standard deviations, and ambient thermodynamic conditions predicts both the histogram shape and cirrus cloud cover fairly well. This suggests that subgrid variability of cloud properties may be similar for vastly different cloud types, and that a universal parameterization of the effects of subgrid variability in GCMs as a function of only a few parameters may be a realistic goal.

Smith, S. A.↗

NASA NTRS2011

New Challenges of Cloud Remote Sensing from Space

Clouds are recognized as a major source of uncertainties in predicting climate change. Lack of observational constraints on cloud processes has hindered the development of more reliable climate and weather models. With the advanced NASA EOS and A-Train sensors, we now have better knowledge about vertical distribution, water content, and occurrence frequency of global cloudiness. New ice water content (IWC) measurements from CloudSat and MLS have led to several improvements in model physics and parameterization schemes. MISR and GPS high-resolution data start to reveal deep insights on cloud processes and dynamicS in the planetary boundary layer (PBL). However, Earth sciences are still facing urgent needs to measure cloud microphysical properties, interactions between clouds and aerosol/precipitation, and processes that are coupled in 3-D space but not adequately sampled by the A-Train curtains or by the 2-D imageries. Submillimeter- wave, multi-angle imaging, and GPS radio occultation have emerged as promising remote sensing techniques to meet the challenges and enable new sciences for mid-tropospheric and PBL clouds.

Wu, Dong L.↗

NASA NTRS2000

The Cirrus Parcel Model Comparison Project

The cirrus Parcel Model Comparison Project involves the systematic comparison of current models of ice crystal nucleation and growth for specified, typical, cirrus cloud environments. In Phase 1 of the project reported here, simulated cirrus cloud microphysical properties are compared for situations of "warm" (-40 C) and "cold" (-60 C) cirrus subject to updrafts of 4, 20 and 100 centimeters per second, respectively. Five models are participating in the project. These models employ explicit microphysical schemes wherein the size distribution of each class of particles (aerosols and ice crystals) is resolved into bins. Simulations are made including both homogeneous and heterogeneous ice nucleation mechanisms. A single initial aerosol population of sulfuric acid particles is prescribed for all simulations. To isolate the treatment of the homogeneous freezing (of haze drops) nucleation process, the heterogeneous nucleation mechanism is disabled for a second parallel set of simulations. Qualitative agreement is found amongst the models for the homogeneous-nucleation-only simulations, e.g., the number density of nucleated ice crystals increases with the strength of the prescribed updraft. However, non-negligible quantitative differences are found. Systematic bias exists between results of a model based on a modified classical theory approach and models using an effective freezing temperature approach to the treatment of nucleation. Each approach is constrained by critical freezing data from laboratory studies. This information is necessary, but not sufficient, to construct consistent formulae for the two approaches. Large haze particles may deviate considerably from equilibrium size in moderate to strong updrafts (20-100 centimeters per second) at -60 C when the commonly invoked equilibrium assumption is lifted. The resulting difference in particle-size-dependent solution concentration of haze particles may significantly affect the ice nucleation rate during the initial nucleation interval. The uptake rate for water vapor excess by ice crystals is another key component regulating the total number of nucleated ice crystals. This rate, the product of ice number concentration and ice crystal diffusional growth rate, partially controls the peak nucleation rate achieved in an air parcel and the duration of the active nucleation time period.

Lin, Ruei-Fong↗

NASA NTRS2008

On the Sensitivity of Atmospheric Ensembles to Cloud Microphysics in Long-Term Cloud-Resolving Model Simulations

Month-long large-scale forcing data from two field campaigns are used to drive a cloud-resolving model (CRM) and produce ensemble simulations of clouds and precipitation. Observational data are then used to evaluate the model results. To improve the model results, a new parameterization of the Bergeron process is proposed that incorporates the number concentration of ice nuclei (IN). Numerical simulations reveal that atmospheric ensembles are sensitive to IN concentration and ice crystal multiplication. Two- (2D) and three-dimensional (3D) simulations are carried out to address the sensitivity of atmospheric ensembles to model dimensionality. It is found that the ensembles with high IN concentration are more sensitive to dimensionality than those with low IN concentration. Both the analytic solutions of linear dry models and the CRM output show that there are more convective cores with stronger updrafts in 3D simulations than in 2D, which explains the differing sensitivity of the ensembles to dimensionality at different IN concentrations.

Zeng, Xiping↗

NASA NTRS2017

Physical Processes Controlling the Spatial Distributions of Relative Humidity in the Tropical Tropopause Layer over the Pacific

The spatial distribution of relative humidity with respect to ice (RHI) in the boreal wintertime tropical tropopause layer (TTL, is asymptotically Equal to 14-18 km) over the Pacific is examined with the measurements provided by the NASA Airborne Tropical TRopopause EXperiment. We also compare the measured RHI distributions with results from a transport and microphysical model driven by meteorological analysis fields. Notable features in the distribution of RHI versus temperature and longitude include (1) the common occurrence of RHI values near ice saturation over the western Pacific in the lower to middle TTL; (2) low RHI values in the lower TTL over the central and eastern Pacific; (3) common occurrence of RHI values following a constant mixing ratio in the middle to upper TTL (temperatures between 190 and 200 K); (4) RHI values typically near ice saturation in the coldest airmasses sampled; and (5) RHI values typically near 100% across the TTL temperature range in air parcels with ozone mixing ratios less than 50 ppbv. We suggest that the typically saturated air in the lower TTL over the western Pacific is likely driven by a combination of the frequent occurrence of deep convection and the predominance of rising motion in this region. The nearly constant water vapor mixing ratios in the middle to upper TTL likely result from the combination of slow ascent (resulting in long residence times) and wave-driven temperature variability. The numerical simulations generally reproduce the observed RHI distribution features, and sensitivity tests further emphasize the strong influence of convective input and vertical motions on TTL relative humidity.

Jensen, Eric J.↗

NASA NTRS2010

Genesis of Pre-Hurricane Felix (2007): Warm Core Formation, Precipitation Evolution, and Predictability - Part 2

This is the second of a two-part study examining the simulated formation of Atlantic Hurricane Felix (2007) in a cloud-representing framework. Here several open issues are addressed concerning the formation of the storm's warm core, the evolution and respective contribution of stratiform versus convective precipitation within the parent wave's pouch, and the sensitivity of the development pathway reported in Part I to different model physics options and initial conditions. All but one of the experiments include ice microphysics as represented by one of several parameterizations, and the partition of convective versus stratiform precipitation is accomplished using a standard numerical technique based on the high-resolution control experiment. The transition to a warm-core tropical cyclone from an initially cold-core, lower tropospheric wave disturbance is analyzed first. As part of this transformation process, it is shown that deep moist convection is sustained near the pouch center. Both convective and stratiform precipitation rates increase with time. While stratiform precipitation occupies a larger area even at the tropical storm stage, deep moist convection makes a comparable contribution to the total rain rate at the pregenesis stage, and a larger contribution than stratiform processes at the storm stage. The convergence profile averaged near the pouch center is found to become dominantly convective with increasing deep moist convective activity there. Low-level convergence forced by interior diabatic heating plays a key role in forming and intensifying the near-surface closed circulation, while the midlevel convergence associated with stratiform precipitation helps to increase the midlevel circulation and thereby contributes to the formation and upward extension of a tropospheric-deep cyclonic vortex. Sensitivity tests with different model physics options and initial conditions demonstrate a similar pregenesis evolution. These tests suggest that the genesis location of a tropical storm is largely controlled by the parent wave's critical layer, whereas the genesis time and intensity of the protovortex depend on the details of the mesoscale organization, which is less predictable. Some implications of the findings are discussed.

Wang, zhuo↗

NASA NTRSDate not supplied

Quantifying Changes in the Arctic Shortwave Cloud Radiative Effects

The shortwave cloud radiative effect (SWCRE) is important on the Arctic surface radiation budget and the major source of inter-model spread in predictions of Arctic climate. To better understand the individual contributions of various radiative processes to changes in SWCRE, the paper presents the use of the extended APRP (Atmospheric Radiative Perturbation Potential) method. This involves adding the absorptivity for the upward beam and considering differences in reflectivity between upward and downward beams, as well as analyzing the cloud masking effect resulting from changes in surface albedo in more detail. Using data from the CMIP5 and CMIP6 climate models, the study decomposes the SWCRE over the Arctic surface and analyzes inter-model differences in quadrupled CO2 simulations. The study takes into account the fact that the response of SWCRE to Arctic warming is influenced by changes in surface albedo, cloud amount, and cloud microphysics. Results show that in the sunlight season, the reduction in surface albedo associated with sea ice loss is directly linked to strong negative SWCRE, which explains the considerable model discrepancy. Arctic clouds can hinder the positive surface albedo feedback by changing the albedo in two ways: (1) decreasing incoming shortwave radiation due to cloud reflection and (2) by decreasing the shortwave reaching the surface after being reflected by clouds. In addition, increased (decreased) cloud amount and cloud liquid water are shown to be less (more) incoming shortwave fluxes at the surface, but not dominating factors to the Arctic surface radiation budget and its inter-model variation. Overall, the extended APRP method offers a useful tool for analyzing the complex interactions between clouds and radiative process, reasonably decomposes the individual SWCRE responses at the Arctic surface, and emphasizes that considering not only the cloud amount or its properties, but also surface albedo change is critical for the prediction of SWCRE on the Arctic surface.

Arctic cloud↗

NASA NTRS2004

Investigation of Polar Stratospheric Cloud Solid Particle Formation Mechanisms Using ILAS and AVHRR Observations in the Arctic

Satellite observations of denitrification and ice clouds in the Arctic lower stratosphere in February 1997 are used with Lagrangian microphysical box model calculations to evaluate nucleation mechanisms of solid polar stratospheric cloud (PSC) particles. The occurrences of ice clouds are not correlated in time and space with the locations of back trajectories of denitrified air masses, indicating that ice particle surfaces are not always a prerequisite for the formation of solid PSCs that lead to denitrification. In contrast, the model calculations incorporating a pseudoheterogeneous freezing process occurring at the vapor-liquid interface can quantitatively explain most of the observed denitrification when the nucleation activation free energy for nitric acid dihydrate formation is raised by only approx.10% relative to the current published values. Once nucleated, the conversion of nitric acid dihydrate to the stable trihydrate phase brings the computed levels of denitrification closer to the measurements. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0320 Atmospheric Composition and Sb~lctureC: loud physics and chemistry; 0340 Atmospheric Composition and Structure: Middle atmosphere-composition and chemistry

Irie, H.↗

NASA NTRS1989

Self-limiting physical and chemical effects in volcanic eruption clouds

One-dimensional aerosol microphysical and photochemical models are used to study the chemistry of stratospheric volcanic clouds. The results indicate that the aerosol microphysical processes of condensation and coagulation produce larger particles as the SO2 injection rate is increased. Larger particles have a smaller optical depth per unit mass and settle out of the stratosphere at a faster rate than smaller ones, restricting the total number of particles in the stratosphere. The microphysical processes moderate the impact of volcanic clouds on the earth's radiation budget and climate, suggesting that volcanic effects may be self limiting. It is noted that the injection of HCl into the stratosphere, which could lead to large ozone changes, is limited by a cold trap effect in which HCl and water vapor condense on ash particles in the rising volcanic plume and fall out as ice.

Pinto, Joseph P.↗