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NASA NTRS2022

Cloud Adjustments From Large-Scale Smoke–Circulation Interactions Strongly Modulate the Southeastern Atlantic Stratocumulus-to-Cumulus Transition

Smoke from southern Africa blankets the southeastern Atlantic Ocean from June to October, producing strong and competing aerosol radiative effects. Smoke effects on the transition between overcast stratocumulus and scattered cumulus clouds are investigated along a Lagrangian (air-mass-following) trajectory in regional climate and large eddy simulation models. Results are compared with observations from three recent field campaigns that took place in August 2017: ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES), CLouds and Aerosol Radiative Impacts and Forcing: Year 2017 (CLARIFY), and Layered Atlantic Smoke Interactions with Clouds (LASIC). The case study is set up around the joint ORACLES–CLARIFY flight that took place near Ascension Island on 18 August 2017. Smoke sampled upstream on an ORACLES flight on 15 August 2017 likely entrained into the marine boundary layer later sampled during the joint flight. The case is first simulated with the WRF-CAM5 regional climate model in three distinct setups: (1) FireOn, in which smoke emissions and any resulting smoke–cloud–radiation interactions are included; (2) FireOff, in which no smoke emissions are included; (3) RadOff, in which smoke emissions and their microphysical effects are included but aerosol does not interact directly with radiation. Over the course of the Lagrangian trajectory, differences in free tropospheric thermodynamic properties between FireOn and FireOff are nearly identical to those between FireOn and RadOff, showing that aerosol–radiation interactions are primarily responsible for the free tropospheric effects. These effects are non-intuitive: in addition to the expected heating within the core of the smoke plume, there is also a “banding” effect of cooler temperature (∼1–2 K) and greatly enhanced moisture (>2 g kg−1) at the plume top. This banding effect is caused by a vertical displacement of the former continental boundary layer in the free troposphere in the FireOn simulation resulting from anomalous diabatic heating due to smoke absorption of sunlight that manifests primarily as a few hundred meters per day reduction in large-scale subsidence over the ocean. A large eddy simulation (LES) is then forced with free tropospheric fields taken from the outputs for the WRF-CAM5 FireOn and FireOff runs. Cases are run by selectively perturbing one variable (e.g., aerosol number concentration, temperature, moisture, vertical velocity) at a time to better understand the contributions from different indirect (microphysical), “large-scale” semi-direct (above-cloud thermodynamic and subsidence changes), and “local” semi-direct (below-cloud smoke absorption) effects. Despite a more than 5-fold increase in cloud droplet number concentration when including smoke aerosol concentrations, minimal differences in cloud fraction evolution are simulated by the LES when comparing the base case with a perturbed aerosol case with identical thermodynamic and dynamic forcings. A factor of 2 decrease in background free tropospheric aerosol concentrations from the FireOff simulation shifts the cloud evolution from a classical entrainment-driven “deepening–warming” transition to trade cumulus to a precipitation-driven “drizzle-depletion” transition to open cells, however. The thermodynamic and dynamic changes caused by the WRF-simulated large-scale adjustments to smoke diabatic heating strongly influence cloud evolution in terms of both the rate of deepening (especially for changes in the inversion temperature jump and in subsidence) and in cloud fraction on the final day of the simulation (especially for the moisture “banding” effect). Such large-scale semi-direct effects would not have been possible to simulate using a small-domain LES model alone.

southeast Atlantic Ocean↗
NASA NTRS1993

Radiative climate forcing by the Mount Pinatubo eruption

Radiative flux anomalies derived from the NASA spaceborne Earth Radiation Budget Experiment were used to determine the volcanic radiative forcing that followed the eruption of Mount Pinatubo in June 1991. They are the first unambiguous, direct measurements of large-scale volcanic forcing. The volcanic aerosols caused a strong cooling effect immediately; the amount of cooling increased through September 1991 as shortwave forcing increased relative to the longwave forcing. The primary effects of the aerosols were a direct increase in albedo over mostly clear areas and both direct and indirect increases in the albedo of cloudy areas.

Minnis, P.↗
NASA NTRS2011

Validating and Improving Long-Term Aerosol Data Records from SeaWiFS

Natural and anthropogenic aerosols influence the radiative balance of the Earth through direct and indirect interactions with incoming solar radiation. However, the quantification of these interactions and their ultimate effect on the Earth's climate still have large uncertainties. This is partly due to the limitations of current satellite data records which include short satellite lifetimes, retrieval algorithm uncertainty, or insufficient calibration accuracy. We have taken the first steps in overcoming this hurdle with the production and public release of an aerosol data record using the radiances from the Sea-viewing Wide Field-of-View Sensor (Sea WiFS). Sea WiFS was launched in late 1997 and provided exceptionally well-calibrated top-of-atmosphere radiance data until December 2010, more than 13 years. We have partnered this data with an expanded Deep Blue aerosol retrieval algorithm. In accordance with Deep Blue's original focus, the latest algorithm retrieves aerosol properties not only over bright desert surfaces, but also over oceans and vegetated surfaces. With this combination of a long time series and global algorithm, we can finally identify the changing patterns of regional aerosol loading and provide insight into longterm variability and trends of aerosols on regional and global scales. In this work, we provide an introduction to Sea WiFS, the current algorithms, and our aerosol data records. We have validated the data over land and ocean with ground measurements from the Aerosol Robotic Network (AERONET) and compared them with other satellites such as MODIS and MISR. Looking ahead to the next data release, we will also provide details on the implemented and planned algorithm improvements, and subsequent validation results.

Bettenhausen, Corey↗
NASA NTRSDate not supplied

TPSAS-NF1676L-11382-DND

Long-range transport of ozone precursor species and carbonaceous aerosols emitted by wildfires may affect the atmospheric composition and regional climate far away from the location of the fires. Major outbreaks of fires occurred in 3 areas of Asia, Kazakhstan, Siberia, and Thailand, during the spring of 2008. Satellite and aircraft-based observations and trajectory studies have identified the transit of the plumes from these fires across the Pacific. We have conducted simulations of the effects of these fires on the atmospheric composition using the Real-time Air Quality Modeling System (RAQMS). RAQMS is a global scale meteorological and chemical modeling system with unified (stratosphere/troposphere) chemistry module. Model results, for example, indicate that increases of 10 ppbv in upper tropospheric ozone at 180W longitude and northern mid-latitudes in April, 2008 could be attributed to these fires. Large increases in aerosol optical depth due to carbonaceous aerosols are also seen nearer the fire location. Both tropospheric ozone and carbonaceous aerosols influence the atmospheric energy balance and climate. We use an off-line radiative transfer model along with the RAQMS chemical and aerosol analyses to calculate the direct radiative forcing during April, 2008, due to Asian wildfire emissions. Arctic indirect radiative forcing due to these emissions are evaluated using RAQMS aerosol extinction analyses in conjunction with MODIS retrievals of cloud liquid water and effective radius. We will discuss the radiative forcing results and the relative influences of the different fire events.

Murali Natarajan↗
NASA NTRS2019

Polarimetric Retrievals of Cloud Droplet Number Concentrations

Cloud droplet number concentration (Nd) is an important parameter of liquid clouds and is crucial to understanding aerosol-cloud interactions. It couples boundary layer aerosol composition, size and concentration with cloud reflectivity. It affects cloud evolution, precipitation, radiative forcing, global climate and, through observation, can be used to partially monitor the first indirect effect. With its unique combination of multi-wavelength, multi-angle, total and polarized reflectance measurements, the Research Scanning Polarimeter (RSP) retrieves Nd with relatively few assumptions. The approach involves measuring cloud optical thickness, mean droplet extinction cross-section and cloud physical thickness. Polarimetric observations are capable of measuring the effective variance, or width, of the droplet size distribution. Estimating cloud geometrical thickness is also an important component of the polarimetric Nd retrieval, which is accomplished using polarimetric measurements in a water vapor absorption band to retrieve the amount of in-cloud water vapor and relating this to physical thickness. We highlight the unique abilities and quantify uncertainties of the polarimetric approach. We validate the approach using observational data from the North Atlantic and Marine Ecosystems Study (NAAMES). NAAMES targets specific phases in the seasonal phytoplankton lifecycle and ocean-atmosphere linkages. This study provides an excellent opportunity for the RSP to evaluate its approach of sensing Nd over a range of concentrations and cloud types with in situ measurements from a Cloud Droplet Probe (CDP). The RSP and CDP, along with an array of other instruments, are flown on the NASA C-130 aircraft, which flies in situ and remote sensing legs in sequence. Cloud base heights retrieved by the RSP compare well with those derived in situ (R=0.83) and by a ceilometer aboard the R.V. Atlantis (R=0.79). Comparing geometric mean values from 12 science flights throughout the NAAMES-1 and NAAMES-2 campaigns, we find a strong correlation between Nd retrieved by the RSP and CDP (R=0.96). A linear least squares fit has a slope of 0.92 and an intercept of 0.3 cm−3. Uncertainty in this comparison can be attributed to cloud 3D effects, nonlinear liquid water profiles, multilayered clouds, measurement uncertainty, variation in spatial and temporal sampling, and assumptions used within the method. Radiometric uncertainties of the RSP measurements lead to biases on derived optical thickness and cloud physical thickness, but these biases largely cancel out when deriving Nd for most conditions and geometries. We find that a polarimetric approach to sensing Nd is viable and the RSP is capable of accurately retrieving Nd for a variety of cloud types and meteorological conditions.

Droplet concentration↗
NASA NTRS1994

Effects of the Mount Pinatubo eruption on the radiative and chemical processes in the troposphere and stratosphere

The Lawrence Livermore National Laboratory two-dimensional zonally-averaged chemical-radiative-transport model of the global atmosphere was used to study the effects of the 15 June 1991 eruption of the Mt. Pinatubo volcano on stratospheric processes. SAGE 2 time-dependent aerosol surface area density and optical extinction data were used as input into the model. By 22 December 1991, a maximum equatorial change of -1.8 percent in column ozone was derived from heterogeneous chemical processes that convert NO(x) into HNO3 on sulfuric acid aerosols. Radiative feedbacks from increased aerosol optical thickness independently changes column ozone by approximately -3.5 percent for the same period. This occurs from increasing the net heating of the lower stratosphere, which indirectly increases chemical reaction rates via their temperature dependence and from changes in actinic fluxes, which directly modify photodissociation rates. Including both heterogeneous and radiative effects changes column ozone by -5.5 percent. The model-derived change overestimates the decrease in column ozone relative to the TOMS instrument on the Nimbus 7 satellite. Maximum local ozone decreases of 12 percent were derived in the equatorial region, at 25 km. Model-derived column NO2 peaked (-14 percent) at 30 deg S in October 1991. The timing of the NO2 peak is consistent with observation, but the model underestimates the magnitude of the decrease. Local concentrations of NO(x) (NO + NO2), ClO(x) (Cl + ClO), and HO(x) (OH + HO2), in the lower stratosphere between 30 deg S and 30 deg N, were calculated to have changed by -40 percent, +100 to +160 percent, and +120 to +140 percent respectively.

Kinnison, Douglas E.↗
NASA NTRSDate not supplied

Impact of COVID-Global Shutdown on Earth's Radiation Budget

Climate is fueled by how much of the sun’s energy is absorbed by Earth. Changes in aerosol emissions have a direct impact how much solar energy is absorbed under clear-sky conditions, which occurs roughly one-third of the time globally. Aerosol emission changes can also indirectly influence clouds and further alter solar energy absorption. In this presentation, we examine the impact of the COVID-19 global shutdown on Earth’s radiation budget at global and regional scales and compare it with other changes that have had an influence on Earth's radiation budget during the past 20 years—including policy-related emission controls, wildfire events and changes in sea-ice extent in polar regions. We use a novel analysis technique together with data from NASA instruments on the Terra, Aqua and Aura satellites and reanalysis data from MERRA-2. We also compare results with state-of-the-art general circulation models that have been nudged to reanalysis data (winds, air temperature and surface 25 pressure) at all levels. Our preliminary results show that the largest COVID-19 impact occurs regionally over the East Asian Marginal Seas, just off the coast of China. We find a 30% reduction in aerosol optical depth according to the MODIS instrument, and an 8% reduction in reflected solar radiation according to the CERES radiation budget instrument. The climate model simulations show remarkable consistency with the observations and furthermore show no evidence of an indirect effect on cloud properties.

Norman G. Loeb↗
NASA NTRS2007

Aerosol Measurements of the Fine and Ultrafine Particle Content of Lunar Regolith

We report the first quantitative measurements of the ultrafine (20 to 100 nm) and fine (100 nm to 20 m) particulate components of Lunar surface regolith. The measurements were performed by gas-phase dispersal of the samples, and analysis using aerosol diagnostic techniques. This approach makes no a priori assumptions about the particle size distribution function as required by ensemble optical scattering methods, and is independent of refractive index and density. The method provides direct evaluation of effective transport diameters, in contrast to indirect scattering techniques or size information derived from two-dimensional projections of high magnification-images. The results demonstrate considerable populations in these size regimes. In light of the numerous difficulties attributed to dust exposure during the Apollo program, this outcome is of significant importance to the design of mitigation technologies for future Lunar exploration.

Greenberg, Paul S.↗
NASA NTRS2017

Exploring the Elevated Water Vapor Signal Associated with Biomass Burning Aerosol over the Southeast Atlantic Ocean

The quantification of radiative forcing due to the cumulative effects of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in our understanding of the physical climate. How the magnitude of these effects may be modified by meteorological conditions is an important aspect of this question. The Southeast Atlantic Ocean (SEA), with seasonal biomass burning (BB) smoke plumes overlying a persistent stratocumulus cloud deck, offers a perfect natural observatory in which to study the complexities of aerosol-cloud interactions. The NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign consists of three field deployments over three years (2016-2018) with the goal of gaining a better understanding of the complex processes (direct and indirect) by which BB aerosols affect clouds. We present results from the first ORACLES field deployment, which took place in September 2016 out of Walvis Bay, Namibia. Two NASA aircraft were flown with a suite of aerosol, cloud, radiation, and meteorological instruments for remote-sensing and in-situ observations. A strong correlation was observed between the aircraft-measured pollution indicators (carbon monoxide and aerosol properties) and atmospheric water vapor content, at all altitudes. Atmospheric reanalysis indicates that convective dynamics over the continent, near likely contribute to this elevated signal. Understanding the mechanisms by which water vapor covaries with plume strength is important to quantifying the magnitude of the aerosol direct and semi-direct effects in the region.

Pistone, Kristina↗
NASA NTRS2018

PACE Technical Report Series, Volume 4: Cloud Retrievals in the PACE Mission: PACE Science Team Consensus Document

Earth is a complex dynamical system exhibiting continuous change in its atmosphere, ocean,and surface elements. Nearly all (99.97%) of the energy driving these systems is linked to the Sun. Measurements of reflected sunlight contain a unique signature of wavelength-specific scattering and absorption interactions occurring between incoming solar energy and atmospheric (molecules, aerosols,clouds) and surface features Clouds can affect significantly both shortwave and long wave radiation, depending on altitude/vertical structure, thermodynamic phase, and optical properties. Low, warm, and optically thick clouds predominantly have a cooling effect, while high, cold, optically thin clouds can cause warming by absorbing warmer radiation emitted from the surface and lower atmosphere.When the net difference between outgoing and incoming solar radiation is matched by the net infrared radiation emitted to space, the Earth's climate is in radiative balance. While radiative forcing components (GHGs, aerosols - direct and indirect) contribute to a net radiative imbalance, climate sensitivity is ultimately determined by the contribution of various system feed backs. The role of cloud feedback in a warming climate is currently the largest inter-model uncertainty in climate sensitivity and therefore in climate prediction [Bony and Dufresne 2005]. A comprehensive understanding of current cloud propertiesand dynamic/microphysical processes requires a global perspective from satellites.

Plankton, Aerosol, Cloud, ocean Ecosystem (PACE)↗
NASA NTRS2016

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300 over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were 50 smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq))/ and various biomass burning tracers (BBt/ across the multi-campaign dataset, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACI, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be 0.12 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/ cu m) and very high aerosol concentrations (2000-3000 cu m) in the most polluted clouds, the estimated ACI value was only 0.06. In this case, competition for water vapor by the high concentration of CCN strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease shortwave radiative flux by 2 and 4 W/sq or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic. We lastly show evidence to suggest that numerous northern latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei. However, the influence of background particles on smoke-driven indirect effects is currently unclear.

Arctic↗
NASA NTRS2000

The Radiative Effects of Martian Water Ice Clouds on the Local Atmospheric Temperature Profile

Mars Pathfinder made numerous discoveries, one of which was a deep temperature inversion that extended from about 15 km down to 8 km above the surface. It has been suggested by Haberle et al. (1999. J. Geophys. Res. 104, 8957-8974.) that radiative cooling by a water ice cloud may generate such an inversion. Clouds can strongly affect the local air temperature due to their ability to radiate efficiently in the infrared and due to the low air mass of the martian atmosphere, which allows the temperature to change during the relatively short lifetime of a cloud. We utilize a time-dependent microphysical aerosol model coupled to a radiative--convective model to explore the effects water ice clouds have on the local martian temperature profile. We constrain the dust and water vapor abundance using data from the Viking Missions and Mars Pathfinder. Water t ice clouds with visible optical depths of r > 0.1 form readily in these simulations. These clouds alter the local air temperature directly, through infrared cooling, and indirectly, by redistributing atmospheric dust. With this model we are able to reproduce the temperature inversions observed by Mars Pathfinder and Mars Global t Surveyor 2000 Academic Press

Colaprete, Anthony↗
NASA NTRS2005

Anvil Glaciation in a Deep Cumulus Updraught over Florida Simulated with the Explicit Microphysics Model. I: Impact of Various Nucleation Processes

Simulations of a cumulonimbus cloud observed in the Cirrus regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE) with an advanced version of the Explicit Microphysics Model (EMM) are presented. The EMM has size-resolved aerosols and predicts the time evolution of sizes, bulk densities and axial ratios of ice particles. Observations by multiple aircraft in the troposphere provide inputs to the model, including observations of the ice nuclei and of the entire size distribution of condensation nuclei. Homogeneous droplet freezing is found to be the source of almost all of the ice crystals in the anvil updraught of this particular model cloud. Most of the simulated droplets that freeze to form anvil crystals appear to be nucleated by activation of aerosols far above cloud base in the interior of the cloud ("secondary" or "in cloud" droplet nucleation). This is partly because primary droplets formed at cloud base are invariably depleted by accretion before they can reach the anvil base in the updraught, which promotes an increase with height of the average supersaturation in the updraught aloft. More than half of these aerosols, activated far above cloud base, are entrained into the updraught of this model cloud from the lateral environment above about 5 km above mean sea level. This confirms the importance of remote sources of atmospheric aerosol for anvil glaciation. Other nucleation processes impinge indirectly upon the anvil glaciation by modifying the concentration of supercooled droplets in the upper levels of the mixed-phase region. For instance, the warm-rain process produces a massive indirect impact on the anvil crystal concentration, because it determines the mass of precipitation forming in the updraught. It competes with homogeneous freezing as a sink for cloud droplets. The effects from turbulent enhancement of the warm-rain process and from the nucleation processes on the anvil ice properties are assessed.

Phillips, Vaughan T. J.↗
NASA NTRS2003

Limits to the Indirect Aerosol Forcing in Stratocumulus

The indirect radiative forcing of aerosols is poorly constrained by the observational data underlying the simple cloud parameterizations in GCMs. signal of cloud response to increased aerosol concentrations from meteorological noise. Recent satellite observations indicate a significant decrease of cloud water in ship tracks, in contrast to an ensemble of in situ measurements showing no average change in cloud water relative to the surrounding clouds. Both results contradict the expectation of cloud water increasing in polluted clouds. We find through large-eddy simulations of stratocumulus that the trend in the satellite data is likely an artifact of sampling only overcast clouds. The simulations instead show cloud cover increasing with droplet concentrations. The simulations also show that increases in cloud water from suppressing drizzle by increased droplet concentrations are favored at night or at extremely low droplet concentrations. At typical droplet concentrations we find that the Twomey effect on cloud albedo is amplified very little by the secondary indirect effect of drizzle suppression, largely because the absorption of solar radiation by cloud water reduces boundary-layer mixing in the daytime and thereby restricts any possible increase in cloud water from drizzle suppression. The cloud and boundary layer respond to radiative heating variations on a time scale of hours, and on longer time scales respond to imbalances between large-scale horizontal advection and the entrainment of inversion air. We analyze the co-varying response of cloud water, cloud thickness, width of droplet size distributions, and dispersion of the optical depth, as well as the overall response of cloud albedo, to changes in droplet concentrations. We also dissect the underlying physical mechanisms through sensitivity studies. Ship tracks represent an ideal natural laboratory to extricate the

Ackerman, Andrew↗
NASA NTRS2012

Retrieval of Aerosol Optical Depth Above Clouds from OMI Observations: Sensitivity Analysis, Case Studies

A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originated in arid and semi-arid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth atmosphere system is especially important. The generally negative (cooling) top of the atmosphere direct effect of absorbing aerosols, may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. In this paper we discuss the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol-cloud separation. The technique was applied to above-cloud aerosol events over the Southern Atlantic Ocean yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.

Torres, O.↗
NASA NTRS2016

Aircraft-Measured Indirect Cloud Effects from Biomass Burning Smoke in the Arctic and Subarctic

The incidence of wildfires in the Arctic and subarctic is increasing; in boreal North America, for example, the burned area is expected to increase by 200-300% over the next 50-100 years, which previous studies suggest could have a large effect on cloud microphysics, lifetime, albedo, and precipitation. However, the interactions between smoke particles and clouds remain poorly quantified due to confounding meteorological influences and remote sensing limitations. Here, we use data from several aircraft campaigns in the Arctic and subarctic to explore cloud microphysics in liquid-phase clouds influenced by biomass burning. Median cloud droplet radii in smoky clouds were approx. 40- 60% smaller than in background clouds. Based on the relationship between cloud droplet number (N(liq)/ and various biomass burning tracers (BBt/ across the multi-campaign data set, we calculated the magnitude of subarctic and Arctic smoke aerosol-cloud interactions (ACIs, where ACI = (1/3) x dln(N(liq))/dln(BBt)) to be approx. 0.16 out of a maximum possible value of 0.33 that would be obtained if all aerosols were to nucleate cloud droplets. Interestingly, in a separate subarctic case study with low liquid water content (0.02 gm/cu m and very high aerosol concentrations (2000- 3000/ cu cm in the most polluted clouds, the estimated ACI value was only 0.05. In this case, competition for water vapor by the high concentration of cloud condensation nuclei (CCN) strongly limited the formation of droplets and reduced the cloud albedo effect, which highlights the importance of cloud feedbacks across scales. Using our calculated ACI values, we estimate that the smoke-driven cloud albedo effect may decrease local summertime short-wave radiative flux by between 2 and 4 W/sq m or more under some low and homogeneous cloud cover conditions in the subarctic, although the changes should be smaller in high surface albedo regions of the Arctic.We lastly explore evidence suggesting that numerous northern-latitude background Aitken particles can interact with combustion particles, perhaps impacting their properties as cloud condensation and ice nuclei.

cloud microphysics↗
NASA NTRS2002

New Results from Space and Field Observations on the Aerosol Direct and Indirect Radiative Forcing

New space observations from the MODIS instrument on board the Terra satellite and analysis of POLDER data flown on the ADEOS satellite, show in great details the spatial and seasonal variability of the global aerosol system. These spaceborne instruments distinguish fine aerosol from man-made regional pollution and biomass burning from mostly natural coarse dust and sea salt aerosol. E.g. fine regional pollution in and around the Indian sub-continent, Europe and North America; smoke from biomass burning in Southern Africa and Southern America; coarse dust from West Africa and mixed dust pollution and smoke from West and central Africa and East Asia. These regions were also studied extensively in focused field experiments and by the distributed AERONET network. The results generate the first climatologies of the aerosol system, are used to derive the aerosol radiative effects and to estimate the anthropogenic component. The measurements are also used to evaluate each other and constrain aerosol transport models.

Kaufman, Yoram J.↗
NASA NTRS2011

Atmospheric Composition Change: Climate-Chemistry Interactions

Chemically active climate compounds are either primary compounds such as methane (CH4), removed by oxidation in the atmosphere, or secondary compounds such as ozone (O3), sulfate and organic aerosols, formed and removed in the atmosphere. Man-induced climate-chemistry interaction is a two-way process: Emissions of pollutants change the atmospheric composition contributing to climate change through the aforementioned climate components, and climate change, through changes in temperature, dynamics, the hydrological cycle, atmospheric stability, and biosphere-atmosphere interactions, affects the atmospheric composition and oxidation processes in the troposphere. Here we present progress in our understanding of processes of importance for climate-chemistry interactions, and their contributions to changes in atmospheric composition and climate forcing. A key factor is the oxidation potential involving compounds such as O3 and the hydroxyl radical (OH). Reported studies represent both current and future changes. Reported results include new estimates of radiative forcing based on extensive model studies of chemically active climate compounds such as O3, and of particles inducing both direct and indirect effects. Through EU projects such as ACCENT, QUANTIFY, and the AEROCOM project, extensive studies on regional and sector-wise differences in the impact on atmospheric distribution are performed. Studies have shown that land-based emissions have a different effect on climate than ship and aircraft emissions, and different measures are needed to reduce the climate impact. Several areas where climate change can affect the tropospheric oxidation process and the chemical composition are identified. This can take place through enhanced stratospheric-tropospheric exchange of ozone, more frequent periods with stable conditions favouring pollution build up over industrial areas, enhanced temperature-induced biogenic emissions, methane releases from permafrost thawing, and enhanced concentration through reduced biospheric uptake. During the last 510 years, new observational data have been made available and used for model validation and the study of atmospheric processes. Although there are significant uncertainties in the modelling of composition changes, access to new observational data has improved modelling capability. Emission scenarios for the coming decades have a large uncertainty range, in particular with respect to regional trends, leading to a significant uncertainty range in estimated regional composition changes and climate impact.

Atmosphere climate chemistry↗