Cloud-Aerosol Interactions: Retrieving Aerosol Angstrom Exponents from CALIPSO Measurements of Opaque Water Clouds
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The NASA/Goddard Subseasonal to Seasonal (GEOS-S2S) prediction model includes an interactive aerosol model that allows for prediction of aerosol optical depth (AOD) and PM2.5, as well as improved meteorological forecasts under certain conditions. A model intercomparison of the impact of interactive aerosol is under way, and results from retrospective forecasts with and without interactive aerosol were performed using GEOS-S2S as part of this intercomparison. Results from the GEOS-S2S system will be shown, demonstrating useful skill in AOD and PM2.5 and an example of the impact on a "forecast of opportunity". These results will serve as motivation for the participation of CESM in this interactive aerosol model intercomparison.
We present here a first global modeling study on the influence of gas-phase chemistry/aerosol interactions on estimates of anthropogenic forcing by tropospheric O3 and aerosols. Concentrations of gas-phase species and sulfate, nitrate, ammonium, black carbon, primary organic carbon, secondary organic carbon, sea salt, and mineral dust aerosols in the preindustrial, present-day, and year 2100 (IPCC SRES A2) atmospheres are simulated online in the Goddard Institute for Space Studies general circulation model II' (GISS GCM II'). With fully coupled chemistry and aerosols, the preindustrial, presentday, and year 2100 global burdens of tropospheric ozone are predicted to be 190, 319, and 519 Tg, respectively. The burdens of sulfate, nitrate, black carbon, and organic carbon are predicted respectively to be 0.32. 0.18, 0.01, 0.33 Tg in preindustrial time, 1.40, 0.48, 0.23, 1.60 Tg in presentday, and 1.37, 1.97, 0.54, 3.31 Tg in year 2100. Anthropogenic O3 is predicted to have a globally and annually averaged present-day forcing of +0.22 W m(sup -2) and year 2100 forcing of +0.57 W m(sup -2) at the top of the atmosphere (TOA). Net anthropogenic TOA forcing by internally mixed sulfate, nitrate, organic carbon, and black carbon aerosols is estimated to be virtually zero in the present-day and +0.34 W m(sup -2) in year 2100, whereas it is predicted to be -0.39 W m(sup -2) in present-day and -0.61 W m(sup -2) in year 2100 if the aerosols are externally mixed. Heterogeneous reactions are shown to be important in affecting anthropogenic forcing. When reactions of N2O5, NO3, NO2, and HO2 on aerosols are accounted for, TOA anthropogenic O3 forcing is less by 20-45% in present-day and by 20-32% in year 2100 at mid to high latitudes in the Northern Hemisphere, as compared with values predicted in the absence of heterogeneous gas aerosol reactions. Mineral dust uptake of HNO3 and O3 is shown to have practically no influence on anthropogenic O3 forcing. Heterogeneous reactions of N2Os, NO3, NO2, and HO2 are predicted to have noticeable impacts on anthropogenic aerosol forcing over industrialized areas, leading to 0-2 W m(sup -2) more anthropogenic aerosol cooling in present-day and 2-8 W m(sup -2) more cooling in year 2100 in these areas as compared with forcings calculated in the absence of heterogeneous reactions. Sea salt uptake of SO2 reduces the magnitude of TOA aerosol cooling by 0.5-1 W m(sup -2) over the oceans around 60 N in the present-day and year 2100 scenarios. Near dust sources, mineral dust uptake of SO2 and HNO3 leads to less anthropogenic aerosol cooling by 0.5-1 W m(sup -2) in the present day and 1-2 W m(sup -2) in year 2100.
Aerosol particles are input into the troposphere by biomass burning, among other sources. These aerosol palls cover large expanses of the earth's surface. Aerosols may directly scatter solar radiation back to space, thus increasing the earth's albedo and act to cool the earth's surface and atmosphere. Aerosols also contribute to the earth's energy balance indirectly. Hygroscopic aerosol act as cloud condensation nuclei (CCN) and thus affects cloud properties. In 1977, Twomey theorized that additional available CCN would create smaller but more numerous cloud droplets in a cloud with a given amount of liquid water. This in turn would increase the cloud albedo which would scatter additional radiation back to space and create a similar cooling pattern as the direct aerosol effect. Estimates of the magnitude of the aerosol indirect effect on a global scale range from 0.0 to -4.8 W/sq m. Thus the indirect effect can be of comparable magnitude and opposite in sign to the estimates of global greenhouse gas forcing Aerosol-cloud interaction is not a one-way process. Just as aerosols have an influence on clouds through the cloud microphysics, clouds have an influence on aerosols. Cloud droplets are solutions of liquid water and CCN, now dissolved. When the cloud droplet evaporates it leaves behind an aerosol particle. This new particle does not have to have the same properties as the original CCN. In fact, studies show that aerosol particles that result from cloud processing are larger in size than the original CCN. Optical properties of aerosol particles are dependent on the size of the particles. Larger particles have a smaller backscattering fraction, and thus less incoming solar radiation will be backscattered to space if the aerosol particles are larger. Therefore, we see that aerosols and clouds modify each other to influence the radiative balance of the earth. Understanding and quantifying the spatial and seasonal patterns of the aerosol indirect forcing may have even greater consequences. Presently we know that through the use of fossil fuel and land-use changes we have increased the concentration of greenhouse gases in the atmosphere. In parallel, we have seen a modest increase of global temperature in the last century. These two observations have been linked as cause and effect by climate models, but this connection is still experimentally not verified. The spatial and seasonal distribution of aerosol forcing is different from that of greenhouse gases, thus generating a different spatial fingerprint of climate change. This fingerprint was suggested as a method to identify the response of the climate system to anthropogenic forcing of greenhouse gases and aerosol. The aerosol fingerprint may be the only way to firmly establish the presence (or absence) of human impact on climate. Aerosol-cloud interaction through the indirect effect will be an important component of establishing this fingerprint.
The real-time treatment of interactive realistically varying aerosol in a global operational forecasting system, as opposed to prescribed (fixed or climatologically varying) aerosols, is a very difficult challenge that only recently begins to be addressed. Experiment results from a recent version of the NASA GEOS-5 forecasting system, inclusive of interactive aerosol treatment, are presented in this work. Four sets of 30 5-day forecasts are initialized from a high quality set of analyses previously produced and documented to cover the period from 15 August to 16 September 2006, which corresponds to the NASA African Monsoon Multidisciplinary Analysis (NAMMA) observing campaign. The four forecast sets are at two different horizontal resolutions and with and without interactive aerosol treatment. The net impact of aerosol, at times in which there is a strong dust outbreak, is a temperature increase at the dust level and decrease in the near-surface levels, in complete agreement with previous observational and modeling studies. Moreover, forecasts in which interactive aerosols are included depict an African Easterly (AEJ) at slightly higher elevation, and slightly displace northward, with respect to the forecasts in which aerosols are not include. The shift in the AEJ position goes in the direction of observations and agrees with previous results.
The state of the art for predicting climate changes due to increasing greenhouse gasses in the atmosphere with high accuracy is problematic. Confidence intervals on current long-term predictions (on the order of 100 years) are so large that the ability to make informed decisions with regard to optimum strategies for mitigating both the causes of climate change and its effects is in doubt. There is ample evidence in the literature that large sources of uncertainty in current climate models are various aerosol effects. One approach to furthering discovery as well as modeling, and verification and validation (V&V) for cloud-aerosol interactions is use of a large "cloud chamber" in a complimentary role to in-situ and remote sensing measurement approaches. Reproducing all of the complex interactions is not feasible, but it is suggested that the physics of certain key processes can be established in a laboratory setting so that relevant fluid-dynamic and cloud-aerosol phenomena can be experimentally simulated and studied in a controlled environment. This report presents a high-level argument for significantly improved laboratory capability, and is meant to serve as a starting point for stimulating discussion within the climate science and other interested communities.
Effect of aerosols from biomass burning on the early development of East Asian monsoon is investigated using various satellites and in situ observations including TOMS Aerosol Index (AI). GPCP precipitation, ISCCP cloud cover, and GISS surface air temperature. Based on TRMM fire produce and mean winds fields at 85Omb. we identified the source and interaction regions of aerosols and investigated aerosol-cloud-precipitation characteristics in those regions. During March-April, northern Thailand, Myanmar. and Laos are major source of smoke from the combustion of agricultural waste. Excessive smoke. represented by high AI, is observed especially during dry and cloud-free year. On the other hand. there is no ground source of smoke in the interaction region. The most of aerosols in this area are believed to be transported from the source region. AI is appeared to be correlated with more clouds and less precipitation in interaction region. It suggests that the aerosol-cloud interaction can alter the distribution of cloud and the characteristics of regional hydrology. Aerosol-induced changes in atmospheric stability and associated circulation turns out to be very important to pre-monsoon rainfall pattern in southern China. Prolonged biomass burning is especially effective in changing rainfall pattern during April and May. Results suggest that excessive aerosol transported from source region may intensify pre-monsoon rain band over central China in May and lead to early monsoon onset.
During the Coupled Ocean-Atmosphere Response Experiment (COARE) of the Tropical Ocean and the Global Atmosphere (TOGA) program we measured cloud and aerosol particles aboard the NASA DC-8 over the warm pool of the western Pacific. Instruments on the aircraft included a condensation nuclei counter, optical particle counters, two-dimensional shadow probes and an ice crystal replicator. The size range covered by these instruments was from =0.01 micron to 6.4 mm diameter; particle shapes were determined for particles of sizes D greater than 1 micron.
The Goddard Cumulus Ensemble (GCE) model with bin spectra microphysics is used to simulate mesoscale convective systems.The model uses explicit bins to represent size spectra of cloud nuclei, water drops, ice crystals, snow and graupel. Each hydrometeorite category is described by 33 mass bins. The simulations provide a unique data set of simulated raindrop size distribution in a realistic dynamic frame. Calculations of radar parameters using simulated drop size distribution serve as an evaluation of numerical model performance. In addition, the GCE bin spectra modes is a very useful tool to study uncertainties related to radar observations; all the environmental parameters are precisely known. In this presentation, we concentrate on the discussion of Z-R (ZDR-R) relation in the simulated systems. Due to computational limitations, the spectra bin model has been run in two dimensions with 31 stretched vertical layers and 1026 horizontal grid points (1 km resolution). Two different cases, one in midlatitude continent, the other in tropical ocean, have been simulated. The continental case is a strong convection which lasted for two hours. The oceanic case is a persistent system with more than 10 hours' life span. It is shown that the simulated Z-R (ZDR-R) relations generally agree with observations using radar and rain gauge data. The spatial and temporal variations of Z-R relation in different locations are also analyzed. Impact of aerosols on cloud formation and raindrop size distribution was studied. Both clean (low CCN) and dirty (high CCN) cases are simulated. The Z-R relation is shown to vary considerable in the initial CCN concentrations.
The reaction of SO2 and NO2 with soot has been studied experimentally by gravimetric determination of chemisorption with subsequent analysis of the chemisorbed species by various techniques. When samples of commercially available carbon black (used as soot surrogate) are exposed to SO2 or NO2 in dry air or N2 as carrier gas, no quantitative chemisorption (less than 5 micrograms per mg of substrate) is observed. However, exposure of the same grade of carbon to a combination of SO2 and NO2 in dry air of N2 results in significant chemisorption (180-200 micrograms/mg), a major fraction of which is analyzed as sulfate.
This article investigates the impact 3 of Saharan dust on the development of tropical cyclones in the Atlantic. A global data assimilation and forecast system, the NASA GEOS-5, is used to assimilate all satellite and conventional data sets used operationally for numerical weather prediction. In addition, this new GEOS-5 version includes assimilation of aerosol optical depth from the Moderate Resolution Imaging Spectroradiometer (MODIS). The analysis so obtained comprises atmospheric quantities and a realistic 3-d aerosol and cloud distribution, consistent with the meteorology and validated against Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and CloudSat data. These improved analyses are used to initialize GEOS-5 forecasts, explicitly accounting for aerosol direct radiative effects and their impact on the atmospheric dynamics. Parallel simulations with/without aerosol radiative effects show that effects of dust on static stability increase with time, becoming highly significant after day 5 and producing an environment less favorable to tropical cyclogenesis.
Aerosol effects on micro/macrophysical properties of marine stratocumulus clouds over the western North Atlantic Ocean (WNAO) are investigated using in situ measurements and large-eddy simulations (LES) for two cold-air outbreak (CAO) cases (28 February and 1 March 2020) during the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). The LES is able to reproduce the vertical profiles of liquid water content (LWC), effective radius reff and cloud droplet number concentration Nc from fast cloud droplet probe (FCDP) in situ measurements for both cases. Furthermore, we show that aerosols affect cloud properties (N c , r eff , and LWC) via the prescribed bulk hygroscopicity of aerosols (¯k) and aerosol size distribution characteristics. N c , r eff , and liquid water path (LWP) are positively correlated to ¯κ and aerosol number concentration (N a ) while cloud fractional cover (CFC) is insensitive to ¯κ and aerosol size distributions for the two cases. The realistic changes to aerosol size distribution (number concentration, width, and the geometrical diameter) with the same meteorology state allow us to investigate aerosol effects on cloud properties without meteorological feedback. We also use the LES results to evaluate cloud properties from two reanalysis products, ERA5 and MERRA-2. Compared to LES, the ERA5 is able to capture the time evolution of LWP and total cloud coverage within the study domain during both CAO cases while MERRA-2 underestimates them.
Southern Africa produces almost a third of the Earth’s biomass burning (BB) aerosol particles, yet the fate of these particles and their influence on regional and global climate is poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA EVS-2 (Earth Venture Suborbital-2) investigation with three intensive observation periods designed to study key atmospheric processes that determine the climate impacts of these aerosols. During the Southern Hemisphere winter and spring (June–October), aerosol particles reaching 3–5 km in altitude are transported westward over the southeast Atlantic, where they interact with one of the largest subtropical stratocumulus (Sc) cloud decks in the world. The representation of these interactions in climate models remains highly uncertain in part due to a scarcity of observational constraints on aerosol and cloud properties, as well as due to the parameterized treatment of physical processes. Three ORACLES deployments by the NASA P-3 aircraft in September 2016, August 2017, and October 2018 (totaling ~ 350 science flight hours), augmented by the deployment of the NASA ER-2 aircraft for remote sensing in September 2016 (totaling ~ 100 science flight hours), were intended to help fill this observational gap. ORACLES focuses on three fundamental science themes centered on the climate effects of African BB aerosols: (a) direct aerosol radiative effects, (b) effects of aerosol absorption on atmospheric circulation and clouds, and (c) aerosol–cloud microphysical interactions. This paper summarizes the ORACLES science objectives, describes the project implementation, provides an overview of the flights and measurements in each deployment, and highlights the integrative modeling efforts from cloud to global scales to address science objectives. Significant new findings on the vertical structure of BB aerosol physical and chemical properties, chemical aging, cloud condensation nuclei, rain and precipitation statistics, and aerosol indirect effects are emphasized, but their detailed descriptions are the subject of separate publications. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project and the dataset it produced.
Observations from the US Department of Energy's Atmospheric Radiation Measurement (ARM) program are used to evaluate the ability of the NASA GISS ModelE global climate model in reproducing observed interactions between aerosols and clouds. Included in the evaluation are comparisons of basic meteorology and aerosol properties, droplet activation, effective radius parameterizations, and surface-based evaluations of aerosol-cloud interactions (ACI). Differences between the simulated and observed ACI are generally large, but these differences may result partially from vertical distribution of aerosol in the model, rather than the representation of physical processes governing the interactions between aerosols and clouds. Compared to the current observations, the ModelE often features elevated droplet concentrations for a given aerosol concentration, indicating that the activation parameterizations used may be too aggressive. Additionally, parameterizations for effective radius commonly used in models were tested using ARM observations, and there was no clear superior parameterization for the cases reviewed here. This lack of consensus is demonstrated to result in potentially large, statistically significant differences to surface radiative budgets, should one parameterization be chosen over another.
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The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) included 40 research flights in the winter and summer months of 2020 using a two-aircraft approach to simultaneously obtain in situ and remote sensing data of regions below, inside, and above boundary layer clouds. This presentation will summarize early findings from the first year of ACTIVATE flights with focus on aerosol and cloud droplet number concentration behavior, formation and evolution of clouds, and analysis of remote sensing retrievals of aerosol and cloud properties. There is a clear annual cycle in cloud droplet number concentration suggesting a marked annual cycle in aerosol-cloud interactions. Although aerosol particles are more abundant in spring and summer, the conditions needed to activate those particles into cloud droplets are weaker than in other colder months. Several flights targeted post-frontal clouds associated with cold air outbreaks pointing to enhanced levels of nucleated particles immediately above such clouds, and that ice formation hastens the transition from closed to open cloud structures in the sampled CAO events. Also observed in the marine boundary layer during CAOs is the frequent occurrence of non-spherical sea salt particles, which has significant implications for remote sensing retrievals.
This chapter describes the aerosol–radiation interactions of absorption, scattering, and emission of electromagnetic radiation by atmospheric aerosol particles, which alter the fluxes of radiative energy in the atmosphere. The chapter begins by defining some fundamental processes, including the particle physical and optical properties that determine the amount of light scattered and absorbed. It then outlines the factors that determine the radiative effect of aerosol–radiation interactions in the atmosphere, including the solar zenith angle, the properties of underlying surfaces, the influence of clouds, and atmospheric temperature, and humidity profiles. It defines the magnitude of the aerosol radiative effect on the climate system as well as the radiative forcing over the industrial period determined from satellite measurements and models for clear-sky and all-sky conditions.
Aerosols have a potentially large effect on climate, particularly through their interactions with clouds, but the magnitude of this effect is highly uncertain. Large volcanic eruptions produce sulfur dioxide, which in turn produces aerosols; these eruptions thus represent a natural experiment through which to quantify aerosol-cloud interactions. Here we show that the massive 2014-2015 fissure eruption in Holuhraun, Iceland, reduced the size of liquid cloud droplets - consistent with expectations - but had no discernible effect on other cloud properties. The reduction in droplet size led to cloud brightening and global-mean radiative forcing of around minus 0.2 watts per square metre for September to October 2014. Changes in cloud amount or cloud liquid water path, however, were undetectable, indicating that these indirect effects, and cloud systems in general, are well buffered against aerosol changes. This result will reduce uncertainties in future climate projections, because we are now able to reject results from climate models with an excessive liquid-water-path response.