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At least 37 records · Page 2

The Role of In-Cloud Wet Removal in Simulating Aerosol Vertical Profiles and Cloud Radiative Forcing

Among the physical processes controlling aerosol vertical profiles, in-cloud wet removal is of utmost importance while its representation in global climate models (GCMs) is crude. In this study, we implement into the Community Atmosphere Model version 6 (CAM6) a physically based aerosol wet removal parameterization scheme that explicitly treats aerosol activation, removal and resuspension. Evaluation against in-situ observations shows that the default scheme substantially overestimates the upper tropospheric black carbon (BC) and sea salt mass. Our physically based scheme reduces BC and sea salt mass by a factor of 10 and 1,000, respectively, in better agreement with observations. Also, the new scheme slightly increases number of aerosol particles between 12 nm and 4.8 μm in diameter, thereby mitigating the aerosol number underestimation in the default scheme. Our new scheme reduces the overestimation of coarse-mode aerosol (0.5–4.8 μm) number. Overall, the aerosol property changes (mass decrease and number increase) reduce the cloud condensation nuclei (CCN) concentration at low supersaturation (i.e., 0.02% and 0.1%), and increase CCN at high supersaturations (i.e., 0.5% and 1%). Consequently, the global annual mean cloud liquid water path increases by 1.89 g m -2 and the ice water path increases by 0.51 g m -2 . The global annual mean shortwave, longwave, and net cloud radiative forcing change by -1.06, 0.57, and -0.48 W m -2 , respectively. Further improvement is needed to reflect the real physics that the removal efficiencies for aerosol mass and number are disproportionate and to advect cloud-borne (activated) aerosols for a complete aerosol lifecycle.

54 ENVIRONMENTAL SCIENCES↗

Parameterization of Cloud Droplet Formation in Global Climate Models

An aerosol activation parameterization has been developed based on a generalized representation of aerosol size and composition within the framework of an ascending adiabatic parcel; this allows for parameterizing the activation of chemically complex aerosol with an arbitrary size distribution and mixing state. The new parameterization introduces the concept of"population splitting", in which the cloud condensation nuclei (CCN) that form droplets are treated as two separate populations; those that have a size close to their critical diameter and those that do not.Explicit consideration of kinetic limitations of droplet growth is introduced. Our treatment of the activation process unravels much of its complexity. As a result of this, a substantial number of conditions of droplet formation can be treated completely free of empirical information or correlations; there are, however, some conditions of droplet activation for which an empirically derived correlation is utilized. Predictions of the parameterization are compared against extensive cloud parcel model simu;lations for a variety of aerosol activation conditions that cover a wide range of chemical variability and CCN concentrations. The parameterization tracks the parcel model simulations closely and robustly. The parameterization presented here is intended to allow for a comprehensive assessment of the aerosol indirect effect in general circulation models.

Nenes, A.↗

62°S Witnesses the Transition of Boundary Layer Marine Aerosol Pattern Over the Southern Ocean (50°S–68°S, 63°E– 150°E) During the Spring and Summer: Results From MARCUS (I)

The Atmospheric Radiation Measurement Mobile Facility-2 was installed onboard the research vessel Aurora Australis to measure aerosol properties during the 2017-2018 Measurement of Aerosols, Radiation, and CloUds over the pristine Southern ocean (MARCUS) Experiment, providing unique data on aerosols latitudinal and seasonal variation, including south of 60 degrees S where previous observations are scarce. Data from a Cloud Condensation Nuclei (CCN) counter and Ultra-High-Sensitivity Aerosol Spectrometer show that both the number concentration (N-CCN) and size distribution of CCN-active aerosols, with diameters (D) between 60 nm < D < 1,000 nm are different over the North Southern Ocean (NSO) (50 degrees S-60 degrees S) and the South Southern Ocean (SSO) (62 degrees S-68 degrees S). The average NSO N-CCN at 0.2% and 0.5% supersaturation were 28% and 49% less than that over the SSO. This increase of CCN over the SSO is caused by the increase of aerosols with 60 nm < D < 200 nm, consistent with calculations of Aerosol Scattering Angstrom Exponents derived from a nephelometer. Aerosol hygroscopicity growth factor measured by the Hygroscopic Tandem Differential Mobility Analyzer stayed close to 1.41 for aerosols with 50 nm < D < 250 nm over the SSO, but increased from 1.30 to 1.67 over the NSO, indicating different chemical compositions. Both CCN and Ice Nucleating Particles (INPs) showed a stronger variation with season than with latitude. The variation of heat-labile and presumably proteinacous INPs suggests an increase of ice nucleating-active microbes in summer.

Niu, Qing↗

An Improved Representation of Aerosol Wet Removal by Deep Convection and Impacts on Simulated Aerosol Vertical Profiles

Here, we introduce a physics-based aerosol wet removal scheme with unified treatments of aerosol transport and removal by convective clouds into the Community Atmosphere Model version 6. Since several important physical processes are still neglected or poorly represented in this new physics-based scheme, we develop secondary improvements to the parameterizations of aerosol activation, resuspension, and cloud-borne aerosol detrainment in this new scheme. Changes in the aerosol wet removal scheme cause tropospheric aerosol concentrations to decrease to different extents: compared to the control run, the physics-based scheme significantly decreases aerosol burdens by up to 60% over the southern Pacific Ocean, whereas the secondary improvements mitigate the decreasing tendency. The burden changes also depend on aerosol chemical components: the sulfate mass decrease is compensated by secondary production, black carbon (BC) is effectively removed via increasing the hygroscopicity of particulate organic matter from 0 to 0.2, and dust shows the most spatially heterogeneous changes. Simulated aerosol profiles are evaluated against aircraft-based observations over the Pacific and Atlantic Oceans. The secondary-improved scheme reduces the overestimations of upper tropospheric BC and sea salt concentrations by a factor of 10 and 1,000, respectively, and reproduces the dependence of BC mass decrease rates on cloud types. Consideration of convective cloud-borne aerosol detrainment plays the most important role in enhancing the aerosol wet removal and decreasing the positive biases of tropospheric BC and sea salt concentrations. We also summarize unresolved issues related to convective cloud genesis and microphysics, cloud-borne aerosol evolution, and BC and dust emissions.

54 ENVIRONMENTAL SCIENCES↗

Evaluation of a New Cloud Droplet Activation Parameterization wtih in Situ Data from CRYSTAL-FACE and CSTRIPE

The accuracy of the 2003 prognostic, physically based aerosol activation parameterization of A. Nenes and J. H. Seinfeld (NS) with modification introduced by C. Fountoukis and A. Nenes in 2005 (modified NS) is evaluated against extensive microphysical data sets collected on board the Center for Interdisciplinary Remotely Piloted Aircraft Studies (CIRPAS) Twin Otter aircraft for cumuliform and stratiform clouds of marine and continental origin. The cumuliform cloud data were collected during NASA's Cirrus Regional Study of Tropical Anvils and Cirrus Layers-Florida Area Cirrus Experiment (CRYSTAL-FACE, Key West, Florida, July 2002), while the stratiform cloud data were gathered during Coastal Stratocumulus Imposed Perturbation Experiment (CSTRIPE, Monterey, California, July 2003). In situ data sets of aerosol size distribution, chemical composition, and updraft velocities are used as input for the NS parameterization, and the evaluation is carried out by comparing predicted cloud droplet number concentrations (CDNC) with observations. This is the first known study in which a prognostic cloud droplet activation parameterization has been evaluated against a wide range of observations. On average, predicted droplet concentration in adiabatic regions is within -20% of observations at the base of cumuliform clouds and -30% of observations at different altitudes throughout the stratiform clouds, all within experimental uncertainty. Furthermore, CDNC is well parameterized using either a single mean updraft velocity w or by weighting droplet nucleation rates with a Gaussian probability density function of w. This study suggests that for nonprecipitating warm clouds of variable microphysics, aerosol composition, and size distribution the modified NS parameterization can accurately predict cloud droplet activation and can be successfully implemented for describing the aerosol activation process in global climate models.

Meskhidze, Nicholas↗

Process Modeling of Aerosol‐Cloud Interaction in Summertime Precipitating Shallow Cumulus Over the Western North Atlantic

Abstract Process modeling of Aerosol‐cloud interaction (ACI) is essential to bridging gaps between observational analysis and climate modeling of aerosol effects in the Earth system and eventually reducing climate projection uncertainties. In this study, we examine ACI in summertime precipitating shallow cumuli observed during the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). Aerosols and precipitating shallow cumuli were extensively observed with in‐situ and remote‐sensing instruments during two research flight cases on 02 June and 07 June, respectively, during the ACTIVATE summer 2021 deployment phase. We perform observational analysis and large‐eddy simulation (LES) of aerosol effect on precipitating cumulus in these two cases. Given the measured aerosol size distributions and meteorological conditions, LES is able to reproduce the observed cloud properties by aircraft such as liquid water content (LWC), cloud droplet number concentration ( N c ) and effective radius r eff . However, it produces smaller liquid water path (LWP) and larger N c compared to the satellite retrievals. Both 02 and 07 June cases are over warm waters of the Gulf Stream and have a cloud top height over 3 km, but the 07 June case is more polluted and has larger LWC. We find that the N a ‐induced LWP adjustment is dominated by precipitation feedback for the 2 June precipitating case and there is no clear entrainment feedback in both cases. An increase of cloud fraction due to a decrease of aerosol number concentration is also shown in the simulations for the 02 June case.

54 ENVIRONMENTAL SCIENCES↗

On the Ability of Space- Based Passive and Active Remote Sensing Observations of CO2 to Detect Flux Perturbations to the Carbon Cycle

Space-borne observations of CO2 are vital to gaining understanding of the carbon cycle in regions of the world that are difficult to measure directly, such as the tropical terrestrial biosphere, the high northern and southern latitudes, and in developing nations such as China. Measurements from passive instruments such as GOSAT (Greenhouse Gases Observing Satellite) and OCO-2 (Orbiting Carbon Observatory 2), however, are constrained by solar zenith angle limitations as well as sensitivity to the presence of clouds and aerosols. Active measurements such as those in development for the Active Sensing of CO2 Emissions over Nights, Days and Seasons (ASCENDS) mission show strong potential for making measurements in the high-latitude winter and in cloudy regions. In this work we examine the enhanced flux constraint provided by the improved coverage from an active measurement such as ASCENDS. The simulation studies presented here show that with sufficient precision, ASCENDS will detect permafrost thaw and fossil fuel emissions shifts at annual and seasonal time scales, even in the presence of transport errors, representativeness errors, and biogenic flux errors. While OCO-2 can detect some of these perturbations at the annual scale, the seasonal sampling provided by ASCENDS provides the stronger constraint. Plain Language Summary: Active and passive remote sensors show the potential to provide unprecedented information on the carbon cycle. With the all-season sampling, active remote sensors are more capable of constraining high-latitude emissions. The reduced sensitivity to cloud and aerosol also makes active sensors more capable of providing information in cloudy and polluted scenes with sufficient accuracy. These experiments account for errors that are fundamental to the top-down approach for constraining emissions, and even including these sources of error, we show that satellite remote sensors are critical for understanding the carbon cycle.

tropical terrestrial biosphere↗

A Concept of a Convection–Cloud Chamber to Study Aerosol–Cloud–Drizzle Interactions

Understanding and quantifying the full chain of processes from aerosol activation to drizzle formation, and the associated feedbacks to the aerosol chemical and physical properties, all within a turbulent cloud are some of the toughest challenges in atmospheric chemistry and physics and are keys to the cloud–precipitation puzzle. This paper describes a concept for a new type of research facility consisting of a cloud chamber plus associated instrumentation and computational models, to explore aerosol–cloud interactions and processing, cloud optical properties, entrainment–cloud interactions, and quantitative assessment of drizzle onset. The envisioned design is for a 3 m × 3 m × 9 m chamber, such that the height is sufficient to achieve long lifetimes for aerosol processing and for significant drizzle growth by collision and coalescence. A suite of computational tools for simulating microphysical properties in the chamber provides a digital twin for designing the chamber and a range of example experiments. Theory and test results from novel remote sensing systems for exploring chemical and physical interactions and evolution of aerosols, cloud droplets, and drizzle within turbulent clouds are described. Testing of technology needed for the operation of a large-volume chamber, including aerosol generation methods and novel materials for water vapor boundary conditions, is described. Simulations suggest that spatially uniform turbulence and microphysical properties can be sustained in a steady state, with reasonable aerosol and water vapor fluxes, and that substantial drizzle can be produced through collision and coalescence of cloud droplets. Remaining challenges for more detailed engineering design and a discussion of possible first-light experiments are described.

54 ENVIRONMENTAL SCIENCES↗

Aerosol-Cloud Interactions during Tropical Deep Convection: Evidence for the Importance of Free Tropospheric Aerosols

NASA's 2002 CRYSTAL-FACE field experiment focused on the formation and evolution of tropical cirrus cloud systems in southern Florida. Multiple aircraft extensively sampled cumulonimbus dynamical and microphysical properties, as well as characterizing ambient aerosol populations both inside and outside the full depth of the convective column. On July 18, unique measurements were taken when a powerful updraft was traversed directly by aircraft, providing a window into the primary source region of cumulonimbus anvil crystals. Observations of the updraft, entered at approximately l0 km altitude and -34 C, indicated more than 200 cloud particles per mL at vertical velocities exceeding 20 m/s and the presence of significant condensation nuclei and liquid water within the core. In this work, aerosol and cloud phase observations are integrated by simulating the updraft conditions using a large-eddy resolving model with 3 explicit multiphase microphysics, including treatment of size-resolved aerosol fields, aerosol activation and freezing, and evaporation of cloud particles back to the aerosol phase. Simulations were initialized with observed thermodynamic and aerosol size distributions profiles and convection was driven by surface fluxes assimilated from the ARPS forecast model. Model results are consistent with the conclusions that most crystals are homogeneously frozen droplets and that entrained free tropospheric aerosols may contribute a significant fraction of the crystals. Thus most anvil crystals appear to be formed aloft in updraft cores, well above cloud base. These conclusions are supported by observations of hydrometeor size distribution made while traversing the dore, as well as aerosol and cloud particle size distributions generally observed by aircraft below 4km and crystal properties generally observed by aircraft above 12km.

Ackerman, A.↗

On the relationship between eastern China aerosols and western North Pacific tropical cyclone activity

How aerosols affect the weather and climate system has received increasing attention. This study finds a significant negative correlation between March–May eastern China aerosol optical depth (AOD) and July–November western North Pacific (WNP) tropical cyclone (TC) frequency during 2003–2020. This time period spans when several aerosol reanalyses are available and both Terra and Aqua Moderate Resolution Imaging Spectroradiometer AOD retrievals are assimilated therein. Composite analyses and budget analyses of dynamical genesis potential indices indicate the importance of large-scale environmental factors, especially vertical velocity and vertical wind shear, associated with changes in AOD that in turn modulate changes in WNP TC frequency. Increased eastern China AOD may facilitate negative Pacific meridional mode development via modulation of the westerly jet, which then forces an anticyclonic circulation over the WNP basin. Increased AOD can also directly decrease the inter-hemispheric temperature differential and increases the intra-hemispheric temperature differential between the equator and the mid-latitudes, thus weakening ascending motion and enhancing vertical wind shear over the WNP, especially the southeastern portion of the basin. Further, all of these large-scale environment changes induced by increased eastern China AOD tend to suppress WNP TCs. This study highlights the potential influence of eastern China aerosol loadings on WNP TCs, thus improving our understanding of TC climate variability over the WNP.

54 ENVIRONMENTAL SCIENCES↗

Using High-Resolution Airborne Remote Sensing to Study Aerosol Near Clouds

The horizontal space in between clear and cloudy air is very complex. This so-called twilight zone includes activated aerosols that are not quite clouds, thin cloud fragments that are not easily observable, and dying clouds that have not quite disappeared. This is a huge challenge for satellite remote sensing, specifically for retrieval of aerosol properties. Identifying what is cloud versus what is not cloud is critically important for attributing radiative effects and forcings to aerosols. At the same time, the radiative interactions between clouds and the surrounding media (molecules, surface and aerosols themselves) will contaminate retrieval of aerosol properties, even in clear skies. Most studies on aerosol cloud interactions are relevant to moderate resolution imagery (e.g. 500 m) from sensors such as MODIS. Since standard aerosol retrieval algorithms tend to keep a distance (e.g. 1 km) from the nearest detected cloud, it is impossible to evaluate what happens closer to the cloud. During Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), the NASA ER-2 flew with the enhanced MODIS Airborne Simulator (eMAS), providing MODIS-like spectral observations at high (50 m) spatial resolution. We have applied MODIS-like aerosol retrieval for the eMAS data, providing new detail to characterization of aerosol near clouds. Interpretation and evaluation of these eMAS aerosol retrievals is aided by independent MODIS-like cloud retrievals, as well as profiles from the co-flying Cloud Physics Lidar (CPL). Understanding aerosolcloud retrieval at high resolution will lead to better characterization and interpretation of long-term, global products from lower resolution (e.g.MODIS) satellite retrievals.

aerosols near clouds↗

Evaluation of liquid cloud albedo susceptibility in E3SM using coupled eastern North Atlantic surface and satellite retrievals

The impact of aerosol number concentration on cloud albedo is a persistent source of spread in global climate predictions due to multi-scale, interactive atmospheric processes that remain difficult to quantify. We use 5 years of geostationary satellite and surface retrievals at the US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) eastern North Atlantic (ENA) site in the Azores to evaluate the representation of liquid cloud albedo susceptibility for overcast cloud scenes in the DOE Energy Exascale Earth System Model version 1 (E3SMv1) and provide possible reasons for model–observation discrepancies. The overall distribution of surface 0.2 % CCN concentration values is reasonably simulated, but simulated liquid water path (LWP) is lower than observed and layer mean droplet concentration (N d ) comparisons are highly variable depending on the N d retrieval technique. E3SMv1's cloud albedo is greater than observed for given LWP and N d values due to a lower cloud effective radius than observed. However, the simulated albedo response to N d is suppressed due to a correlation between the solar zenith angle (SZA) and N d created by the seasonal cycle that is not observed. Controlling for this effect by examining the cloud optical depth (COD) shows that E3SMv1's COD response to CCN concentration is greater than observed. For surface-based retrievals, this is only true after controlling for cloud adiabaticity because E3SMv1's adiabaticities are much lower than observed. Assuming a constant adiabaticity in surface retrievals as done in top-of-atmosphere (TOA) retrievals narrows the retrieved ln N d distribution, which increases the cloud albedo sensitivity to ln N d to match the TOA sensitivity. The greater sensitivity of COD to CCN is caused by a greater Twomey effect in which the sensitivity of N d to CCN is greater than observed for TOA-retrieved N d , and once model–observation cloud adiabaticity differences are removed, this is also true for surface-retrieved N d . The LWP response to N d in E3SMv1 is overall negative as observed. Despite reproducing the observed LWP–N d relationship, observed clouds become much more adiabatic as N d increases, while E3SMv1 clouds do not, associated with more heavily precipitating clouds that are partially but not completely caused by deeper clouds and weaker inversions in E3SMv1. These cloud property differences indicate that the negative LWP–N d relationship is likely not caused by the same mechanisms in E3SMv1 and observations. The negative simulated LWP response also fails to mute the excessively strong Twomey effect, highlighting potentially important confounding factor effects that likely render the LWP–N d relationship non-causal. N d retrieval scales and assumptions, particularly related to cloud adiabaticity, contribute to substantial spreads in the model–observation comparisons, though enough consistency exists to suggest that aerosol activation, drizzle, and entrainment processes are critical areas to focus E3SMv1 development for improving the fidelity of aerosol–cloud interactions in E3SM.

54 ENVIRONMENTAL SCIENCES↗

Aerosol‐Correlated Cloud Activation for Clean Conditions in the Tropical Atlantic Boundary Layer During LASIC

Abstract Aerosol measurements during the DOE ARM Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign were used to quantify the differences between clean and smoky cloud condensation nuclei (CCN) budgets. Accumulation‐mode particles accounted for ∼70% of CCN at supersaturations <0.3% in clean and smoky conditions. Aitken‐mode particles contributed <20% and sea‐spray‐mode particles <10% at supersaturations <0.3%, but at supersaturations >0.3% Aitken particles contributions increased to 30%–40% of clean CCN. For clean conditions, the Hoppel minimum diameter was correlated to the accumulation‐mode number concentration, indicating aerosol‐correlated cloud activation was controlling the lower diameter cutoff for which particles serve as CCN. For smoky conditions, the contributions of Aitken particles increase and the correlation of cloud activation to accumulation‐mode particles is masked by the lower‐hygroscopicity smoke. These results provide the first multi‐month in situ quantitative constraints on the role of aerosol number size distributions in controlling cloud activation in the tropical Atlantic boundary layer.

54 ENVIRONMENTAL SCIENCES↗

Retrieving the complex refractive index of atmospheric aerosols from ratios of solar spectral extinction measurements

The technique proposed by Fymat (1976) for retrieving the complex refractive index of atmospheric aerosols using narrowband spectral transmission ratios, taken within an overall narrow spectral interval, is investigated in the case of modelled polydispersions of rural, maritime-continental, maritime-sea spray and meteoric dust aerosols. It is confirmed that for not too broad size distributions most of the information comes from a narrow size range of 'active' aerosols so that, under these circumstances, the refractive index components can indeed be retrieved essentially independently of the size distribution. For 0.1% accurate data in three colors, the technique can provide the real and imaginary components of the index respectively within 0.07% and 0.3% accuracy.

Fymat, A. L.↗

On the Feasibility of Studying Shortwave Aerosol Radiative Forcing of Climate Using Dual-Wavelength Aerosol Backscatter Lidar

The current low confidence in the estimates of aerosol-induced perturbations of Earth's radiation balance is caused by the highly non-uniform compositional, spatial and temporal distributions of tropospheric aerosols on a global scale owing to their heterogeneous sources and short lifetimes. Nevertheless, recent studies have shown that the inclusion of aerosol effects in climate model calculations can improve agreement with observed spatial and temporal temperature distributions. In light of the short lifetimes of aerosols, determination of their global distribution with space-borne sensors seems to be a necessary approach. Until recently, satellite measurements of tropospheric aerosols have been approximate and did not provide the full set of information required to determine their radiative effects. With the advent of active aerosol remote sensing from space (e.g., PICASSO-CENA), the applicability fo lidar-derived aerosol 180 deg -backscatter data to radiative flux calculations and hence studies of aerosol effects on climate needs to be investigated.

Redemann, Jens↗

Wintertime synoptic patterns of midlatitude boundary layer clouds over the western North Atlantic: Climatology and insights from in-situ ACTIVATE observations

The winter synoptic evolution of the western North Atlantic and its influence on the atmospheric boundary layer is described by means of a regime classification based on Self Organizing Maps applied to 12 year of data (2009-2020). The regimes are classified into categories according to daily 600-hPa geopotential height: dominant ridge, trough to ridge eastward transition (trough-ridge), dominant trough, and ridge to trough eastward transition (ridge-trough). A fifth synoptic regime resembles the winter climatological mean. Coherent changes in sea-level pressure and large-scale winds are in concert with the synoptic regimes: 1) the ridge regime is associated with a well-developed anticyclone; 2) the trough-ridge gives rise to a low pressure center over the ocean, ascents, and northerly winds over the coastal zone; 3) trough is associated with the eastward displacement of a cyclone, coastal subsidence, and northerly winds, all representative characteristics of cold-air outbreaks; 4) the ridge-trough regime features the development of an anticyclone and weak coastal winds. Low clouds are characteristic of the trough regime, with both trough and trough-ridge featuring synoptic maxima in cloud droplet number concentration (N d ). The N d increase is primarily observed near the coast, concomitant with strong surface heat fluxes exceeding by more than 400 W m -2 compared to fluxes further east. Five consecutive days of aircraft observations collected during the ACTIVATE campaign corroborates the climatological characterization, confirming the occurrence of high N d for days identified as trough. This study emphasizes the role of boundary-layer dynamics and aerosol activation and their roles in modulating cloud microphysics.

54 ENVIRONMENTAL SCIENCES↗