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At least 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Assessment of long-term WRF–CMAQ simulations for understanding direct aerosol effects on radiation "brightening" in the United States

Long-term simulations with the coupled WRF–CMAQ (Weather Research and Forecasting–Community Multi-scale Air Quality) model have been conducted to systematically investigate the changes in anthropogenic emissions of SO 2 and NO x over the past 16 years (1995–2010) across the United States (US), their impacts on anthropogenic aerosol loading over North America, and subsequent impacts on regional radiation budgets. In particular, this study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO 2 and NO x associated with control measures under the Clean Air Act (CAA) especially on trends in solar radiation. Extensive analyses conducted by Gan et al. (2014a) utilizing observations (e.g., SURFRAD, CASTNET, IMPROVE, and ARM) over the past 16 years (1995–2010) indicate a shortwave (SW) radiation (both all-sky and clear-sky) "brightening" in the US. The relationship of the radiation brightening trend with decreases in the aerosol burden is less apparent in the western US. One of the main reasons for this is that the emission controls under the CAA were aimed primarily at reducing pollutants in areas violating national air quality standards, most of which were located in the eastern US, while the relatively less populated areas in the western US were less polluted at the beginning of this study period. Comparisons of model results with observations of aerosol optical depth (AOD), aerosol concentration, and radiation demonstrate that the coupled WRF–CMAQ model is capable of replicating the trends well even though it tends to underestimate the AOD. In particular, the sulfate concentration predictions were well matched with the observations. The discrepancies found in the clear-sky diffuse SW radiation are likely due to several factors such as the potential increase of ice particles associated with increasing air traffic, the definition of "clear-sky" in the radiation retrieval methodology, and aerosol semi-direct and/or indirect effects which cannot be readily isolated from the observed data.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Investigation of short-term effective radiative forcing of fire aerosols over North America using nudged hindcast ensembles

Aerosols from fire emissions can potentially have large impact on clouds and radiation. However, fire aerosol sources are often intermittent, and their effect on weather and climate is difficult to quantify. Here we investigated the short-term effective radiative forcing of fire aerosols using the global aerosol–climate model Community Atmosphere Model version 5 (CAM5). Different from previous studies, we used nudged hindcast ensembles to quantify the forcing uncertainty due to the chaotic response to small perturbations in the atmosphere state. Daily mean emissions from three fire inventories were used to consider the uncertainty in emission strength and injection heights. The simulated aerosol optical depth (AOD) and mass concentrations were evaluated against in situ measurements and reanalysis data. Overall, the results show the model has reasonably good predicting skills. Short (10-day) nudged ensemble simulations were then performed with and without fire emissions to estimate the effective radiative forcing. Results show fire aerosols have large effects on both liquid and ice clouds over the two selected regions in April 2009. Ensemble mean results show strong negative shortwave cloud radiative effect (SCRE) over almost the entirety of southern Mexico, with a 10-day regional mean value of −3.0 W m −2 . Over the central US, the SCRE is positive in the north but negative in the south, and the regional mean SCRE is small (−0.56 W m −2 ). For the 10-day average, we found a large ensemble spread of regional mean shortwave cloud radiative effect over southern Mexico (15.6 % of the corresponding ensemble mean) and the central US (64.3 %), despite the regional mean AOD time series being almost indistinguishable during the 10-day period. Moreover, the ensemble spread is much larger when using daily averages instead of 10-day averages. This demonstrates the importance of using a large ensemble of simulations to estimate the short-term aerosol effective radiative forcing.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Simulation of the transport, vertical distribution, optical properties and radiative impact of smoke aerosols with the ALADIN regional climate model during the ORACLES-2016 and LASIC experiments

Estimates of the direct radiative effect (DRE) from absorbing smoke aerosols over the southeast Atlantic Ocean (SAO) require simulation of the microphysical and optical properties of stratocumulus clouds as well as of the altitude and shortwave (SW) optical properties of biomass burning aerosols (BBAs). In this study, we take advantage of the large number of observations acquired during the ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES-2016) and Layered Atlantic Smoke Interactions with Clouds (LASIC) projects during September 2016 and compare them with datasets from the ALADIN-Climate (Aire Limitée Adaptation dynamique Développement InterNational) regional model. The model provides a good representation of the liquid water path but the low cloud fraction is underestimated compared to satellite data. The modeled total-column smoke aerosol optical depth (AOD) and above-cloud AOD are consistent ( ~0.7 over continental sources and ~0.3 over the SAO at 550 nm) with the Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2), Ozone Monitoring Instrument (OMI) or Moderate Resolution Imaging Spectroradiometer (MODIS) data. The simulations indicate smoke transport over the SAO occurs mainly between 2 and 4 km, consistent with surface and aircraft lidar observations. The BBA single scattering albedo is slightly overestimated compared to the Aerosol Robotic Network (AERONET) and more significantly when compared to Ascension Island surface observations. The difference could be due to the absence of internal mixing treatment in the ALADIN-Climate model. The SSA overestimate leads to an underestimation of the simulated SW radiative heating compared to ORACLES data. ALADIN-Climate simulates a positive (monthly mean) SW DRE of about +6 W m -2 over the SAO (20 ° S–10 ° N and 10 ° W–20 ° E) at the top of the atmosphere and in all-sky conditions. Over the continent, the presence of BBA is shown to significantly decrease the net surface SW flux, through direct and semi-direct effects, which is compensated by a decrease (monthly mean) in sensible heat fluxes ( -25 W m -2 ) and surface land temperature ( -1.5 ° C) over Angola, Zambia and the Democratic Republic of the Congo, notably. The surface cooling and the lower tropospheric heating decrease the continental planetary boundary layer height by about ~200 m.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Intercomparison of biomass burning aerosol optical properties from in situ and remote-sensing instruments in ORACLES-2016

The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60%. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD 400 > 0.4 ).The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 > nm (SSA 500 ) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Direct and semi-direct radiative forcing of biomass-burning aerosols over the southeast Atlantic (SEA) and its sensitivity to absorbing properties: a regional climate modeling study

Simulations are performed for the period 2000-2015 by two different regional climate models, ALADIN and RegCM, to quantify the direct and semi-direct radiative effects of biomass-burning aerosols (BBAs) in the southeast Atlantic (SEA) region. Different simulations have been performed using strongly absorbing BBAs in accordance with recent in situ observations over the SEA. For the July-August-September (JAS) season, the single scattering albedo (SSA) and total aerosol optical depth (AOD) simulated by the ALADIN and RegCM models are consistent with the MACv2 climatology and MERRA-2 and CAMS-RA reanalyses near the biomass-burning emission sources. However, the above-cloud AOD is slightly underestimated compared to satellite (MODIS and POLDER) data during the transport over the SEA. The direct radiative effect exerted at the continental and oceanic surfaces by BBAs is significant in both models and the radiative effects at the top of the atmosphere indicate a remarkable regional contrast over SEA (in all-sky conditions), with a cooling (warming) north (south) of 10°S, which is in agreement with the recent MACv2 climatology. In addition, the two models indicate that BBAs are responsible for an important shortwave radiative heating of ~0.5-1K per day over SEA during JAS with maxima between 2 and 4 km a.m.s.l. (above mean sea level). At these altitudes, BBAs increase air temperature by ~0.2-0.5 K, with the highest values being co-located with low stratocumulus clouds. Vertical changes in air temperature limit the subsidence of air mass over SEA, creating a cyclonic anomaly. The opposite effect is simulated over the continent due to the increase in lower troposphere stability. The BBA semi-direct effect on the lower troposphere circulation is found to be consistent between the two models. Changes in the cloud fraction are moderate in response to the presence of smoke, and the models differ over the Gulf of Guinea. Finally, the results indicate an important sensitivity of the direct and semi-direct effects to the absorbing properties of BBAs. Over the stratocumulus (Sc) region, DRE varies from +0.94 W m -2 (scattering BBAs) to +3.93 W m -2 (most absorbing BBAs).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Impact of biomass burning aerosols on radiation, clouds, and precipitation over the Amazon: relative importance of aerosol–cloud and aerosol–radiation interactions

Biomass burning (BB) aerosols can influence regional and global climate through interactions with radiation, clouds, and precipitation. Here, we investigate the impact of BB aerosols on the energy balance and hydrological cycle over the Amazon Basin during the dry season. We performed simulations with a fully coupled meteorology–chemistry model, the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), for a range of different BB emission scenarios to explore and characterize nonlinear effects and individual contributions from aerosol–radiation interactions (ARIs) and aerosol–cloud interactions (ACIs). The ARIs of BB aerosols tend to suppress low-level liquid clouds by local warming and increased evaporation and to facilitate the formation of high-level ice clouds by enhancing updrafts and condensation at high altitudes. In contrast, the ACIs of BB aerosol particles tend to enhance the formation and lifetime of low-level liquid clouds by providing more cloud condensation nuclei (CCN) and to suppress the formation of high-level ice clouds by reducing updrafts and condensable water vapor at high altitudes (>8 km). For scenarios representing the lower and upper limits of BB emission estimates for recent years (2002–2016), we obtained total regional BB aerosol radiative forcings of –0.2 and 1.5 W m –2 , respectively, showing that the influence of BB aerosols on the regional energy balance can range from modest cooling to strong warming. We find that ACIs dominate at low BB emission rates and low aerosol optical depth (AOD), leading to an increased cloud liquid water path (LWP) and negative radiative forcing, whereas ARIs dominate at high BB emission rates and high AOD, leading to a reduction of LWP and positive radiative forcing. In all scenarios, BB aerosols led to a decrease in the frequency of occurrence and rate of precipitation, caused primarily by ACI effects at low aerosol loading and by ARI effects at high aerosol loading. The dependence of precipitation reduction on BB aerosol loading is greater in a strong convective regime than under weakly convective conditions. Overall, our results show that ACIs tend to saturate at high aerosol loading, whereas the strength of ARIs continues to increase and plays a more important role in highly polluted episodes and regions. This should hold not only for BB aerosols over the Amazon, but also for other light-absorbing aerosols such as fossil fuel combustion aerosols in industrialized and densely populated areas. The importance of ARIs at high aerosol loading highlights the need for accurately characterizing aerosol optical properties in the investigation of aerosol effects on clouds, precipitation, and climate.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM 2.5 , often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m 2 g –1 observed average) and light-scattering enhancement factor (ƒ(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm –3 in the model vs. observed average of 1.5 g cm –3 ) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 1: Experimental protocols and surface changes

There is now substantial literature on climate model studies of equatorial or tropical stratospheric SO 2 injections that aim to counteract the surface warming produced by rising concentrations of greenhouse gases. Here we present the results from the first systematic intercomparison of climate responses in three Earth system models wherein the injection of SO 2 occurs at different latitudes in the lower stratosphere: CESM2-WACCM6, UKESM1.0 and GISS-E2.1-G. The first two use a modal aerosol microphysics scheme, while two versions of GISS-E2.1-G use a bulk aerosol (One-Moment Aerosol, OMA) and a two-moment (Multiconfiguration Aerosol TRacker of mIXing state, MATRIX) microphysics approach, respectively. Our aim in this work is to determine commonalities and differences between the climate model responses in terms of the distribution of the optically reflective sulfate aerosols produced from the oxidation of SO 2 and in terms of the surface response to the resulting reduction in solar radiation. A focus on understanding the contribution of characteristics of models transport alongside their microphysical and chemical schemes, and on evaluating the resulting stratospheric responses in different models, is given in the companion paper (Bednarz et al., 2023). The goal of this exercise is not to evaluate these single-point injection simulations as stand-alone proposed strategies to counteract global warming; instead we determine sources and areas of agreement and uncertainty in the simulated responses and, ultimately, the possibility of designing a comprehensive intervention strategy capable of managing multiple simultaneous climate goals through the combination of different injection locations. We find large disagreements between GISS-E2.1-G and the CESM2-WACCM6 and UKESM1.0 models regarding the magnitude of cooling per unit of aerosol optical depth (AOD) produced, which varies from 4.7 K per unit of AOD in CESM2-WACCM6 to 16.7 K in the GISS-E2.1-G version with two-moment aerosol microphysics. By normalizing the results with the global mean response in each of the models and thus assuming that the amount of SO 2 injected is a free parameter that can be managed independently, we highlight some commonalities in the overall distributions of the aerosols, in the inter-hemispheric surface temperature response and in shifts to the Intertropical Convergence Zone, as well as some areas of disagreement, such as the extent of the aerosol confinement in the equatorial region and the efficiency of the transport to polar latitudes. In conclusion, we demonstrate that it is possible to use these simulations to produce more comprehensive injection strategies in multiple climate models. However, large differences in the injection magnitudes can be expected, potentially increasing inter-model spreads in some stratospheric quantities (such as aerosol distribution) while reducing the spread in the surface response in terms of temperature and precipitation; furthermore, the selection of the injection locations may be dependent on the models' specific stratospheric transport.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Influence of covariance of aerosol and meteorology on co-located precipitating and non-precipitating clouds over the Indo-Gangetic Plain

Aerosol–cloud–precipitation interaction (ACPI) plays a pivotal role in the global and regional water cycle and the earth's energy budget; however, it remains highly uncertain due to the different underlying physical mechanisms. Therefore, this study aims to systematically analyze the effects of aerosols and meteorological factors on ACPI in the co-located precipitating clouds (PCs) and non-precipitating clouds (NPCs) in winter and summer seasons by employing the long-term (2001–2021) retrievals from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Tropical Rainfall Measuring Mission (TRMM) coupled with the National Center for Environmental Prediction/National Center for Atmospheric Research (NCEP/NCAR) reanalysis-II datasets over the Indo-Gangetic Plain (IGP). The results exhibit a decadal increase in aerosol optical depth (AOD) over Lahore (5.2 %), Delhi (9 %), Kanpur (10.7 %), and Gandhi College (22.7 %) and a decrease over Karachi (-1.9 %) and Jaipur (-0.5 %). The most stable meteorology with high values of lower-tropospheric stability (LTS) is found in both seasons over Karachi. In the summer season, the occurrence frequency of clouds is high (74 %) over Gandhi College, 60 % of which are PCs. Conversely, the lowest number of PCs is found over Karachi. Similarly, in the winter season, the frequency of cloud occurrence is low over Karachi and high over Lahore and Gandhi College. The analysis of cloud top pressure (CTP) and cloud optical thickness (COT) indicates high values of cloud fraction (CF) for thick and high-level clouds over all study areas except Karachi. The microphysical properties such as cloud effective radius (CER) and cloud droplet number concentration (CDNC) bear high values (CER ≳ 15 µm and CDNC ≳ 50 cm -3 ) for both NPCs and PCs in summer. The AOD–CER correlation is good (weak) for PCs (NPCs) in winter. Similarly, the sensitivity value of the first indirect effect (FIE) is high (ranging from 0.2 ± 0.13 to 0.3 ± 0.01 in winter and from 0.19 ± 0.03 to 0.32 ± 0.05 in summer) for PCs and low for NPCs. The sensitivity value for the second indirect effect (SIE) is relatively higher (such as 0.6 ± 0.14 in winter and 0.4 ± 0.04 in summer) than FIE. Sensitivity values of the aerosol-cloud interaction (ACI) are low (i.e., -0.06 ± 0.09) for PCs in summer. Furthermore, the precipitation rate (PR) exhibits high values in the summer season, primarily due to the significant contribution from optically thick clouds with lower CDNC (≲ 50 cm -3 ) and larger CER and the intermediate contribution from optically thick clouds with higher CDNC ( ≳ 50 cm -3 ).

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Quantifying the impacts of marine aerosols over the southeast Atlantic Ocean using a chemical transport model: implications for aerosol–cloud interactions

The southeast Atlantic region, characterized by persistent stratocumulus clouds, has one of the highest uncertainties in aerosol radiative forcing and significant variability across climate models. In this study, we analyze the seasonally varying role of marine aerosol sources and identify key uncertainties in aerosol composition at cloud-relevant altitudes over the southeast Atlantic using the GEOS-Chem chemical transport model. We evaluate simulated aerosol optical depth (AOD) and speciated aerosol concentrations against those collected from ground observations and aircraft campaigns such as LASIC, ORACLES, and CLARIFY, conducted during 2017. The model consistently underestimates AOD relative to AERONET, particularly at remote locations like Ascension Island. However, when compared with aerosol mass concentrations from aircraft campaigns during the biomass burning period, it performs adequately at cloud-relevant altitudes, with a normalized mean bias (NMB) between -3.5 % (CLARIFY) and -7.5 % (ORACLES). At these altitudes, in the model, organic aerosols (63 %) dominate during the biomass burning period, while sulfate (41 %) prevails during austral summer, when dimethylsulfide (DMS) emissions peak in the model. Our findings indicate that marine sulfate can account for up to 69 % of total sulfate during the high-DMS period. Sensitivity analyses indicate that refining DMS emissions and oxidation chemistry may increase sulfate aerosol produced from marine sources, highlighting that there remains large uncertainty as to the role of DMS emissions in the marine boundary layer. Additionally, we find marine primary organic aerosol emissions may substantially increase total organic aerosol concentrations, particularly during austral summer. This study underscores the imperative need to refine marine emissions and their chemical transformations, as aerosols from marine sources are a major component of total aerosols at cloud-relevant altitudes and may impact uncertainties in aerosol radiative forcing over the southeast Atlantic.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

Size-resolved process understanding of stratospheric sulfate aerosol following the Pinatubo eruption

Stratospheric sulfate aerosol produced by volcanic eruptions plays important roles in atmospheric chemistry and the global radiative balance of the atmosphere. The simulation of stratospheric sulfate concentrations and optical properties is highly dependent on the chemistry scheme and microphysical treatment. In this work, we implemented a sophisticated gas-phase chemistry scheme (full chemistry, FC) and a 5-mode version of the Modal Aerosol Module with Prognostic Stratospheric Aerosol (MAM5-PSA) for the interactive treatment of stratospheric sulfate aerosol in the Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2) model to better simulate the chemistry-aerosol feedback following the Pinatubo eruption, and to compare it against a simulation using simplified chemistry (SC) and the default 4-mode version of the Modal Aerosol Module (MAM4). MAM5-PSA experiments were found to better capture the stratospheric sulfate burden from the eruption of the volcano to the end of 1992 as compared to the High-resolution Infrared Sounder (HIRS) observations, and the formation of sulfate in MAM5-PSA with FC (with an additional OH replenishment reaction) was significantly faster than in MAM4 with FC. Analyses of microphysical processes indicate that more sulfate aerosol mass was generated in total in FC experiments than in SC experiments. MAM5-PSA performs better than MAM4 in simulation of aerosol optical depth (AOD); AOD anomalies from the MAM5-PSA experiment have better agreement with observations. The simulated largest changes in global mean net radiative flux at the top of the atmosphere following the eruption were about −3 W m −2 in MAM5-PSA experiments and roughly −1.5 W m −2 in MAM4 experiments.

AEROSOL↗
DOE OSTI2024

Cloud condensation nuclei concentrations derived from the CAMS reanalysis

Determining number concentrations of cloud condensation nuclei (CCN) is one of the first steps in the chain in analysis of cloud droplet formation, the direct microphysical link between aerosols and cloud droplets, and a process key for aerosol–cloud interactions (ACI). However, due to sparse coverage of in situ measurements and difficulties associated with retrievals from satellites, a global exploration of their magnitude, source as well as temporal and spatial distribution cannot be easily obtained. Thus, a better representation of CCN numbers is one of the goals for quantifying ACI processes and achieving uncertainty-reduced estimates of their associated radiative forcing. Here, we introduce a new CCN dataset which is derived based on aerosol mass mixing ratios from the latest Copernicus Atmosphere Monitoring Service reanalysis (CAMSRA) in a diagnostic model that uses CAMSRA aerosol properties and a simplified kappa-Köhler framework suitable for global models. The emitted aerosols in CAMSRA are not only based on input from emission inventories using aerosol observations, they also have a strong tie to satellite-retrieved aerosol optical depth (AOD) as this is assimilated as a constraining factor in the reanalysis. Furthermore, the reanalysis interpolates for cases of poor or missing retrievals and thus allows for a full spatiotemporal quantification of CCN numbers. The derived CCN dataset captures the general trend and spatial and temporal distribution of total CCN number concentrations and CCN from different aerosol species. A brief evaluation with ground-based in situ measurements demonstrates the improvement of the modelled CCN over the sole use of AOD as a proxy for CCN as the overall correlation coefficient improved from 0.37 to 0.71. However, we find the modelled CCN from CAMSRA to be generally high biased and find a particular erroneous overestimation at one heavily polluted site which emphasises the need for further validation. The CCN dataset (https://doi.org/10.26050/WDCC/QUAERERE_CCNCAMS_v1, Block, 2023), which is now freely available to users, features 3-D CCN number concentrations of global coverage for various supersaturations and aerosol species covering the years 2003–2021 with daily frequency. This dataset is one of its kind as it offers lots of opportunities to be used for evaluation in models and in ACI studies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Towards an improved representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model: RegCM

Mitigation of carbonaceous aerosol emissions is expected to provide climate and health co-benefits. The accurate representation of carbonaceous aerosols in climate models is critical for reducing uncertainties in their climate feedback. In this regard, emission fluxes and aerosol life cycle processes are the two primary sources of uncertainties. Here, we demonstrate that the incorporation of a dynamic ageing scheme and emission estimates that are updated for the local sources improves the representation of carbonaceous aerosols over the Indian monsoon region in a regional climate model, RegCM, compared with its default configuration. The respective mean black carbon (BC) and organic carbon (OC) surface concentrations in 2010 are estimated to be 4.25 and 10.35 µg m -3 over the Indo-Gangetic Plain (IGP) in the augmented model. The BC column burden over the polluted IGP is found to be 2.47 mg m -2 , 69.95 % higher than in the default model configuration and much closer to available observations. The anthropogenic aerosol optical depth (AOD) increases by more than 19 % over the IGP due to the model enhancement, also leading to a better agreement with observed AOD. The respective top-of-the-atmosphere, surface, and atmospheric anthropogenic aerosol short-wave radiative forcing are estimated at -0.3, -9.3, and 9.0 W m -2 over the IGP and -0.89, -5.33, and 4.44 W m -2 over Peninsular India (PI). Our results suggest that the combined effect of two modifications leads to maximum improvements in the model performance in regions where emissions play a dominant role.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

Trans-Pacific transport and evolution of aerosols: Evaluation of quasi-global WRF-Chem simulation with multiple observations

A fully coupled meteorology-chemistry model (WRF-Chem, the Weather Research and Forecasting model coupled with chemistry) has been configured to conduct quasi-global simulation for 5 years (2010–2014) and evaluated with multiple observation data sets for the first time. The evaluation focuses on the simulation over the trans-Pacific transport region using various reanalysis and observational data sets for meteorological fields and aerosol properties. The simulation generally captures the overall spatial and seasonal variability of satellite retrieved aerosol optical depth (AOD) and absorbing AOD (AAOD) over the Pacific that is determined by the outflow of pollutants and dust and the emissions of marine aerosols. The assessment of simulated extinction Ångström exponent (EAE) indicates that the model generally reproduces the variability of aerosol size distributions as seen by satellites. In addition, the vertical profile of aerosol extinction and its seasonality over the Pacific are also well simulated. The difference between the simulation and satellite retrievals can be mainly attributed to model biases in estimating marine aerosol emissions as well as the satellite sampling and retrieval uncertainties. Compared with the surface measurements over the western USA, the model reasonably simulates the observed magnitude and seasonality of dust, sulfate, and nitrate surface concentrations, but significantly underestimates the peak surface concentrations of carbonaceous aerosol likely due to model biases in the spatial and temporal variability of biomass burning emissions and secondary organic aerosol (SOA) production. A sensitivity simulation shows that the trans-Pacific transported dust, sulfate, and nitrate can make significant contribution to surface concentrations over the rural areas of the western USA, while the peaks of carbonaceous aerosol surface concentrations are dominated by the North American emissions. Both the retrievals and simulation show small interannual variability of aerosol characteristics for 2010–2014 averaged over three Pacific sub-regions. Furthermore, the evaluation in this study demonstrates that the WRF-Chem quasi-global simulation can be used for investigating trans-Pacific transport of aerosols and providing reasonable inflow chemical boundaries for the western USA, allowing one to further understand the impact of transported pollutants on the regional air quality and climate with high-resolution nested regional modeling.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2013

Campaign datasets for Two-Column Aerosol Project (TCAP)

This campaign was designed to provide a detailed set of observations with which to 1) perform radiative and cloud condensation nuclei (CCN) closure studies, 2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing 3) extend a previously developed technique to investigate aerosol indirect effects, and 4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) was deployed on Cape Cod, Massachusetts for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation and cloud characteristics at a location subject to both clear- and cloudy- conditions, and clean- and polluted-conditions. These observations were supplemented by two aircraft intensive observation periods (IOPS), one in the summer and a second in the winter. Each IOP required two aircraft.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1986

Time and space integrating acousto-optic folded spectrum processing for SETI

Time and space integrating folded spectrum techniques utilizing acousto-optic devices (AOD) as 1-D input transducers are investigated for a potential application as wideband, high resolution, large processing gain spectrum analyzers in the search for extra-terrestrial intelligence (SETI) program. The space integrating Fourier transform performed by a lens channels the coarse spectral components diffracted from an AOD onto an array of time integrating narrowband fine resolution spectrum analyzers. The pulsing action of a laser diode samples the interferometrically detected output, aliasing the fine resolution components to baseband, as required for the subsequent charge coupled devices (CCD) processing. The raster scan mechanism incorporated into the readout of the CCD detector array is used to unfold the 2-D transform, reproducing the desired high resolution Fourier transform of the input signal.

Wagner, K.↗
NASA NTRS2000

Clear-Sky Closure Studies of Lower Tropospheric Aerosol and Water Vapor During ACE-2 Using Airborne Sunphotometer, Airborne In-Situ, Space-Borne, and Ground-Based Measurements

We report on clear-sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE-2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in-situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space-borne NOAA/AVHRR data and ground-based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud-free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in-situ aerosol size-distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (lambda = 380-1060 nm) is 3-8%. In the MBL there is a tendency for the in-situ results to be slightly lower than the sunphotometer measurements (10-17% at lambda = 525 nm), but these differences are within the combined error bars of the measurements and computations.

Schmid, Beat↗