Cimel Sunphotometer Quality Checked and filtered Aerosol Optical Thickness
This is a quality checked aerosol optical depth (version 3) data ingested from Aeronet.
54 ENVIRONMENTAL SCIENCES↗
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The Global Atmosphere‐aerosol Model ICON‐A‐HAM2.3–Initial Model Evaluation and Effects of Radiation Balance Tuning on Aerosol Optical Thickness
Abstract The Hamburg Aerosol Module version 2.3 (HAM2.3) from the ECHAM6.3‐HAM2.3 global atmosphere‐aerosol model is coupled to the recently developed icosahedral nonhydrostatic ICON‐A (icon‐aes‐1.3.00) global atmosphere model to yield the new ICON‐A‐HAM2.3 atmosphere‐aerosol model. The ICON‐A and ECHAM6.3 host models use different dynamical cores, parameterizations of vertical mixing due to sub‐grid scale turbulence, and parameter settings for radiation balance tuning. Here, we study the role of the different host models for simulated aerosol optical thickness (AOT) and evaluate impacts of using HAM2.3 and the ECHAM6‐HAM2.3 two‐moment cloud microphysics scheme on several meteorological variables. Sensitivity runs show that a positive AOT bias over the subtropical oceans is remedied in ICON‐A‐HAM2.3 because of a different default setting of a parameter in the moist convection parameterization of the host models. The global mean AOT is biased low compared to MODIS satellite instrument retrievals in ICON‐A‐HAM2.3 and ECHAM6.3‐HAM2.3, but the bias is larger in ICON‐A‐HAM2.3 because negative AOT biases over the Amazon, the African rain forest, and the northern Indian Ocean are no longer compensated by high biases over the sub‐tropical oceans. ICON‐A‐HAM2.3 shows a moderate improvement with respect to AOT observations at AERONET sites. A multivariable bias score combining biases of several meteorological variables into a single number is larger in ICON‐A‐HAM2.3 compared to standard ICON‐A and standard ECHAM6.3. In the tropics, this multivariable bias is of similar magnitude in ICON‐A‐HAM2.3 and in ECHAM6.3‐HAM2.3. In the extra‐tropics, a smaller multivariable bias is found for ICON‐A‐HAM2.3 than for ECHAM6.3‐HAM2.3.
54 ENVIRONMENTAL SCIENCES↗
Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause
Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.
54 ENVIRONMENTAL SCIENCES↗
Estimation of Sea Spray Aerosol Surface Area Over the Southern Ocean Using Scattering Measurements
This study focuses on methods to estimate dry marine aerosol surface area (SA) from bulk optical measurements. Aerosol SA is used in many models' ice nucleating particle (INP) parameterizations, as well as influencing particle light scattering, hygroscopic growth, and reactivity, but direct observations are scarce in the Southern Ocean (SO). Two campaigns jointly conducted in austral summer 2018 provided co-located measurements of aerosol SA from particle size distributions and lidar to evaluate SA estimation methods in this region. Mie theory calculations based on measured size distributions were used to test a proposed approximation for dry aerosol SA, which relies on estimating effective scattering efficiency (Q) as a function of Ångström exponent (å). For distributions with dry å < 1, Q = 2 was found to be a good approximation within ±50%, but for distributions with dry å > 1, an assumption of Q = 3 as in some prior studies underestimates dry aerosol SA by a factor of 2 or more. We propose a new relationship between dry å and Q, which can be used for –0.2 < å < 2, and suggest å = 0.8 as the cutoff between primary and secondary marine aerosol-dominated distributions. Application of a published methodology to retrieve dry marine aerosol SA from lidar extinction profiles overestimated aerosol SA by a factor of 3–5 during these campaigns. Using Microtops aerosol optical thickness measurements, we derive alternative lidar conversion parameters from our observations, applicable to marine aerosol over the SO.
54 ENVIRONMENTAL SCIENCES↗
Cloud, Aerosol, and Radiative Properties Over the Western North Atlantic Ocean
This study examines the atmospheric properties of weather states (WSs) derived from the International Satellite Cloud Climatology Project (ISCCP) over the Western North Atlantic Ocean. In particular, radiation and aerosol data corresponding to two sites in the study domain, Pennsylvania State University and Bermuda, were examined to characterize the atmospheric properties of the various satellite-derived WSs. At both sites, the fair weather WS was most prevalent, followed by the cirrus WS. Differences in the seasonality of the various WSs were observed at the two sites. Fractional sky cover and effective shortwave cloud transmissivity derived from ground-based radiation measurements were able to capture differences among the satellite-derived WSs. Speciated aerosol optical thicknesses (AOT) from the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) were used to investigate potential differences in aerosol properties among the WSs. The clear sky WS exhibited below-average seasonal values of AOT at both sites year-round, as well as relatively high rates of occurrence with low AOT events. In addition, the clear sky WS showed above-average contributions from dust and black carbon to the total AOT year-round. Finally, transitions between various WSs were examined under low, high, and mid-range AOT conditions. The most common pathway was for the WSs to remain in the same state after a 3 hr interval. Some WSs, such as midlatitude storms, deep convection, middle top, and shallow cumulus, were more prevalent as ending states under high AOT conditions. This work motivates examining differences in aerosol properties between WSs in other regions.
54 ENVIRONMENTAL SCIENCES↗
Australian wildfire smoke in the stratosphere: the decay phase in 2020/2021 and impact on ozone depletion
Abstract. Record-breaking wildfires raged in southeastern Australia in late December 2019 and early January 2020. Rather strong pyrocumulonimbus (pyroCb) convection developed over the fire areas and lofted enormous amounts of biomass burning smoke into the tropopause region and caused the strongest wildfire-related stratospheric aerosol perturbation ever observed around the globe. We discuss the geometrical, optical, and microphysical properties of the stratospheric smoke layers and the decay of this major stratospheric perturbation. A multiwavelength polarization Raman lidar at Punta Arenas (53.2∘ S, 70.9∘ W), southern Chile, and an elastic backscatter Raman lidar at Río Grande (53.8∘ S, 67.7∘ W) in southern Argentina, were operated to monitor the major record-breaking event until the end of 2021. These lidar measurements can be regarded as representative for mid to high latitudes in the Southern Hemisphere. A unique dynamical feature, an anticyclonic, smoke-filled vortex with 1000 km horizontal width and 5 km vertical extent, which ascended by about 500 m d−1, was observed over the full last week of January 2020. The key results of the long-term study are as follows. The smoke layers extended, on average, from 9 to 24 km in height. The smoke partly ascended to more than 30 km height as a result of self-lofting processes. Clear signs of a smoke impact on the record-breaking ozone hole over Antarctica in September–November 2020 were found. A slow decay of the stratospheric perturbation detected by means of the 532 nm aerosol optical thickness (AOT) yielded an e-folding decay time of 19–20 months. The maximum smoke AOT was around 1.0 over Punta Arenas in January 2020 and thus 2 to 3 orders of magnitude above the stratospheric aerosol background of 0.005. After 2 months with strongly varying smoke conditions, the 532 nm AOT decreased to 0.03-0.06 from March–December 2020 and to 0.015–0.03 throughout 2021. The particle extinction coefficients at 532 nm were in the range of 10–75 Mm−1 in January 2020 and, later on, mostly between 1 and 5 Mm−1. Combined lidar–photometer retrievals revealed typical smoke extinction-to-backscatter ratios of 69 ± 19 sr (at 355 nm), 91 ± 17 sr (at 532 nm), and 120 ± 22 sr (at 1064 nm). An ozone reduction of 20 %–25 % in the 15–22 km height range was observed over Antarctica and New Zealand ozonesonde stations in the smoke-polluted air, with particle surface area concentrations of 1–5 µm2 cm−3.
Ohneiser, Kevin↗
Intra-annual variations of regional total column ozone, aerosol optical depth, and water vapor from ground-based, satellite-based and model-based observations
The Microtops II ozonometer has been deployed to continuously measure the total column ozone (TCO), pre-cipitable water content (PWC) and aerosol optical thickness (AOT) at Atigre village (16.74° N, 74.37° E, 604 m above sea level, masl) located on the southeastern slope of Indian western Ghats. The Microtops II ozonometer measurements during the period from September 2017 to June 2018 were analyzed along with the retrieved products of Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) onboard NASA's Terra satellites and also the ERA-interim reanalysis model. We found that the TCO (or PWC) data from the OMI (or MODIS) and the ERA reanalysis model data products are in good agreement. The mea-surements showed strong seasonal variability such that TCO was lowest in the winter season but increased in the summer season, and both PWC and AOT were lowest in the post-monsoon season and increased in the summer season. In continuous ERA-interim reanalysis TCO observations, we found the three types of periodicities in the daily mean TCO as well as PWC (i) The weekly (7 days), (ii) quasi-biweekly (14 to 16 days), (iii) Madden Julian Oscillations (MJO) (30–60 days) oscillations. These oscillations depend on the periodic weather changes in the troposphere. We also observe that the average day to day variability in daily mean TCO observations in the observational period is about 1.4%, 1.1%, 2.62% in the Microtops II ozonometer, ERA-interim reanalysis, and OMI data respectively. We found the positive correlation between daily mean AOT and PWC in all seasons (except monsoon), which is maximum in the winter season, showing the hygroscopic nature of aerosols. The sources of water vapor and aerosol at our location are also studied using back-trajectory analysis.
Nade, Dada R.↗
Natural and anthropogenic contributions to the hurricane drought of the 1970s–1980s
Atlantic hurricane activity experienced a pronounced lull during the 1970s and 1980s. The current explanation that anthropogenic aerosol radiative forcing cooled the sea surface locally fails to capture the magnitude of this large decrease in activity. To explain this hurricane drought, we propose that the radiative effects of sulfate aerosols from Europe and North-America decreased precipitation in the Sahara-Sahel region, leading to an enhancement of dust regional emissions and transport over the Atlantic. This dust in turn enhanced the local decrease of sea-surface temperature and of hurricane activity. Here, we show that dust emissions from the Sahara peaked in phase with regional sulfate aerosol optical thickness and Sahel drought conditions, and that dust optical depth variations alone can explain nearly half of the sea-surface temperature depression in the 1970s and 1980s.
54 ENVIRONMENTAL SCIENCES↗
Properties and Controlling Processes of Aerosol and Cloud Condensation Nuclei in Marine Boundary Layer Over Eastern North Atlantic (Final Report)
Remote marine low cloud systems have large spatial and temporal coverages. Because of their relatively low optical thickness and background aerosol concentrations, marine low clouds are particularly susceptible to perturbations in aerosols associated with anthropogenic emissions. Recent studies show that a large fraction of the global aerosol indirect forcing can be attributed to changes in marine low clouds, despite their relatively long distance from most anthropogenic sources. Currently, there remain large uncertainties in the magnitude of the global aerosol indirect radiative forcing. One major contribution to this large uncertainty derives from poor understanding of the aerosols under natural conditions, the perturbation by anthropogenic emissions, and the processes that drive them. In this project, we took advantage of the comprehensive, multi-dimensional characterization of meteorological parameters, trace gases, aerosol, cloud, and drizzle fields during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) and the long-term measurements at the Atmospheric Radiation Measurement (ARM) Eastern North Atlantic (ENA) site on Graciosa Island. By synergistically combining in situ measurements, remote sensing retrievals, and model simulations, we quantified aerosol properties in the ENA, their vertical profiles, and variations with season, synoptic state, and airmass. We investigated key aerosol processes, including entrainment of free troposphere aerosol into marine boundary layer, new particle formation, growth of Aitken mode particles, and the influences of these processes on the cloud condensation nuclei (CCN) population in marine boundary layer. The representation of key aerosol processes in the Energy Exascale Earth System Model (E3SM) was evaluated using the observations. This project has led to 26 publications, which are listed at the end of this report.
54 ENVIRONMENTAL SCIENCES↗
Long-Term Trends in Aerosols, Low Clouds, and Large-Scale Meteorology Over the Western North Atlantic From 2003 to 2020
Here, a continuous decrease in aerosols over the Western North Atlantic Ocean (WNAO) on a decadal timescale provides a long-term benchmark to evaluate how various natural and anthropogenic processes affect the manifestation of aerosol-cloud interactions in this region. Furthermore, the WNAO serves as a natural laboratory with diverse aerosol sources, marine boundary layer clouds more variable than those in marine stratocumulus deck regions, and unique flow regimes established by the Gulf Stream and the semi-permanent Bermuda High. We investigate how satellite-retrieved macrophysical and microphysical properties of low clouds and the surface shortwave irradiance changed from 2003 to 2020, in tandem with this aerosol decrease. The decadal changes in large-scale meteorology related to the North Atlantic Oscillation (NAO) are also examined. We find a reduction in low-cloud optical thickness, accompanied by fewer and larger cloud droplets, yet observe no significant changes in low-cloud fraction and liquid water path. Despite the reduction in low-cloud optical thickness together with aerosol decrease, a corresponding increase in the trends of surface shortwave irradiance, also known as surface brightening, is lacking. This absence of brightening is potentially related to concomitant changes found in large-scale meteorology associated with NAO—Bermuda High strengthening, sea surface warming, and atmospheric moistening— as well as an increase in high-level cloud fraction that can counteract the surface brightening. Ultimately, our findings suggest that spatial patterns of decadal meteorological variability introduce complexities in the surface cloud radiative effect over the WNAO, thereby complicating the isolation and examination of aerosol-cloud interactions.
54 ENVIRONMENTAL SCIENCES↗
Steady-state mixing state of black carbon aerosols from a particle-resolved model
Abstract. Black carbon (BC) exerts a notable warming effect due to its strong light absorption, largely influenced by its “mixing state”. However, due to computational constraints, the mixing state is challenging to accurately represent in large-scale models. In this study, we employ a particle-resolved model to simulate the evolution of BC mixing state based on field observation. Our result shows that aerosol compositions, coating thickness (CT) distribution, and optical properties of BC aerosols all exhibit a tendency toward a steady state with a characteristic timescale of less than 1 d, considerably shorter than the BC atmospheric lifetime. The rapid attainment of a steady state suggests that it is reasonable to disregard this pre-steady-state period and instead concentrate on the average properties of BC across extensive spatial and temporal scales. The distribution of CT follows an exponential linear distribution and can be characterized by a single slope parameter k. This distribution is independent of the BC core's distribution. In the model simulation, the mean CT, equivalent to the 1/k, is 62 nm, which is consistent with the statistical results indicating a mean CT of 63 nm. Utilizing the slope parameter k, which effectively characterizes the CT distribution under the steady-state simplifying assumption, the BC absorption enhancement closely corresponds to the results obtained via the particle-resolved method. This study simplifies the BC mixing state description and yields a precise evaluation of the BC optical properties, which has the potential utility for modeling efforts in the refinement of the assessment of BC's radiative effects.
Zhang, Zhouyang↗
Aquaplanets as a Framework for Examination of Aerosol Effects
Although fundamental to the planetary radiative balance, aerosol impacts are highly uncertain in climate simulations because of the uneven distribution of aerosol sources and the complex interactions with radiation and clouds that are difficult to represent in climate models. This study proposes that aquaplanet configurations represent an idealized framework to investigate aerosol effects. As a simple demonstration, a series of aquaplanet simulations with the Community Atmosphere Model version 6 shows that the spatial distribution of aerosol emissions changes the aerosol effective radiative forcing even with unchanged total emissions. Some statistical properties of the simulations are presented to show that relatively short model integrations yield robust results. Much of the aerosol effect is shown to arise from aerosol–cloud interactions, especially through rapid adjustments associated with the aerosol lifetime effect that alter the cloud optical thickness.
54 ENVIRONMENTAL SCIENCES↗
Aerosol-induced closure of marine cloud cells: enhanced effects in the presence of precipitation
Abstract. The Weather Research Forecasting (WRF) version 4.3 model is configured within a Lagrangian framework to quantify the impact of aerosols on evolving cloud fields. Kilometer-scale simulations utilizing meteorological boundary conditions are based on 10 case study days offering diverse meteorology during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA). Measurements from aircraft, the ground-based Atmosphere Radiation Measurement (ARM) site at Graciosa Island in the Azores, and A-Train and geostationary satellites are utilized for validation, demonstrating good agreement with the WRF-simulated cloud and aerosol properties. Higher aerosol concentration leads to suppressed drizzle and increased cloud water content in all case study days. These changes lead to larger radiative cooling rates at cloud top, enhanced vertical velocity variance, and increased vertical and horizontal wind speed near the base of the lower-tropospheric inversion. As a result, marine cloud cell area expands, narrowing the gap between shallow clouds and increasing cloud optical thickness, liquid water content, and the top-of-atmosphere outgoing shortwave flux. While similar aerosol effects are observed in lightly to non-raining clouds, they tend to be smaller by comparison. These simulations show a relationship between cloud cell area expansion and the radiative adjustments caused by liquid water path and cloud fraction changes. The adjustments are positive and scale as 74 % and 51 %, respectively, relative to the Twomey effect. While higher-resolution large-eddy simulations may provide improved representation of cloud-top mixing processes, these results emphasize the importance of addressing mesoscale cloud-state transitions in the quantification of aerosol radiative forcing that cannot be attained from traditional climate models.
54 ENVIRONMENTAL SCIENCES↗
Glaciation of liquid clouds, snowfall, and reduced cloud cover at industrial aerosol hot spots
The ability of anthropogenic aerosols to freeze supercooled cloud droplets remains debated. Here, in this work, we present observational evidence for the glaciation of supercooled liquid-water clouds at industrial aerosol hot spots at temperatures between -10° and -24°C. Compared with the nearby liquid-water clouds, shortwave reflectance was reduced by 14% and longwave radiance was increased by 4% in the glaciation-affected regions. There was an 8% reduction in cloud cover and an 18% reduction in cloud optical thickness. Additionally, daily glaciation-induced snowfall accumulations reached 15 millimeters. Glaciation events downwind of industrial aerosol hot spots indicate that anthropogenic aerosols likely serve as ice-nucleating particles. However, rare glaciation events downwind of nuclear power plants indicate that factors other than aerosol emissions may also play a role in the observed glaciation events.
54 ENVIRONMENTAL SCIENCES↗
Evaluation of cloud height, optical thickness, and phase retrievals from the CHROMA algorithm applied to Sentinel-3 OLCI data
We previously developed the Cloud Height Retrieval from O 2 Molecular Absorption (CHROMA) algorithm for the Ocean Color Instrument (OCI) on the new NASA Plankton, Aerosol, Cloud, ocean Ecosystem (PACE) mission. Here, we apply CHROMA to observations from the Ocean Land Colour Instrument (OLCI) to guide expectations for PACE, as it will take some time to obtain large-scale validation data for OCI. We use cloud top height (CTH), phase, and (for liquid clouds) cloud optical thickness (COT) data from the ground-based Atmospheric Radiation Measurement (ARM) network to evaluate the OLCI retrievals. We found that OLCI and Moderate Resolution Imaging Spectroradiometer (MODIS) CTH compare similarly well to the ARM reference. OLCI has a tendency to underestimate CTH as CTH increases, and algorithm assumptions about cloud geometric thickness may contribute to this. ARM COT from multifilter shadowband radiometers (MFRSR) and Sun photometers are well-correlated with one another, albeit with a roughly 30 % offset on average; OLCI and MODIS COT agree more closely with the MFRSR data. OLCI retrieval uncertainty estimates show skill at telling low-uncertainty cases from high-uncertainty ones, although CTH uncertainties are underestimated. Additionally, we compare the OLCI data to satellite retrievals based on thermal infrared measurements from MODIS and Sea and Land Surface Temperature Radiometer (SLSTR) data. Differences are broadly consistent with physical expectations based on the A-band vs. thermal techniques, although one key challenge in such aggregated comparisons is different cloud masking sensitivities and algorithm failure rates meaning additional sampling differences are introduced. We conclude by discussing the transition to and possible enhancements for PACE OCI.
Sayer, Andrew M. [Univ. of Maryland Baltimore Coun↗
Modeled and observed properties related to the direct aerosol radiative effect of biomass burning aerosol over the southeastern Atlantic
Biomass burning smoke is advected over the southeastern Atlantic Ocean between July and October of each year. This smoke plume overlies and mixes into a region of persistent low marine clouds. Model calculations of climate forcing by this plume vary significantly in both magnitude and sign. NASA EVS-2 (Earth Venture Suborbital-2) ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) had deployments for field campaigns off the west coast of Africa in 3 consecutive years (September 2016, August 2017, and October 2018) with the goal of better characterizing this plume as a function of the monthly evolution by measuring the parameters necessary to calculate the direct aerosol radiative effect. Here, this dataset and satellite retrievals of cloud properties are used to test the representation of the smoke plume and the underlying cloud layer in two regional models (WRF-CAM5 and CNRM-ALADIN) and two global models (GEOS and UM-UKCA). The focus is on the comparisons of those aerosol and cloud properties that are the primary determinants of the direct aerosol radiative effect and on the vertical distribution of the plume and its properties. The representativeness of the observations to monthly averages are tested for each field campaign, with the sampled mean aerosol light extinction generally found to be within 20 % of the monthly mean at plume altitudes. When compared to the observations, in all models, the simulated plume is too vertically diffuse and has smaller vertical gradients, and in two of the models (GEOS and UM-UKCA), the plume core is displaced lower than in the observations. Plume carbon monoxide, black carbon, and organic aerosol masses indicate underestimates in modeled plume concentrations, leading, in general, to underestimates in mid-visible aerosol extinction and optical depth. Biases in mid-visible single scatter albedo are both positive and negative across the models. Observed vertical gradients in single scatter albedo are not captured by the models, but the models do capture the coarse temporal evolution, correctly simulating higher values in October (2018) than in August (2017) and September (2016). Uncertainties in the measured absorption Ångstrom exponent were large but propagate into a negligible (<4 %) uncertainty in integrated solar absorption by the aerosol and, therefore, in the aerosol direct radiative effect. Model biases in cloud fraction, and, therefore, the scene albedo below the plume, vary significantly across the four models. The optical thickness of clouds is, on average, well simulated in the WRF-CAM5 and ALADIN models in the stratocumulus region and is underestimated in the GEOS model; UM-UKCA simulates cloud optical thickness that is significantly too high. Overall, the study demonstrates the utility of repeated, semi-random sampling across multiple years that can give insights into model biases and how these biases affect modeled climate forcing. The combined impact of these aerosol and cloud biases on the direct aerosol radiative effect (DARE) is estimated using a first-order approximation for a subset of five comparison grid boxes. A significant finding is that the observed grid box average aerosol and cloud properties yield a positive (warming) aerosol direct radiative effect for all five grid boxes, whereas DARE using the grid-box-averaged modeled properties ranges from much larger positive values to small, negative values. It is shown quantitatively how model biases can offset each other, so that model improvements that reduce biases in only one property (e.g., single scatter albedo but not cloud fraction) would lead to even greater biases in DARE. Across the models, biases in aerosol extinction and in cloud fraction and optical depth contribute the largest biases in DARE, with aerosol single scatter albedo also making a significant contribution.
54 ENVIRONMENTAL SCIENCES↗
Analysis of contrasting aerosol indirect effects in liquid water clouds over the northern part of Arabian Sea
The extensive daily statistics of aerosol properties, cloud properties, and their mutual correlations provide crucial information for better assessing future climate change. Here, in this paper, 14 years (2010–2023) of data from the Moderate Resolution Imaging Spectroradiometer (MODIS) are analyzed over the northern part of Arabian Sea (Latitude: 21°–25° N and Longitude: 62°–68° E) to assess the characteristics of aerosols and clouds and their relationships under different meteorological conditions. When aerosol optical depth (AOD) is less than ~0.7, the observations exhibit a positive correlation between AOD and cloud droplet effective radius (CDR) but negative correlations between AOD and cloud droplet number concentration (CDNC), between AOD and cloud optical depth (COD), between AOD and cloud liquid water path (CLWP), and between AOD and cloud geometrical thickness (H). The corresponding aerosol-cloud correlations change signs when the AOD values are larger than 0.7. However, the single folded positive AOD-cloud fraction (CF) relationship is observed in both AOD regimes. Similar correlations are also observed between precipitable water vapor (PWV) and CDR, CDNC, COD, H, CF and CLWP, together with a positive correlation between PWV and AOD. Further isolation of the environmental effects from aerosol effects by stratifying AOD and cloud data into different LTS and PWV bins shows that the signature of the well-known Twomey effect is observed under high LTS-high PWV conditions, while an opposite effect (anti-Twomey) is observed under low PWV conditions, regardless of LTS values. Additionally, negative correlations between AOD and COD, AOD and CLWP, and AOD and H are observed under low LTS, regardless of PWV conditions, with a slight positive correlation when AOD >0.4 under high LTS and PWV conditions.
54 ENVIRONMENTAL SCIENCES↗
Cloud Top Radiative Cooling Rate Drives Non-Precipitating Stratiform Cloud Responses to Aerosol Concentration
Increases in aerosol concentration are well known to influence the microphysical processes and radiative properties of clouds. By reducing droplet size, an increase in aerosol can lessen collision efficiency and increase liquid water path (LWP) in precipitating clouds or enhance evaporation rate and decrease LWP in non-precipitating clouds. We utilize large eddy simulations to further investigate these aerosol indirect effects in Arctic mixed-phase clouds and find, in agreement with previous studies, precipitating clouds to experience an increase in LWP and non-precipitating clouds a decrease in LWP. Most importantly however, our results reveal a different explanation for why such an LWP decrease occurs in decoupled, non-precipitating clouds. We find enhanced evaporation near cloud top to be driven primarily by a strengthening of maximum radiative cooling rate with aerosol concentration which drives stronger entrainment, an effect that holds true even in clouds that are optically thick.
58 GEOSCIENCES↗