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Abstract: We report on a multiyear set of airborne field campaigns (2005–16) off the California coast to examine aerosols, clouds, and meteorology, and how lessons learned tie into the upcoming NASA Earth Venture Suborbital (EVS-3) campaign: Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE; 2019–23). The largest uncertainty in estimating global anthropogenic radiative forcing is associated with the interactions of aerosol particles with clouds, which stems from the variability of cloud systems and the multiple feedbacks that affect and hamper efforts to ascribe changes in cloud properties to aerosol perturbations. While past campaigns have been limited in flight hours and the ability to fly in and around clouds, efforts sponsored by the Office of Naval Research have resulted in 113 single aircraft flights (>500 flight hours) in a fixed region with warm marine boundary layer clouds. All flights used nearly the same payload of instruments on a Twin Otter to fly below, in, and above clouds, producing an unprecedented dataset. We provide here i) an overview of statistics of aerosol, cloud, and meteorological conditions encountered in those campaigns and ii) quantification of model-relevant metrics associated with aerosol–cloud interactions leveraging the high data volume and statistics. Based on lessons learned from those flights, we describe the pragmatic innovation in sampling strategy (dual-aircraft approach with combined in situ and remote sensing) that will be used in ACTIVATE to generate a dataset that can advance scientific understanding and improve physical parameterizations for Earth system and weather forecasting models, and for assessing next-generation remote sensing retrieval algorithms.

The North Atlantic Aerosols and Marine Ecosystems Study (NAAMES) is an interdisciplinary investigation to improve understanding of Earth's ocean ecosystem-aerosol-cloud system. Specific overarching science objectives for NAAMES are to (1) characterize plankton ecosystem properties during primary phases of the annual cycle and their dependence on environmental forcings, (2) determine how these phases interact to recreate each year the conditions for an annual plankton bloom, and (3) resolve how remote marine aerosols and boundary layer clouds are influenced by plankton ecosystems. Four NAAMES field campaigns were conducted in the western subarctic Atlantic between November 2015 and April 2018, with each campaign targeting specific seasonal events in the annual plankton cycle. A broad diversity of measurements were collected during each campaign, including ship, aircraft, autonomous float and drifter, and satellite observations. Here, we present an overview of NAAMES science motives, experimental design, and measurements. We then briefly describe conditions and accomplishments during each of the four field campaigns and provide information on how to access NAAMES data. The intent of this manuscript is to familiarize the broad scientific community with NAAMES and to provide a common reference overview of the project for upcoming publications.

The western North Atlantic Ocean is strongly influenced by continental outflow, making it an ideal region to study the atmospheric transition from a polluted coastline to the marine environment. Utilizing eight transit flights between the NASA Langley Research Center (LaRC) in Hampton, Virginia, and the remote island of Bermuda from NASA's Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE), we examine the evolution of trace gas and aerosol properties off the US East Coast. The first pair of flights flew along the wind trajectory of continental outflow, while the other flights captured a mix of marine and continental air mass sources. For measurements within the boundary layer (BL), there was an offshore decline in particle N<100nm , N>100nm , CH 4 , CO, and CO 2 concentrations, all leveling off around ∼900 km offshore from the LaRC. These trends are strongest for the first pair of flights. In the BL, offshore declines in organic mass fraction and increases in sulfate mass fraction coincide with increasing hygroscopicity based on f (RH) measurements. Free troposphere measurements show a decline in N<100nm , but other measured parameters are more variable when compared to the prominent offshore gradients seen in the BL. Pollution layers exist in the free troposphere, such as smoke plumes, that can potentially entrain into the BL. This work provides detailed case studies with a broad set of high-resolution measurements to further our understanding of the transition between continental and marine environments. [ABSTRACT FROM AUTHOR]

Remote marine regions comprise a high fraction of Earth's surface, but in situ vertically resolved measurements over these locations remain scarce. Here we use airborne data during 15 vertical spiral soundings (0.15–8.5 km) over Bermuda during the NASA Aerosol Cloud meTeorology Interactions over the western ATlantic Experiment (ACTIVATE) to investigate the impact of different source regions on the vertical structure of trace gases, aerosol particles, and meteorological variables over 1000 km offshore of the US East Coast. Results reveal significant differences in vertical profiles of variables between three different air mass source categories (North America, Ocean, Caribbean/North Africa) identified using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model: (i) the strongest pollution signature is from air masses from the North America category, while the weakest one is from the Ocean category; (ii) North America air has the highest levels of CO, CH 4 , submicron particle number concentration, aerosol mass spectrometer (AMS) mass, and organic mass fraction along with smoke layers in the free troposphere (FT); (iii) Ocean air has the highest relative amount of nitrate, non-sea-salt sulfate, and oxalate, which are key acidic species participating in chloride depletion; (iv) air masses from the Caribbean/North Africa showed a pronounced coarse aerosol signature in the FT and reduced aerosol hygroscopicity, which is associated with dust transport; and (v) there is considerable vertical heterogeneity for almost all variables examined, including higher O 3 and submicron particle concentrations with altitude, suggesting that the FT is a potential contributor of both constituents in the marine boundary layer. This study highlights the importance of considering air mass source origin and vertical resolution to capture aerosol and trace gas properties over remote marine areas. [ABSTRACT FROM AUTHOR]

With the ongoing expansion of global observation networks, it is expected that we shall routinely analyze records of geophysical variables such as temperature from multiple collocated instruments. Validating datasets in this situation is not a trivial task because every observing system has its own bias and noise. Triple collocation is a general statistical framework to estimate the error characteristics in three or more observational-based datasets. In a triple colocation analysis, several metrics are routinely reported but traditional multiple-panel plots are not the most effective way to display information. A new formula of error variance is derived for connecting the key terms in the triple collocation theory. A diagram based on this formula is devised to facilitate triple collocation analysis of any data from observations, as illustrated using three aerosol optical depth datasets from the recent Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). An observational-based skill score is also derived to evaluate the quality of three datasets by taking into account both error variance and correlation coefficient. Several applications are discussed and sample plotting routines are provided. [ABSTRACT FROM AUTHOR]

Ocean surface wind speed (i.e., wind speed 10 m above sea level) is a critical parameter used by atmospheric models to estimate the state of the marine atmospheric boundary layer (MABL). Accurate surface wind speed measurements in diverse locations are required to improve characterization of MABL dynamics and assess how models simulate large-scale phenomena related to climate change and global weather patterns. To provide these measurements, this study introduces and evaluates a new surface wind speed data product from the NASA Langley Research Center nadir-viewing High Spectral Resolution Lidar – generation 2 (HSRL-2) using data collected as part of the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. The HSRL-2 can directly measure vertically resolved aerosol backscatter and extinction profiles without additional constraints or assumptions, enabling the instrument to accurately derive atmospheric attenuation and directly determine surface reflectance (i.e., surface backscatter). Also, the high horizontal spatial resolution of the HSRL-2 retrievals (0.5 s or ∼ 75 m along track) allows the instrument to probe the fine-scale spatial variability in surface wind speeds over time along the flight track and over breaks in broken cloud fields. A rigorous evaluation of these retrievals is performed by comparing coincident HSRL-2 and National Center for Atmospheric Research (NCAR) Airborne Vertical Atmosphere Profiling System (AVAPS) dropsonde data, owing to the joint deployment of these two instruments on the ACTIVATE King Air aircraft. These comparisons show correlations of 0.89, slopes of 1.04 and 1.17, and y intercepts of - 0.13 and - 1.05 ms-1 for linear and bisector regressions, respectively, and the overall accuracy is calculated to be 0.15 ± 1.80 ms-1. It is also shown that the dropsonde surface wind speed data most closely follow the HSRL-2 distribution of wave slope variance using the distribution proposed by Hu et al. (2008) rather than the ones proposed by Cox and Munk (1954) and Wu (1990) for surface wind speeds below 7 ms-1 , with this category comprising most of the ACTIVATE data set. The retrievals are then evaluated separately for surface wind speeds below 7 ms-1 and between 7 and 13.3 ms-1 and show that the HSRL-2 retrieves surface wind speeds with a bias of ∼ 0.5 ms-1 and an error of ∼ 1.5 ms-1 , a finding not apparent in the cumulative comparisons. Also, it is shown that the HSRL-2 retrievals are more accurate in the summer (- 0.18 ± 1.52 ms-1) than in the winter (0.63 ± 2.07 ms-1), but the HSRL-2 is still able to make numerous (N=236) accurate retrievals in the winter. Overall, this study highlights the abilities and assesses the performance of the HSRL-2 surface wind speed retrievals, and it is hoped that further evaluation of these retrievals will be performed using other airborne and satellite data sets. [ABSTRACT FROM AUTHOR]

Mesoscale organization of marine convective clouds into linear or clustered states is prevalent across the tropical and subtropical oceans, and its investigation served as a guiding focus for a series of process study flights conducted as part of the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) during summer 2020, 2021, and 2022. These select ACTIVATE flights involved a novel strategy for coordinating two aircraft, with respective remote sensing and in situ sampling payloads, to probe regions of organized shallow convection for several hours. The main purpose of this measurement report is to summarize the aircraft sampling approach, describe the characteristics and evolution of the cases, and provide an overview of the datasets that can serve as a starting point for more detailed modeling and analysis studies. Six flights are described, involving a total of 80 dropsonde profiles that capture the environment surrounding clustered shallow convection. The flights include detailed observations of the vertical structure of cloud systems, comprising up to 20 in situ sampling levels. Four cases involved deepening convection rooted in the marine boundary layer that developed vertically to 2–5 km with varying precipitation amounts, while two cases captured more complex and developed cumulus congestus systems extending above 5 km. In addition to the thermodynamic and dynamic characterization afforded by dropsonde and in situ measurements, the datasets include cloud and aerosol microphysics, trace gas concentrations, aerosol and droplet composition, and cloud and aerosol remote sensing from high-spectral-resolution lidar and polarimetry. [ABSTRACT FROM AUTHOR]

Aerosol optical depth was retrieved from two airborne remote sensing instruments, the Research Scanning Polarimeter (RSP) and Second Generation High Spectral Resolution Lidar (HSRL-2), during the National Aeronautics and Space Administration (NASA) Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). The field campaign offers a unique opportunity to evaluate an extensive 3-year dataset under a wide range of meteorological conditions from two instruments on the same platform. However, a long-standing issue in atmospheric field studies is that there is a lack of reference datasets for properly validating field measurements and estimating their uncertainties. Here we address this issue by using the triple collocation method, in which a third collocated satellite dataset from the Moderate Resolution Imaging Spectroradiometer (MODIS) is introduced for comparison. HSRL-2 is found to provide a more accurate retrieval than RSP over the study region. The error standard deviation of HSRL-2 with respect to the ground truth is 0.027. Moreover, this approach enables us to develop a simple, yet efficient, quality control criterion for RSP data. The physical reasons for the differences in two retrievals are determined to be cloud contamination, aerosols near the surface, multiple aerosol layers, absorbing aerosols, non-spherical aerosols, and simplified retrieval assumptions. These results demonstrate the pathway for optimal aerosol retrievals by combining information from both lidars and polarimeters for future airborne and satellite missions. [ABSTRACT FROM AUTHOR]

The Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) is a six-year (2019-2024) NASA Earth-Venture Suborbital-3 (EVS-3) mission to robustly characterize aerosol-cloud-meteorology interactions over the western North Atlantic Ocean (WNAO) during winter and summer seasons, with a focus on marine boundary layer clouds. This characterization requires understanding the aerosol life cycle (sources and sinks), composition, transport pathways, and distribution in the WNAO region. We use the GEOS-Chem chemical transport model driven by the MERRA-2 reanalysis to simulate tropospheric aerosols that are evaluated against in situ and remote sensing measurements from Falcon and King Air aircraft, respectively, as well as ground-based and satellite observations over the WNAO during the winter (Feb. 14 - Mar. 12) and summer (Aug. 13 - Sep. 30) field deployments of ACTIVATE 2020. Transport of pollution in the boundary layer behind cold fronts is a major mechanism for the North American continental outflow to the WNAO during Feb.-Mar. 2020. While large-scale frontal lifting is a dominant mechanism in winter, convective lifting significantly increases the vertical extent of major continental outflow aerosols in summer. Turbulent mixing is found to be the dominant process responsible for the vertical transport of sea salt within and ventilation out of the boundary layer in winter. The simulated boundary layer aerosol composition and optical depth (AOD) in the ACTIVATE flight domain are dominated by sea salt, followed by organic aerosol and sulfate. Compared to winter, boundary layer sea salt concentrations increased in summer over the WNAO, especially from the ACTIVATE flight areas to Bermuda, because of enhanced surface winds and emissions. Dust concentrations also significantly increased in summer because of long-range transport from North Africa. Comparisons of model and aircraft submicron non-refractory aerosol species (measured by an HR-ToF-AMS) vertical profiles show that intensive measurements of sulfate, nitrate, ammonium, and organic aerosols in the lower troposphere over the WNAO in winter provide useful constraints on model aerosol wet removal by precipitation scavenging. Comparisons of model aerosol extinction (at 550 nm) with the King Air High Spectral Resolution Lidar-2 (HSRL-2) measurements (at 532 nm) and CALIOP/CALIPSO satellite retrievals (at 532 nm) indicate that the model generally captures the continental outflow of aerosols, the land-ocean aerosol extinction gradient, and the mixing of anthropogenic aerosols with sea salt. Large enhancements of aerosol extinction at ~1.5-6.0 km altitudes from long-range transport of the western U.S. fire smoke were observed by HSRL-2 and CALIOP during Aug.-Sep. 2020. Model simulations with biomass burning (BB) emissions injected up to the mid-troposphere (vs. within the BL) better reproduce these remote-sensing observations, Falcon aircraft organic aerosol vertical profiles, as well as AERONET AOD measurements over eastern U.S. coast and Tudor Hill, Bermuda. High aerosol (mostly coarse-mode sea salt) extinction near the top (~1.5-2.0 km) of the marine BL along with high relative humidity and cloud extinction were typically seen over the WNAO (< 35°N) in the CALIOP aerosol extinction profiles and GEOS-Chem simulations, suggesting strong hygroscopic growth of sea salt particles and sea salt seeding of marine boundary layer clouds. Contributions of different emission types (anthropogenic, BB, biogenic, marine, and dust) to the total AOD over the WNAO in the model are also quantified. Future modeling efforts should focus on improving parameterizations for aerosol wet scavenging and sea salt emissions, implementing realistic BB emission injection height, and applying high-resolution models that better resolve vertical transport. [ABSTRACT FROM AUTHOR]

Inadequate knowledge about the complex microphysical and optical processes of the aerosol–cloud system severely restricts our ability to quantify the resultant impact on climate. Contrary to the negative radiative forcing (cooling) exerted by aerosols in cloud-free skies over dark surfaces, the absorbing aerosols, when lofted over the clouds, can potentially lead to significant warming of the atmosphere. The sign and magnitude of the aerosol radiative forcing over clouds are determined mainly by the amount of aerosol loading, the absorption capacity of aerosols or single-scattering albedo (SSA), and the brightness of the underlying cloud cover. In satellite-based algorithms that use measurements from passive sensors, the assumption of aerosol SSA is known to be the largest source of uncertainty in quantifying above-cloud aerosol optical depth (ACAOD). In this paper, we introduce a novel synergy algorithm that combines direct airborne measurements of ACAOD and the top-of-atmosphere (TOA) spectral reflectance from Ozone Monitoring Instrument (OMI) and Moderate Resolution Imaging Spectroradiometer (MODIS) sensors of NASA's A-train satellites to retrieve (1) SSA of light-absorbing aerosols lofted over the clouds and (2) aerosol-corrected cloud optical depth (COD). Radiative transfer calculations show a marked sensitivity of the TOA measurements to ACAOD, SSA, and COD, further suggesting that the availability of accurate ACAOD allows retrieval of SSA for above-cloud aerosol scenes using the "color ratio" algorithm developed for satellite sensors carrying ultraviolet (UV) and visible-near-IR (VNIR) wavelength bands. The proposed algorithm takes advantage of airborne measurements of ACAOD acquired from the High Spectral Resolution Lidar-2 (HSRL-2) and Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) sun photometer operated during the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign (September 2016, August 2017, and October 2018) over the southeastern Atlantic Ocean and synergizes them with TOA reflectance from OMI and MODIS to derive spectral SSA in the near-UV (354–388 nm) and VNIR (470–860 nm), respectively. When compared against the ORACLES airborne remote sensing and in situ measurements and the inversion dataset of the ground-based Aerosol Robotic Network (AERONET) over land, the retrieved spectral SSAs from the satellites, on average, were found to be within agreement of ∼ 0.01 – the difference well within the uncertainties involved in all these inversion datasets. The retrieved SSA above the clouds at UV–Vis-NIR wavelengths shows a distinct increasing trend from August to October, which is consistent with the ORACLES in situ measurements, AERONET inversions, and previous findings. The sensitivity analysis quantifying theoretical uncertainties in the retrieved SSA shows that errors in the measured ACAOD, aerosol layer height, and the ratio of the imaginary part of the refractive index (spectral dependence) of aerosols by 20 %, 1 km, and 10 %, respectively, produce an error in the retrieved SSA at 388 nm (470 nm) by 0.017 (0.015), 0.008 (0.002), and 0.03 (0.005). The development of the proposed aerosol–cloud algorithm implies a possible synergy of Cloud–Aerosol Lidar with Orthogonal Polarization (CALIOP) and OMI–MODIS passive sensors to deduce a global product of ACAOD and SSA. Furthermore, the presented synergy algorithm assumes implications for future missions, such as the Atmosphere Observing System (AOS) and the Earth Cloud Aerosol and Radiation Explorer (EarthCARE). The availability of the intended global dataset can help constrain climate models with the much-needed observational estimates of the radiative effects of aerosols in cloudy regions and expand our ability to study aerosol effects on clouds. [ABSTRACT FROM AUTHOR]

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 (Nc) and effective radius reff. However, it produces smaller liquid water path (LWP) and larger Nc 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 Na‐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. Plain Language Summary: Aerosol‐cloud‐interaction (ACI) regulates the energy budget of the Earth and poses the largest uncertainty in climate projection. Particularly, ACI of low clouds is poorly understood and causes the spread of Earth System Models (ESMs) in predicting cloud and climate responses to aerosol changes. Process studies have shown a nonlinear cloud water amount and cloud fraction adjustments due to aerosol changes via precipitation and cloud top entrainment, which are not often captured correctly in ESMs. This study explores the physical mechanisms of ACI in marine low clouds with a focus on precipitating low clouds using a cloud process model and unprecedented field campaign measurements of meteorology states, cloud properties, and aerosols collected during the Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment. We show that the aerosol‐induced cloud water amount adjustment is dominated by changes in precipitation and there is no clear entrainment feedback in both cases. Our findings can help improve the representation of ACI within precipitating marine low clouds in ESMs. Key Points: Aerosol‐cloud interactions in precipitating shallow cumuli are investigated using large‐eddy simulations (LES) and observationsLES show that aerosol‐induced cumulus cloud water adjustment is dominated by precipitation with no clear entrainment feedbackAn increase in cloud fraction in response to aerosol number concentration decrease is shown in the precipitating cumuli [ABSTRACT FROM AUTHOR]

The western North Atlantic Ocean is strongly influenced by continental outflow, making it an ideal region to study the atmospheric transition from a polluted coastline to the marine environment. Utilizing eight transit flights between NASA Langley Research Center (LaRC) in Hampton, Virginia and the remote island of Bermuda from NASA's Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE), we examine the evolution of trace gas and aerosol properties off the U.S. East Coast. The first pair of flights flew along the wind trajectory of continental outflow, while the other flights captured a mix of marine and continental air mass sources. For measurements within the boundary layer (BL), there was an offshore decline in particle N<100 nm, N>100 nm, CH4, CO, and CO2 concentrations, all leveling off around ~900 km offshore from LaRC. These trends are strongest for the first pair of flights. In the BL, offshore declines in organic mass fraction and increases in sulfate mass fraction coincide with increasing hygroscopicity based on f(RH) measurements. Free troposphere measurements show a decline in N<100 nm but other measured parameters are more variable when compared to the prominent offshore gradients seen in the BL. Pollution layers exist in the free troposphere, such as smoke plumes, that can potentially entrain into the BL. This work provides detailed case studies with a broad set of high-resolution measurements to further our understanding of the transition between continental and marine environments. [ABSTRACT FROM AUTHOR]

This paper introduces the new Ocean Derived Column Optical Depth (ODCOD) algorithm. ODCOD is now being used to retrieve column optical depths from the 532 nm measure-ments acquired by the Cloud-Aerosol Lidar with Orthogonal Polari-zation (CALIOP) onboard the Cloud-Aerosol Lidar Infrared Pathfinder Satellite Observations (CALIPSO) spacecraft. ODCOD retrieves total column optical depths using the lidar backscatter signal return from the ocean surface, together with collocated wind speed estimates from Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA‑2). An advantage of ODCOD retrievals is that the column optical depths include contributions from particulates throughout the entire column including regions with attenuated backscatter below the CALIOP layer detection thresholds. In contrast, the standard CALIOP processing only estimates optical depths for clouds and aerosols detected by the CALIOP layer detection scheme. In this paper we describe the ODCOD algorithm, develop uncertainty estimates, and characterize the ODCOD retrievals relative to existing datasets. The paper presents detailed comparisons of ODCOD retrievals to collocated measurements from Langley Research Center's airborne high spectral resolution lidars (HSRL), daytime estimates derived from Moderate Resolution Imaging Spectro-radio-meter (MODIS), and daytime and nighttime optical depths estimates from the Synergized Optical Depth of Aerosols (SODA) algorithm. ODCOD aerosol-only optical depth estimates are higher compared to airborne HSRL measurements by 0.009 ± 0.043 (median ± median absolute deviation) or 6 % ± 27 % relative difference, lower than MODIS by ‑0.009 ± 0.041 (8.0 % ± 34 % relative difference), higher in the daytime than SODA by 0.004 ± 0.035 (12 % ± 34 % relative difference), and higher in the nighttime by 0.027 ± 0.034 (20 % ± 33 % relative difference). In addition to being a new method of retrieving column optical depth, ODCOD's estimates are independent from the standard CALIOP optical depth retrieval algorithms and have potential for further advances in the CALIPSO data record both to validate CALIOP estimates and as a potential column constraint for future improvements to extinction retrievals. [ABSTRACT FROM AUTHOR]

Eighteen long-range flights over the Pacific Ocean between 38° S to 20° N and 166° E to 90° W were made by the NASA DC-8 aircraft during the NASA Pacific Exploratory Mission (PEM) Tropics B conducted from March 6 to April 18, 1999. Two lidar systems were flown on the DC-8 to remotely measure vertical profiles of ozone (O3), water vapor (H2O), aerosols, and clouds from near the surface to the upper troposphere along their flight track. In situ measurements of a wide range of gases and aerosols were made on the DC-8 for comprehensive characterization of the air and for correlation with the lidar remote measurements. The transition from northeasterly flow of Northern Hemispheric (NH) air on the northern side of the Intertropical Convergence Zone (ITCZ) to generally easterly flow of Southern Hemispheric (SH) air south of the ITCZ was accompanied by a significant decrease in O3, carbon monoxide, hydrocarbons, and aerosols and an increase in H2O. Trajectory analyses indicate that air north of the ITCZ came from Asia and/or the United States, while the air south of the ITCZ had a long residence time over the Pacific, perhaps originating over South America several weeks earlier. Air south of the South Pacific Convergence Zone (SPCZ) came rapidly from the west originating over Australia or Africa. This air had enhanced O3 and aerosols and an associated decrease in H2O. Average latitudinal and longitudinal distributions of O3 and H2O were constructed from the remote and in situ O3 and H2O data, and these distributions are compared with results from PEM-Tropics A conducted in August-October 1996. During PEM-Tropics B, low O3 air was found in the SH across the entire Pacific Basin at low latitudes. This was in strong contrast to the photochemically enhanced O3 levels found across the central and eastern Pacific low latitudes during PEM-Tropics A. Nine air mass types were identified for PEM-Tropics B based on their O3, aerosols, clouds, and potential vorticity characteristics. The data from each flight were binned by altitude according to air mass type, and these results showed the relative observational frequency of the different air masses as a function of altitude in seven regions over the Pacific. The average chemical composition of the major air mass types was determined from in situ measurements in the NH and SH, and these results provided insight into the origin, lifetime, and chemistry of the air in these regions. Copyright 2001 by the American Geophysical Union.

Aerosol optical depth was retrieved from two airborne remote sensing instruments, the Research Scanning Polarimeter (RSP) and Second Generation High Spectral Resolution Lidar (HSRL-2), during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE). The field campaign offers a unique opportunity to evaluate an extensive 3-year dataset under a wide range of meteorological conditions from two instruments on the same platform. However, a longstanding issue in atmospheric field studies is that there is a lack of reference datasets for properly validating field measurements and estimating their uncertainties. Here we address this issue by using the triple collocation method, in which a third collocated satellite dataset from the Moderate Resolution Imaging Spectroradiometer (MODIS) is introduced for comparison. HSRL-2 is found to provide a more accurate retrieval than RSP over the study region. The error standard deviation of HSRL-2 with respect to the ground truth is 0.027. Moreover, this approach enables us to develop a simple, yet efficient, quality control criterion for RSP data. The physical reasons for the differences in two retrievals are determined to be cloud contamination, aerosols near surface, multiple aerosol layers, absorbing aerosols, non-spherical aerosols, and simplified retrieval assumptions. These results demonstrate the pathway for optimal aerosol retrievals by combining information from both lidar and polarimeter for future airborne and satellite missions. [ABSTRACT FROM AUTHOR]

This study introduces and evaluates ocean surface wind speed retrieval capabilities of the High Spectral Resolution Lidar – generation 2 (HSRL-2) instrument through comparison with wind speed data collected by National Center for Atmospheric Research (NCAR) Airborne Vertical Atmospheric Profiling System (AVAPS) dropsondes. Wind speed is derived from HSRL-2 measurements of the transmitted laser's specular reflection off the ocean surface. The magnitude of the surface reflectivity is determined by the surface's wave-slope variance, which is driven by surface winds. The assessment relies on the multi-year airborne data set collected as part of NASA's Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) campaign, where HSRL-2 retrievals and AVAPS dropsonde measurements of surface wind speeds were horizontally synchronized owing to their joint deployment on one of two aircraft used during the mission. A total of 577 collocated HSRL-2 - dropsonde surface wind speed data points over the northwest Atlantic Ocean are used for this study. Treating the dropsonde wind speeds as truth, it is found that, through two established wind speed – wave-slope parameterizations, the HSRL-2 wind speed retrievals have small errors (0.15 m s−1 ± 1.80 m s−1 and 0.62 m s−1 ± 1.70 m s−1) and high correlation coefficients (0.89 and 0.88) with dropsonde wind speed measurements. Also, HSRL-2 wind speed error is higher in winter than in summer due at least partly to the higher frequency of low wind speeds and reduced cloud fraction in summer. Two research flights from 28 August 2020 and 1 March 2020 serve as detailed case studies to show the success of the collocation method based on ACTIVATE's spatial-coordination strategy and how HSRL-2 wind speed retrievals can enhance science-oriented studies such as those related to cloud evolution and general air-sea interaction. Another case flight examined from 11 January 2022 demonstrates the challenge of conducting HSRL-2 wind speed retrievals in high cloud fraction conditions. Overall, this study highlights the airborne HSRL-2's ability to retrieve surface wind speeds with accuracy as well as the potential of using dropsondes to validate aircraft instrument data sets within a field campaign. [ABSTRACT FROM AUTHOR]

Due to their fast evolution and large natural variability in macro- and microphysical properties, the accurate representation of boundary layer clouds in current climate models remains a challenge. One of the regions with large intermodel spread in the Coupled Model Intercomparison Project Phase 6 ensemble is the western North Atlantic Ocean. Here, statistically representative in situ measurements can help to develop and constrain the parameterization of clouds in global models. To this end, we performed comprehensive measurements of boundary layer clouds, aerosol, trace gases, and radiation in the western North Atlantic Ocean during the NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) mission. In total, 174 research flights with 574 flight hours for cloud and precipitation measurements were performed with the HU-25 Falcon during three winter (February–March 2020, January–April 2021, and November 2021–March 2022) and three summer seasons (August–September 2020, May–June 2021, and May–June 2022). Here we present a statistical evaluation of 16 140 individual cloud events probed by the fast cloud droplet probe and the two-dimensional stereo cloud probe during 155 research flights in a representative and repetitive flight strategy allowing for robust statistical data analyses. We show that the vertical profiles of distributions of the liquid water content and the cloud droplet effective diameter (ED) increase with altitude in the marine boundary layer. Due to higher updraft speeds, higher cloud droplet number concentrations (Nliquid) were measured in winter compared to summer despite lower cloud condensation nucleus abundance. Flight cloud cover derived from statistical analysis of in situ data is reduced in summer and shows large variability. This seasonal contrast in cloud coverage is consistent with a dominance of a synoptic pattern in winter that favors conditions for the formation of stratiform clouds at the western edge of cyclones (post-cyclonic). In contrast, a dominant summer anticyclone is concomitant with the occurrence of shallow cumulus clouds and lower cloud coverage. The evaluation of boundary layer clouds and precipitation in the Nliquid ED phase space sheds light on liquid, mixed-phase, and ice cloud properties and helps to categorize the cloud data. Ice and liquid precipitation, often masked in cloud statistics by a high abundance of liquid clouds, is often observed throughout the cloud. The ACTIVATE in situ cloud measurements provide a wealth of cloud information useful for assessing airborne and satellite remote-sensing products, for global climate and weather model evaluations, and for dedicated process studies that address precipitation and aerosol–cloud interactions. [ABSTRACT FROM AUTHOR]

Inadequate knowledge about the complex microphysical and optical processes of the aerosol-cloud system severely restricts our ability to quantify the resultant impact on climate. Contrary to the negative radiative forcing (cooling) exerted by aerosols in cloud-free skies over dark surfaces, the absorbing aerosols, when lofted over the clouds, can potentially lead to significant warming of the atmosphere. The sign and magnitude of the aerosol radiative forcing over clouds are determined mainly by the amount of aerosol loading, the absorption capacity of aerosols or single-scattering albedo (SSA), and the brightness of the underlying cloud cover. In the satellite-based algorithms that use measurements from passive sensors, the assumption of aerosol SSA is known to be the largest source of uncertainty in quantifying above-cloud aerosol optical depth (ACAOD). In this paper, we introduce a novel synergy algorithm that combines direct airborne measurements of ACAOD and the top-of-atmosphere (TOA) spectral reflectance from OMI and MODIS sensors of NASA's A-train satellites to retrieve 1) SSA of light-absorbing aerosols lofted over the clouds, and 2) aerosol-corrected cloud optical depth (COD). Radiative transfer calculations show a marked sensitivity of the TOA measurements to ACAOD, SSA, and COD, further suggesting that the availability of accurate ACAOD allows retrieval of SSA for above-cloud aerosols scenes using the 'color ratio' algorithm developed for satellite sensors carrying ultraviolet (UV) and visible-near-IR (VNIR) wavelength bands. The proposed algorithm takes advantage of airborne measurements of ACAOD acquired from the High-spectral Resolution Lidar-2 (HSRL-2) and Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) Sunphotometer operated during the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign (September 2016, August 2017, and October 2018) over the southeastern Atlantic Ocean, and synergize them with TOA reflectance from OMI and MODIS to derive spectral SSA in the near-UV (354-388 nm) and VIS-near-IR (470-860 nm), respectively. When compared against the ORACLES airborne remote sensing and in situ measurements and the inversion dataset of ground-based AERONET over land, the retrieved spectral SSAs from the satellites, on average, were found to be higher overall by ~0.01-0.02--a positive bias still within the uncertainties involved in all these inversion datasets. The sensitivity analysis quantifying theoretical uncertainties in the retrieved SSA shows that errors in the measured ACAOD, aerosol layer height, and the ratio of the imaginary part of the refractive index (spectral dependence) of aerosols by 20%, 1 km, and 10%, respectively, produce an error in the retrieved SSA by 0.017 (0.01), 0.008 (0.001), and 0.03 (0.005) at 388 (470) nm. The development of the proposed aerosol-cloud algorithm implies a possible synergy of CALIOP lidar and OMI-MODIS passive sensors to deduce a global product of ACAOD and SSA. The availability of such global dataset can help constrain the climate models with the much-needed observational estimates of the radiative effects of aerosols in cloudy regions and expand our ability to study aerosol effects on clouds. [ABSTRACT FROM AUTHOR]

Inadequate knowledge about the complex microphysical and optical processes of the aerosol-cloud system severely restricts our ability to quantify the resultant impact on climate. Contrary to the negative radiative forcing (cooling) exerted by aerosols in cloud-free skies over dark surfaces, the absorbing aerosols, when lofted over the clouds, can potentially lead to significant warming of the atmosphere. The sign and magnitude of the aerosol radiative forcing over clouds are determined mainly by the amount of aerosol loading, the absorption capacity of aerosols or single-scattering albedo (SSA), and the brightness of the underlying cloud cover. In the satellite-based algorithms that use measurements from passive sensors, the assumption of aerosol SSA is known to be the largest source of uncertainty in quantifying above-cloud aerosol optical depth (ACAOD). In this paper, we introduce a novel synergy algorithm that combines direct airborne measurements of ACAOD and the top-of-atmosphere (TOA) spectral reflectance from OMI and MODIS sensors of NASA's A-train satellites to retrieve 1) SSA of light-absorbing aerosols lofted over the clouds, and 2) aerosol-corrected cloud optical depth (COD). Radiative transfer calculations show a marked sensitivity of the TOA measurements to ACAOD, SSA, and COD, further suggesting that the availability of accurate ACAOD allows retrieval of SSA for above-cloud aerosols scenes using the 'color ratio' algorithm developed for satellite sensors carrying ultraviolet (UV) and visible-near-IR (VNIR) wavelength bands. The proposed algorithm takes advantage of airborne measurements of ACAOD acquired from the High-spectral Resolution Lidar-2 (HSRL-2) and Spectrometer for Sky-Scanning, Sun-Tracking Atmospheric Research (4STAR) Sunphotometer operated during the ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign (September 2016, August 2017, and October 2018) over the southeastern Atlantic Ocean, and synergize them with TOA reflectance from OMI and MODIS to derive spectral SSA in the near-UV (354–388 nm) and VIS-near-IR (470–860 nm), respectively. When compared against the ORACLES airborne remote sensing and in situ measurements and the inversion dataset of ground-based AERONET over land, the retrieved spectral SSAs from the satellites, on average, were found to be higher overall by ~0.01–0.02—a positive bias still within the uncertainties involved in all these inversion datasets. The sensitivity analysis quantifying theoretical uncertainties in the retrieved SSA shows that errors in the measured ACAOD, aerosol layer height, and the ratio of the imaginary part of the refractive index (spectral dependence) of aerosols by 20 %, 1 km, and 10 %, respectively, produce an error in the retrieved SSA by 0.017 (0.01), 0.008 (0.001), and 0.03 (0.005) at 388 (470) nm. The development of the proposed aerosol-cloud algorithm implies a possible synergy of CALIOP lidar and OMI-MODIS passive sensors to deduce a global product of ACAOD and SSA. The availability of such global dataset can help constrain the climate models with the much-needed observational estimates of the radiative effects of aerosols in cloudy regions and expand our ability to study aerosol effects on clouds. [ABSTRACT FROM AUTHOR]

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 years 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: (a) the ridge regime is associated with a well‐developed anticyclone; (b) the trough‐ridge gives rise to a low‐pressure center over the ocean, ascents, and northerly winds over the coastal zone; (c) trough is associated with the eastward displacement of a cyclone, coastal subsidence, and northerly winds, all representative characteristics of cold‐air outbreaks; and (d) 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 (Nd). The Nd 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 Nd for days identified as trough. This study emphasizes the role of boundary‐layer dynamics and aerosol activation and their roles in modulating cloud microphysics. Plain Language Summary: The synoptic evolution of boundary layer clouds over the western North Atlantic is described by means of a regime classification based on Self‐Organizing Maps. The analysis is able to capture events with low and high low‐cloud coverage. High‐cloud coverage days are associated with cold‐air outbreaks (CAOs). The combination of cold and dry conditions gives rise to an enhancement of surface heat fluxes during CAO, consistent with an increase in cloud fraction. In addition, prevailing winds during CAO days explain the occurrence of a synoptic maximum in cloud droplet number concentration, linked to transport of continental aerosol over the ocean. Overall, the dynamics of midlatitude low clouds substantially differ from archetypal stratocumulus clouds regimes. Key Points: Winter synoptic evolution is well described by a clustering method applied to 600 hPa geopotential heightMarine low clouds are characteristic of the trough regime, associated with strong surface heat fluxesCold‐air outbreaks are associated with trough and ridge–trough regimes, and witness peaks in cloud droplet number and aerosol concentrations [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for the modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, the use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate–nitrate–ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r=0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of the dry effective radius (Reff) for SNA and OM aerosol is designed to represent the airborne measurements (R2=0.74 ; slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2=0.72 ; slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73 and slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Aerosol effects on micro/macrophysical properties of marine stratocumulus clouds over the western North Atlantic Ocean (WNAO) are investigated using in situ measurements and large-eddy simulations (LES) for two cold-air outbreak (CAO) cases (28 February and 1 March 2020) during the Aerosol Cloud Meteorology Interactions over the Western Atlantic Experiment (ACTIVATE). The LES is able to reproduce the vertical profiles of liquid water content (LWC), effective radius reff and cloud droplet number concentration Nc from fast cloud droplet probe (FCDP) in situ measurements for both cases. Furthermore, we show that aerosols affect cloud properties (Nc, reff, and LWC) via the prescribed bulk hygroscopicity of aerosols (κ ¯) and aerosol size distribution characteristics. Nc, reff, and liquid water path (LWP) are positively correlated to κ ¯ and aerosol number concentration (Na) while cloud fractional cover (CFC) is insensitive to κ ¯ and aerosol size distributions for the two cases. The realistic changes to aerosol size distribution (number concentration, width, and the geometrical diameter) with the same meteorology state allow us to investigate aerosol effects on cloud properties without meteorological feedback. We also use the LES results to evaluate cloud properties from two reanalysis products, ERA5 and MERRA-2. Compared to LES, the ERA5 is able to capture the time evolution of LWP and total cloud coverage within the study domain during both CAO cases while MERRA-2 underestimates them. [ABSTRACT FROM AUTHOR]

Accurately capturing cloud condensation nuclei (CCN) concentrations is key to understanding the aerosol–cloud interactions that continue to feature the highest uncertainty amongst numerous climate forcings. In situ CCN observations are sparse, and most non-polarimetric passive remote sensing techniques are limited to providing column-effective CCN proxies such as total aerosol optical depth (AOD). Lidar measurements, on the other hand, resolve profiles of aerosol extinction and/or backscatter coefficients that are better suited for constraining vertically resolved aerosol optical and microphysical properties. Here we present relationships between aerosol backscatter and extinction coefficients measured by the airborne High Spectral Resolution Lidar 2 (HSRL-2) and in situ measurements of CCN concentrations. The data were obtained during three deployments in the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project, which took place over the southeast Atlantic (SEA) during September 2016, August 2017, and September–October 2018. Our analysis of spatiotemporally collocated in situ CCN concentrations and HSRL-2 measurements indicates strong linear relationships between both data sets. The correlation is strongest for supersaturations (S) greater than 0.25 % and dry ambient conditions above the stratocumulus deck, where relative humidity (RH) is less than 50 %. We find CCN–HSRL-2 Pearson correlation coefficients between 0.95–0.97 for different parts of the seasonal burning cycle that suggest fundamental similarities in biomass burning aerosol (BBA) microphysical properties. We find that ORACLES campaign-average values of in situ CCN and in situ extinction coefficients are qualitatively similar to those from other regions and aerosol types, demonstrating overall representativeness of our data set. We compute CCN–backscatter and CCN–extinction regressions that can be used to resolve vertical CCN concentrations across entire above-cloud lidar curtains. These lidar-derived CCN concentrations can be used to evaluate model performance, which we illustrate using an example CCN concentration curtain from the Weather Research and Forecasting Model coupled with physics packages from the Community Atmosphere Model version 5 (WRF-CAM5). These results demonstrate the utility of deriving vertically resolved CCN concentrations from lidar observations to expand the spatiotemporal coverage of limited or unavailable in situ observations. [ABSTRACT FROM AUTHOR]

Recently, we successfully demonstrated a new compact and robust ozone DIAL lidar for smaller aircraft such as the NASA B200 and the ER-2 high-altitude aircraft. This is the first NASA airborne lidar to incorporate advanced solid-state lasers to produce the required power at the required ultraviolet wavelengths, and is compact and robust enough to operate nearly autonomously on the high-altitude ER-2 aircraft. This technology development resulted in the first new NASA airborne ozone DIAL instrument in more than 15 years. The combined ozone, aerosol, and clouds measurements provide valuable information on the chemistry, radiation, and dynamics of the atmosphere. In particular, from the ER-2 it offers a unique capability to study the upper troposphere and lower stratosphere.

Biomass burning aerosol impacts aspects of the atmosphere and Earth system through direct and semi-direct effects, as well as influencing air quality. Despite its importance, the representation of biomass burning aerosol is not always accurate in numerical weather prediction and climate models or reanalysis products. Using observations collected as part of the Cloud, Aerosol and Monsoon Processes Philippines Experiment (CAMP 2 Ex) in August through October of 2019, aerosol concentration and optical properties are evaluated within the Goddard Earth Observing System (GEOS) and its underlying aerosol module, GOCART. In the operational configuration, GEOS assimilates aerosol optical depth observations at 550 nm from AERONET and MODIS to constrain aerosol fields. Particularly for biomass burning aerosol, without the assimilation of aerosol optical depth, aerosol extinction is underestimated compared to observations collected in the Philippines region during the CAMP 2 Ex campaign. The assimilation process adds excessive amounts of carbon to account for the underestimated extinction, resulting in positive biases in the mass of black and organic carbon, especially within the boundary layer, relative to in situ observations from the Langley Aerosol Research Group Experiment. Counteracting this, GEOS is deficient in sulfate and nitrate aerosol just above the boundary layer. Aerosol extinction within GEOS is a function of the mass of different aerosol species, the ambient relative humidity, the assumed spectral optical properties, and particle size distribution per species. The relationship between dry and ambient extinction in GEOS reveals that hygroscopic growth is too high within the model for biomass burning aerosol. An additional concern lies in the assumed particle size distribution for GEOS, which has a single mode radius that is too small for organic carbon. Variability in the observed particle size distribution for biomass burning aerosol within a single flight also illuminates the fact that a single assumed particle size distribution is not sufficient and that for a proper representation, a more advanced aerosol module within GEOS may be necessary. [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate-nitrate-ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r = 0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM, and the ratio between the two components (OM/SNA) are the major indicators for SNA and OM dry aerosol size. A parameterization of dry effective radius (Reff) for SNA and OM aerosol is proposed, which well represents the airborne measurements (R² = 0.74, slope = 1.00) and the GEOS-Chem-TOMAS simulation (R² = 0.72, slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R² from 0.68 to 0.73, slope from 0.75 to 34 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Accurate representation of aerosol optical properties is essential for modeling and remote sensing of atmospheric aerosols. Although aerosol optical properties are strongly dependent upon the aerosol size distribution, use of detailed aerosol microphysics schemes in global atmospheric models is inhibited by associated computational demands. Computationally efficient parameterizations for aerosol size are needed. In this study, airborne measurements over the United States (DISCOVER-AQ) and South Korea (KORUS-AQ) are interpreted with a global chemical transport model (GEOS-Chem) to investigate the variation in aerosol size when organic matter (OM) and sulfate-nitrate-ammonium (SNA) are the dominant aerosol components. The airborne measurements exhibit a strong correlation (r = 0.83) between dry aerosol size and the sum of OM and SNA mass concentration (MSNAOM). A global microphysical simulation (GEOS-Chem-TOMAS) indicates that MSNAOM, and the ratio between the two components are the major indicators for SNA and OM dry aerosol size. A parameterization of dry effective radius (Reff) for SNA and OM aerosol is proposed, which well represents the airborne measurements (R2 = 0.74, slope = 1.00) and the GEOS-Chem-TOMAS simulation (R2 = 0.72, slope = 0.81). When applied in the GEOS-Chem high-performance model, this parameterization improves the agreement between the simulated aerosol optical depth (AOD) and the ground-measured AOD from the Aerosol Robotic Network (AERONET; R2 from 0.68 to 0.73, slope from 0.75 to 0.96). Thus, this parameterization offers a computationally efficient method to represent aerosol size dynamically. [ABSTRACT FROM AUTHOR]

Accurately capturing cloud condensation nuclei (CCN) concentrations is key to understanding the aerosol-cloud interactions that continue to feature the highest uncertainty amongst numerous climate forcings. In situ CCN observations are sparse and most non-polarimetric passive remote sensing techniques are limited to providing column-effective CCN proxies such as total aerosol optical depth (AOD). Lidar measurements, on the other hand, resolve profiles of aerosol extinction and/or backscatter coefficients that are better suited for constraining vertically-resolved aerosol optical and microphysical properties. Here we present relationships between aerosol backscatter and extinction coefficients measured by the airborne High Spectral Resolution Lidar 2 (HSRL-2) and in situ measurements of CCN concentrations. The data were obtained during three deployments in the NASA ObseRvations of Aerosols above Clouds and their intEractionS (ORACLES) project, which took place over the Southeast Atlantic (SEA) during September 2016, August 2017, and September-October 2018. Our analysis of spatiotemporally collocated in situ CCN concentrations and HSRL-2 measurements indicates strong linear relationships between both data sets. The correlation is strongest for supersaturations greater than 0.25% and dry ambient conditions above the stratocumulus deck, where relative humidity (RH) is less than 50%. We find CCN - HSRL-2 Pearson correlation coefficients between 0.95-0.97 for different parts of the seasonal burning cycle that suggest fundamental similarities in biomass burning aerosol (BBA) microphysical properties. We find that ORACLES campaign-average values of in situ CCN and in situ extinction coefficients are qualitatively similar to those from other regions and aerosol types, demonstrating overall representativeness of our data set. We compute CCN - backscatter and CCN - extinction regressions that can be used to resolve vertical CCN concentrations across entire above-cloud lidar curtains. These lidar-derived CCN concentrations can be used to evaluate model performance, which we illustrate using an example CCN concentration curtain from WRF-CAM5. These results demonstrate the utility of deriving vertically-resolved CCN concentrations from lidar observations to expand the spatiotemporal coverage of limited or unavailable in situ observations. [ABSTRACT FROM AUTHOR]

Monitoring and modeling aerosol particle life cycle in Southeast Asia (SEA) is challenged by high cloud cover, complex meteorology, and the wide range of aerosol species, sources, and transformations found throughout the region. Satellite observations are limited, and there are few in situ observations of aerosol extinction profiles, aerosol properties, and environmental conditions. Therefore, accurate aerosol model outputs are crucial for the region. This work evaluates the Navy Aerosol Analysis and Prediction System Reanalysis (NAAPS-RA) aerosol optical thickness (AOT) and light extinction products using airborne aerosol and meteorological measurements from the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP 2 Ex) conducted in 2019 during the SEA southwest monsoon biomass burning season. Modeled AOTs and extinction coefficients are compared to those retrieved with a high spectral resolution lidar (HSRL-2). Agreement between simulated and retrieved AOT (R2= 0.78, relative bias =- 5 %, normalized root mean square error (NRMSE) = 48 %) and aerosol extinction coefficients (R2= 0.80, 0.81, and 0.42; relative bias = 3 %, -6 %, and -7 %; NRMSE = 47 %, 53 %, and 118 % for altitudes between 40–500, 500–1500, and >1500 m, respectively) is quite good considering the challenging environment and few opportunities for assimilations of AOT from satellites during the campaign. Modeled relative humidities (RHs) are negatively biased at all altitudes (absolute bias =-5 %, -8 %, and -3 % for altitudes <500 500–1500 and >1500 m, respectively), motivating interest in the role of RH errors in AOT and extinction simulations. Interestingly, NAAPS-RA AOT and extinction agreement with the HSRL-2 does not change significantly (i.e., NRMSE values do not all decrease) when RHs from dropsondes are substituted into the model, yet biases all move in a positive direction. Further exploration suggests changes in modeled extinction are more sensitive to the actual magnitude of both the extinction coefficients and the dropsonde RHs being substituted into the model as opposed to the absolute differences between simulated and measured RHs. Finally, four case studies examine how model errors in RH and the hygroscopic growth parameter, γ , affect simulations of extinction in the mixed layer (ML). We find NAAPS-RA overestimates the hygroscopicity of (i) smoke particles from biomass burning in the Maritime Continent (MC) and (ii) anthropogenic emissions transported from East Asia. This work mainly provides insight into the relationship between errors in modeled RH and simulations of AOT and extinction in a humid and tropical environment influenced by a myriad of meteorological conditions and particle types. These results can be interpreted and addressed by the modeling community as part of the effort to better understand, quantify, and forecast atmospheric conditions in SEA. [ABSTRACT FROM AUTHOR]

We assess the CALIPSO Version 4.2 (V4) aerosol typing and assigned lidar ratios over ocean using aerosol optical depth (AOD) retrievals from the Synergized Optical Depth of Aerosols (SODA) algorithm and retrieved columnar lidar ratio estimated by combining SODA AOD and CALIPSO attenuated backscatter (CALIPSO–SODA). Six aerosol types – clean marine, dusty marine, dust, polluted continental/smoke, polluted dust, and elevated smoke – are characterized using CALIPSO–SODA over ocean and the results are compared against the prescribed V4 lidar ratios, when only one aerosol type is present in the atmospheric column. For samples detected at 5 or 20 km spatial resolutions and having AOD > 0.05, the CALIPSO–SODA lidar ratios are significantly different between different aerosol types, and are consistent with the type-specific values assigned in V4 to within 10 sr (except for polluted continental/smoke). This implies that the CALIPSO classification scheme generally categorizes specific aerosols types correctly over regions where they are abundant. We find remarkable daytime/nighttime regional agreement for clean marine aerosol over the open ocean (CALIPSO–SODA = 20–25 sr, V4 = 23 sr), elevated smoke over the southeast Atlantic (CALIPSO–SODA = 65–75 sr, V4 = 70 sr), and dust over the subtropical Atlantic adjacent to the African continent (CALIPSO–SODA = 40–50 sr, V4 = 44 sr). In contrast, daytime polluted continental/smoke lidar ratio is more than 20 sr smaller than the constant V4 value for that type, attributed in part to the challenge of classifying tenuous aerosol with low signal-to-noise ratio. Dust over most of the Atlantic Ocean features CALIPSO–SODA lidar ratios less than 40 sr, possibly suggesting the presence of dust mixed with marine aerosols or lidar ratio values that depend on source and evolution of the aerosol plume. The new dusty marine type introduced in V4 features similar magnitudes and spatial distribution as its clean marine counterpart with lidar ratio differences of less than 3 sr, and nearly identical values over the open ocean, implying that some modification of the classification scheme for the marine subtypes is warranted. [ABSTRACT FROM AUTHOR]

The Lidar Atmospheric Sensing Experiment (LASE) on board the NASA DC-8 measured high-resolution profiles of water vapor and aerosols, and cloud distributions in 14 flights over the eastern North Atlantic during the NASA African Monsoon Multidisciplinary Analyses (NAMMA) field experiment. These measurements were used to study African easterly waves (AEWs), tropical cyclones (TCs), and the Saharan air layer (SAL). These LASE measurements represent the first simultaneous water vapor and aerosol lidar measurements to study the SAL and its interactions with AEWs and TCs. Three case studies were selected for detailed analysis: (i) a stratified SAL, with fine structure and layering (unlike a well-mixed SAL), (ii) a SAL with high relative humidity (RH), and (iii) an AEW surrounded by SAL dry air intrusions. Profile measurements of aerosol scattering ratios, aerosol extinction coefficients, aerosol optical thickness, water vapor mixing ratios, RH, and temperature are presented to illustrate their characteristics in the SAL, convection, and clear air regions. LASE extinction-to-backscatter ratios for the dust layers varied from 35 [+ or -] 5 to 45 [+ or -] 5 sr, well within the range of values determined by other lidar systems. LASE aerosol extinction and water vapor profiles are validated by comparison with onboard in situ aerosol measurements and GPS dropsonde water vapor soundings, respectively. An analysis of LASE data suggests that the SAL suppresses low-altitude convection. Midlevel convection associated with the AEW and transport are likely responsible for high water vapor content observed in the southern regions of the SAL on 20 August 2008. This interaction is responsible for the transfer of about 7 x [10.sup.15] J (or 8 x [10.sup.3] J [m.sup.-2]) latent heat energy within a day to the SAL. Initial modeling studies that used LASE water vapor profiles show sensitivity to and improvements in model forecasts of an AEW. DOI: 10.1175/2009JAS3136.1

The Atmospheric Radiation Measurement program Raman lidar was upgraded in 2004 with a new data system that provides simultaneous measurements of both the photomultiplier analog output voltage and photon counts. We describe recent improvements to the algorithm used to merge these two signals into a single signal with improved dynamic range. The effect of modifications to the algorithm are evaluated by comparing profiles of water vapor mixing ratio from the lidar with radiosonde measurements over a six month period. The modifications that were implemented resulted in a reduction of the mean bias in the daytime water vapor mixing ratio from a 3% dry bias to well within 1%. This improvement was obtained by ignoring the temporal variation of the glue coefficients and using only the nighttime average glue coefficients throughout the entire diurnal cycle. OCIS codes: 010.3640, 010.7340, 040.5250, 280.3640, 290.5860, 120.0280.

Biomass burning in southwestern Africa produces smoke plumes that are transported over the Atlantic Ocean and overlie vast regions of stratocumulus clouds. This aerosol layer contributes to direct and indirect radiative forcing of the atmosphere in this region particularly during the months of August, September, and October. There was a multi-year international campaign to study this aerosol and its interactions with clouds. Here, we report on the evolution of aerosol distributions and properties as measured by the airborne high spectral resolution lidar (HSRL-2) during the ORACLES (Observations of Aerosols above Clouds and their intEractionS) campaign in September 2016. The NASA Langley HSRL-2 instrument was flown on the NASA ER-2 aircraft for several days in September 2016. Data were aggregated at two pairs of 2 ∘ × 2 ∘ grid boxes to examine the evolution of the vertical profile of aerosol properties during transport over the ocean. Results showed that the structure of the profile of aerosol extinction and microphysical properties is maintained over a 1 to 2 d timescale. In the 3–5 km altitude range, 95 % of the aerosol extinction was contributed by particles in the 0.05–0.50 µm radius size range with the aerosol in this size range having an average effective radius of 0.16 µm. This indicates that there is essentially no scavenging or dry deposition at these altitudes. Moreover, there is very little day-to-day variation in these properties, such that time sampling as happens in such campaigns may be representative of longer periods such as monthly means. Below 3 km, there is considerable mixing with larger aerosol, most likely continental source near land. Furthermore, these measurements indicated that there was often a distinct gap between the bottom of the aerosol layer and cloud tops at the selected locations as evidenced by a layer of several hundred meters that contained relatively low aerosol extinction values above the clouds. [ABSTRACT FROM AUTHOR]

To determine the impact of dynamic and aerosol processes on marine low clouds, we examine the seasonal impact of updraft speed w and cloud condensation nuclei concentration at 0.43 % supersaturation (NCCN0.43%) on the cloud droplet number concentration (NC) of low-level clouds over the western North Atlantic Ocean. Aerosol and cloud properties were measured with instruments on board the NASA LaRC Falcon HU-25 during the ACTIVATE (Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment) mission in summer (August) and winter (February–March) 2020. The data are grouped into different NCCN0.43% loadings, and the density functions of NC and w near the cloud bases are compared. For low updrafts (w < 1.3 ms-1), NC in winter is mainly limited by the updraft speed and in summer additionally by aerosols. At larger updrafts (w > 3 ms-1), NC is impacted by the aerosol population, while at clean marine conditions cloud nucleation is aerosol-limited, and for high NCCN0.43% it is influenced by aerosols and updraft. The aerosol size distribution in winter shows a bimodal distribution in clean marine environments, which transforms to a unimodal distribution in high NCCN0.43% due to chemical and physical aerosol processes, whereas unimodal distributions prevail in summer, with a significant difference in their aerosol concentration and composition. The increase of NCCN0.43% is accompanied with an increase of organic aerosol and sulfate compounds in both seasons. We demonstrate that NC can be explained by cloud condensation nuclei activation through upwards processed air masses with varying fractions of activated aerosols. The activation highly depends on w and thus supersaturation between the different seasons, while the aerosol size distribution additionally affects NC within a season. Our results quantify the seasonal influence of w and NCCN0.43% on NC and can be used to improve the representation of low marine clouds in models. [ABSTRACT FROM AUTHOR]

A compact, highly robust airborne High Spectral Resolution Lidar (HSRL) that provides measurements of aerosol backscatter and extinction coefficients and aerosol depolarization at two wavelengths has been developed, tested, and deployed on nine field experiments (over 650 flight hours). A unique and advantageous design element of the HSRL system is the ability to radiometrically calibrate the instrument internally, eliminating any reliance on vicarious calibration from atmospheric targets for which aerosol loading must be estimated. This paper discusses the design of the airborne HSRL, the internal calibration and accuracy of the instrument, data products produced, and observations and calibration data from the first two field missions: the Joint Intercontinental Chemical Transport Experiment--Phase B (INTEX-B)/Megacity Aerosol Experiment--Mexico City (MAX-Mex)/Megacities Impacts on Regional and Global Environment (MILAGRO) field mission (hereafter MILAGRO) and the Gulf of Mexico Atmospheric Composition and Climate Study/Texas Air Quality Study II (hereafter GoMACCS/TexAQS II). OCIS codes: 010.0010, 010.1110, 280.0280, 280.1100, 280.1310, 280.3640.

We present the results of a comparison study in which a simple, automated, and unsupervised algorithm, which we call the arrange and average algorithm, was used to infer microphysical parameters (complex refractive index (CRI), effective radius, total number, surface area, and volume concentrations) of atmospheric aerosol particles. The algorithm normally uses backscatter coefficients (β) at 355, 532, and 1064 nm and extinction coefficients (α) at 355 and 532 nm as input information. We compared the performance of the algorithm for the existing “3β+α” and potential “3β+3α” configurations of a multiwavelength aerosol Raman lidar or highspectral-resolution lidar (HSRL). The “3β+3α” configuration uses an extra extinction coefficient at 1064 nm. Testing of the algorithm is based on synthetic optical data that are computed from prescribed CRIs and monomodal logarithmically normal particle size distributions that represent spherical, primarily fine mode aerosols. We investigated the degree to which the microphysical results retrieved by this algorithm benefits from the increased number of input extinction coefficients.

The combination of backscatter coefficients measured at 355, 532 and 1064 nm and extinction coefficients at 355 and 532 nm (i.e. 3β+2α) can be used to retrieve profiles of optical and microphysical properties of aerosols, such as effective radius, total volume concentration and total number concentration. NASA LaRC HSRL-2 is an airborne multi-wavelength high spectral resolution lidar in operation that provides the full 3β+2α dataset. HSRL-2 was deployed during DISCOVER-AQ along with other airborne and ground-based instruments that also measured many aerosol parameters in close proximity to the HSRL-2 system, allowing us to evaluate the performance of an automated and unsupervised retrieval algorithm that has been recently developed. We present the results from California (Jan/Feb 2013) and Texas (Sep 2013) DISCOVER-AQ.