Abstract. While most large-scale smoke advection occurs within the free troposphere, Maritime Continent smoke transport is suspected to be unique in its long-range, near-surface transport. Such a pathway likely creates strong gradients and uncertainties in interpreting satellite and model data on light extinction, air pollution, and cloud condensation nuclei. This paper documents High Spectral Resolution Lidar (HSRL) data from the 2019 ONR PISTON cruise and NASA CAMP2Ex flights that revealed Maritime Continent smoke and pollution transport pathways and heterogeneity around the Marine Atmospheric Boundary Layer (MABL) over thousands of kilometers. Observations showed that 95 % of integrated aerosol backscatter occurred below 2500 m altitude. The R/V Sally Ride observed 50th and 84th percentile aerosol backscatter altitudes at ~600 and ~1500 m respectively, regardless of aerosol loading. Peak backscatter values occurred within or near the MABL top, diminishing as we approached 2–3 km altitude, but with occasional plumes reaching the melting level at 4800 m. At monsoonal scales, aerosol models largely account for the observed directional wind shear that causes altitude-dependent particle transport: near-surface particles remain in the core monsoon flow around the MABL, while at lower latitudes, aerosol layers aloft advect more eastwardly. Around the MABL, however, significant cloud-scale variability exists due to fine-scale flow, halo-entrainment-detrainment, and cold pool phenomena. Backscatter enhancements beneath individual clouds, extending to the ocean surface, likely relate to MABL-free troposphere exchange and air-sea interaction. So while aerosol transport occurs near the surface, particle extinction heterogeneity must still be considered for in situ observations and satellite retrievals.

While most large-scale smoke advection occurs within the free troposphere, Maritime Continent smoke is suspected to be unique in its long-range, near-surface transport. Such a pathway likely creates strong gradients and uncertainties in interpreting satellite and model data on light extinction, air pollution, and cloud condensation nuclei. This paper documents High Spectral Resolution Lidar (HSRL) data from the 2019 ONR PISTON cruise and NASA CAMP2Ex flights that revealed Maritime Continent smoke and pollution transport pathways and heterogeneity around the Marine Atmospheric Boundary Layer (MABL) over thousands of kilometers. Observations showed that 95 % of integrated aerosol backscatter occurred below 2500 m altitude. The R/V Sally Ride observed 50th and 84th percentile aerosol backscatter altitudes at ∼600 and ∼1500 m respectively, regardless of aerosol loading. Peak backscatter values occurred within or near the MABL top, diminishing as we approached 2–3 km altitude, but with occasional plumes reaching the melting level at 4800 m. At monsoonal scales, aerosol models largely account for the observed directional wind shear that causes altitude-dependent particle transport: near-surface particles remain in the core monsoon flow around the MABL, while at lower latitudes, aerosol layers aloft advect more eastwardly. Around the MABL, however, significant cloud-scale variability exists due to fine-scale flow, halo-entrainment-detrainment, and cold pool phenomena. Backscatter enhancements beneath individual clouds, extending to the ocean surface, likely relate to MABL-free troposphere exchange and air-sea interaction. So while aerosol transport occurs near the surface, particle extinction heterogeneity must still be considered for in situ observations and satellite retrievals.

The High-Spectral-Resolution Lidar (HSRL) Pathfinder Mission concept is designed to provide HSRL measurements at 532 nm and elastic backscatter lidar measurements at 1064 nm. The instrument is based on Clio, the HSRL that was descoped from NASA's Atmosphere Observing System (AOS) mission due to cost constraints. The NASA Langley Research Center (LaRC) developed the HSRL Pathfinder concept as an example of a lower-cost mission to advance the technology and demonstrate the measurement capability originally planned for AOS. Cost savings are achieved via a Class-D instrument development approach and some reductions in performance from the original Clio design. Despite these changes, the HSRL Pathfinder Mission promises to provide valuable observations for advancing studies of aerosol and cloud radiative effects, cloud microphysics, aerosol-cloud interaction, aerosol transport and speciation, and air quality. The design also enables scientifically important observations of depth-resolved ocean subsurface optical properties, snow water equivalent, and seasonal sea ice, making HSRL Pathfinder a truly multifunctional lidar mission.

Fine particulate matter (PM2.5) concentrations in Metro Manila, Philippines have consistently exceeded the guideline values set by the World Health Organization (WHO). Although there has been much progress in understanding the components and sources of PM2.5, limited research has been done on the influence of meteorological factors. In particular, the influence of the planetary boundary layer height (PBLH) on PM2.5 concentration has not been studied due to inadequate observations. From January 2019–June 2020, measurements from a High Spectral Resolution Lidar (HSRL) filled this gap and allowed for PBLH estimation and aerosol typing. This paper investigates the roles of PBLH and regional and local wind circulations on the temporal evolution of aerosol pollution. Results show that daytime and nighttime PBLH variability is associated with solar heating and radiative cooling, respectively. Cloud-free conditions during the dry season yield a higher PBL growth rate than during the wet season when lower daytime and elevated nighttime PBLH are observed. Lower PM2.5 levels are generally observed during daytime when PBLH is at its maximum. However, the PBLH has a significant inverse correlation with PM2.5 only in the months of December-January-February. We find that horizontal directional wind shear between synoptic and mesoscale circulations confounds the PM2.5 - PBLH relationship by creating stagnant conditions conducive to aerosol accumulation. The lower 20% of PM2.5 concentrations occur during the prevalence of strong monsoon winds. On the other hand, the upper 80% are found during the occurrence of compound mesoscale winds (i.e., sea/land/lake/valley/mountain breezes and channeling monsoon winds). In addition, mountain breeze is found to be associated with lifting of aerosols, resulting in multi-layering within the PBL. The findings in the present study emphasize the role of complex topography and mesoscale scale winds arising from the landscape on aerosol pollution variability.

The performance of a model field-widened Michelson interferometer (FWMI) as the spectral discriminator for a 1064-nm high-spectral resolution lidar (HSRL) channel is presented. The technique of HSRL separates the Doppler-broadened molecular backscatter from the narrow Mie scattering from atmospheric aerosols using a fine-tuned narrowband filter or spectral discriminator. Our simulated FWMI consists of one glass arm and one air spaced arm with a composite metal spacer designed to make the interferometer thermally invariant. The FWMI is pressure tuned to the desired wavelength.

We present our prototype for a semiconductor-based high-spectral-resolution LiDAR (HSRL) system with a simplified optical setup. Traditionally, HSRL systems split the received signal into two channels: one channel measures the molecular backscatter, and the other channel measures both molecular and aerosol backscatters. An etalon or molecular vapor absorption line is used to separate out the narrow aerosol spectrum from the Doppler broadened molecular backscatter. By modulating our seed laser between the center of a rubidium absorption line and just off the absorption line, we are able to combine both HSRL channels into a single physical optical path.

The NASA Langley Research Center (LaRC) has designed the Clio High Spectral Resolution Lidar (HSRL) instrument concept for NASA's Atmosphere Observing System (AOS). The AOS mission is being developed by NASA in response to the National Academy of Sciences Decadal Survey for Earth Observations from Space and addresses two of five core science foci recommended through the Decadal Survey process: a focus on aerosol impacts on climate and air quality and a focus on global hydrological cycle and cloud-climate feedbacks. The AOS mission implementation, which follows the NASA Aerosol-Cloud-Convection-Precipitation (ACCP) Study recommendations, includes several instruments deployed in two orbital planes, one inclined and one polar. Clio is designed for deployment to the polar orbital plane along with a Doppler radar, microwave radiometer, polarimeter, long-wave IR imaging radiometer, and aerosol and water vapor limb sounders and contributes to both the aerosol and cloud science foci of the mission. Clio capabilities would provide major advances in aerosol and cloud measurements over those available from past spaceborne cloud/aerosol lidars in terms of accuracy, precision, sensitivity, and information content.

Continuous measurements of aerosol extinction coefficient ( σ ext ) from the High Spectral Resolution Lidar (HSRL) in Seoul from 2016 to 2018 were used to investigate the diurnal variation of the aerosol optical depth (AOD). Nighttime AOD displayed a larger mean and standard deviation (0.45 ± 0.47) than daytime (0.40 ± 0.29). Hygroscopic growth of aerosols under humid conditions was a key factor in the relative enhancement of nighttime AOD. Taking advantage of the HSRL's vertically resolved measurements, the contribution of aerosols within the boundary layer (BL) and free troposphere (FT) to AOD and its temporal variation were investigated. Unlike the diurnal AOD variation, AOD within the BL (AOD BL ) showed similar diurnal variations with the mixing layer height (MLH), displaying lower nighttime values with a peak around 14–15 local standard time. However, the low correlation between MLH and AOD BL ( R 2 = 0.06) implied that MLH was not the sole deterministic factor of AOD BL . A larger AOD of FT aerosols (AOD FT ) was observed during spring due to frequent elevated dust layers. Using mean σ ext within the BL and surface PM 10 concentrations, the mass extinction efficiency (MEE) of aerosols in Seoul was estimated. The PM 10 MEE showed a mean of 5.40 g m −2 and displayed significant variability by PM 2.5 to PM 10 ratio, season, and ambient relative humidity. The uncertainty of estimated surface PM 10 concentrations was minimized when the seasonality and humidity factor in MEE were taken into account (the normalized mean bias decreased from 10.6%, using a single MEE value, to 6.2%).

Ground-based thermodynamic and kinematic profilers were placed adjacent to the western shore of Lake Michigan at two sites as part of the 2017 LakeMichigan Ozone Study. The southern site near Zion, Illinois, hosted a microwave radiometer (MWR) and a sodar wind profiler, while the northern site in Sheboygan, Wisconsin, featured an Atmospheric Emitted Radiance Interferometer (AERI), a Doppler lidar, and a High Spectral Resolution Lidar (HSRL). Each site experienced several lake-breeze events during the experiment. Composite time series and time-height cross sections were constructed relative to the lake-breeze arrival time so that commonalities across events could be explored. The composited surface observations indicate that the wind direction of the lake breeze was consistently southeasterly at both sites regardless of its direction before the arrival of the lake-breeze front. Surface relative humidity increased with the arriving lake breeze, though this was due to cooler air temperatures as absolute moisture content stayed the same or decreased. The profiler observations show that the lake breeze penetrated deeper when the local environment was unstable and preexisting flow was weak. The cold air associated with the lake breeze remained confined to the lowest 200 m of the troposphere even if the wind shift was observed at higher altitudes. The evolution of the lake breeze corresponded well to observed changes in baroclinicity and calculated changes in circulation. Collocated observations of aerosols showed increases in number and mass concentrations after the passage of the lake-breeze front.

A record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019–May 2020) and over Punta Arenas in southern Chile at 53.2∘ S (January 2020–November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10–12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10–12 km, smoke particle surface area (SA) concentrations of 5–7 µm2 cm−3 (Antarctica, spring 2021) and 6–10 µm2 cm−3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4–1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2–3.5 mPa (Arctic, 20 %–30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1–2 mPa (10 %–20 % contribution to the total ozone loss over Antarctica) was observed in the 14–23 km PSC height range in September–October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm−3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26–30 Dobson units (9 %–10 %, September 2020, 2021) and 52–57 Dobson units (17 %–20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70–80∘ S.

Fireworks degrade air quality, reduce visibility, alter atmospheric chemistry, and cause short-term adverse health effects. However, there have not been any comprehensive physicochemical and optical measurements of fireworks and their associated impacts in a Southeast Asia megacity, where fireworks are a regular part of the culture. Size-resolved particulate matter (PM) measurements were made before, during, and after New Year 2019 at the Manila Observatory in Quezon City, Philippines, as part of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex). A high-spectral-resolution lidar (HSRL) recorded a substantial increase in backscattered signal associated with high aerosol loading ∼440 m above the surface during the peak of firework activities around 00:00 (local time). This was accompanied by PM2.5 concentrations peaking at 383.9 µg m−3. During the firework event, water-soluble ions and elements, which affect particle formation, growth, and fate, were mostly in the submicrometer diameter range. Total (>0.056 µm) water-soluble bulk particle mass concentrations were enriched by 5.7 times during the fireworks relative to the background (i.e., average of before and after the firework). The water-soluble mass fraction of PM2.5 increased by 18.5 % above that of background values. This corresponded to increased volume fractions of inorganics which increased bulk particle hygroscopicity, kappa (κ), from 0.11 (background) to 0.18 (fireworks). Potassium and non-sea-salt (nss) SO42- contributed the most (70.9 %) to the water-soluble mass, with their mass size distributions shifting from a smaller to a larger submicrometer mode during the firework event. On the other hand, mass size distributions for NO3-, Cl−, and Mg2+ (21.1 % mass contribution) shifted from a supermicrometer mode to a submicrometer mode. Being both uninfluenced by secondary aerosol formation and constituents of firework materials, a subset of species were identified as the best firework tracer species (Cu, Ba, Sr, K+, Al, and Pb). Although these species (excluding K+) only contributed 2.1 % of the total mass concentration of water-soluble ions and elements, they exhibited the highest enrichments (6.1 to 65.2) during the fireworks. Surface microscopy analysis confirmed the presence of potassium/chloride-rich cubic particles along with capsule-shaped particles in firework samples. The results of this study highlight how firework emissions change the physicochemical and optical properties of water-soluble particles (e.g., mass size distribution, composition, hygroscopicity, and aerosol backscatter), which subsequently alters the background aerosol's respirability, influence on surroundings, ability to uptake gases, and viability as cloud condensation nuclei (CCN).

This study focuses on the accuracy of longwave radiation flux retrievals at the top and bottom of the atmosphere at Eureka station, Canada, in the high Arctic. We report comparisons between seven products derived from (a) calculations based on a combination of ground‐based and space‐based lidar and radar observations, (b) standard radiometric observations from the CERES sensor, (c) direct observations at the surface from a broadband radiation station, and (d) the ERA‐Interim and ERA5 reanalyzes. Statistical, independent analyses are first performed to look at recurring bias and trends in fluxes at Top and Bottom of the Atmosphere (TOA, BOA). The analysis is further refined by comparing fluxes derived from coincident observations decomposed by scene types. Results show that radiative transfer calculations using ground‐based lidar‐radar profiles derived at Eureka agree well with TOA LW fluxes observed by CERES and with BOA LW fluxes reference. CloudSat‐CALIPSO also shows good agreement with calculations from ground‐based sensor observations, with a relatively small bias. This bias is shown to be largely due to low and thick cloud occurrences that the satellites are insensitive to owing to attenuation from clouds above and surface clutter. These conditions of opaque low clouds, cause an even more pronounced bias for CERES BOA flux calculation in winter, due to the deficit of low clouds identified by MODIS. ERA‐I and ERA5 fluxes behave differently, the large positive bias observed with ERA‐I is much reduced in ERA5. ERA5 is closer to reference observations due to better behavior of low and mid‐level clouds and surface temperature.

Iodine is an atmospheric trace element emitted from oceans that efficiently destroys ozone (O3). Low O3 in airborne dust layers is frequently observed but poorly understood. We show that dust is a source of gas-phase iodine, indicated by aircraft observations of iodine monoxide (IO) radicals inside lofted dust layers from the Atacama and Sechura Deserts that are up to a factor of 10 enhanced over background. Gas-phase iodine photochemistry, commensurate with observed IO, is needed to explain the low O3 inside these dust layers (below 15 ppbv; up to 75% depleted). The added dust iodine can explain decreases in O3 of 8% regionally and affects surface air quality. Our data suggest that iodate reduction to form volatile iodine species is a missing process in the geochemical iodine cycle and presents an unrecognized aeolian source of iodine. Atmospheric iodine has tripled since 1950 and affects ozone layer recovery and particle formation.

Intrusions of warm, moist air into the Arctic during winter have emerged as important contributors to Arctic surface warming. Previous studies indicate that temperature, moisture, and hydrometeor enhancements during intrusions all make contributions to surface warming via emission of radiation down to the surface. Here, datasets from instrumentation at the Atmospheric Radiation Measurement User Facility in Utqia & x121;vik (formerly Barrow) for the six months from November through April for the six winter seasons of 2013/14-2018/19 were used to quantify the atmospheric state. These datasets subsequently served as inputs to compute surface downwelling longwave irradiances via radiative transfer computations at 1-min intervals with different combinations of constituents over the six winter seasons. The computed six winter average irradiance with all constituents included was 205.0 W m(-2), close to the average measured irradiance of 206.7 W m(-2), a difference of -0.8%. During this period, water vapor was the most important contributor to the irradiance. The computed average irradiance with dry gas was 71.9 W m(-2). Separately adding water vapor, liquid, or ice to the dry atmosphere led to average increases of 2.4, 1.8, and 1.6 times the dry atmosphere irradiance, respectively. During the analysis period, 15 episodes of warm, moist air intrusions were identified. During the intrusions, individual contributions from elevated temperature, water vapor, liquid water, and ice water were found to be comparable to each other. These findings indicate that all properties of the atmospheric state must be known in order to quantify the radiation coming down to the Arctic surface during winter.

Lidar retrievals of aerosol extinction and collocated relative humidity (RH) were acquired during the Department of Energy Combined High Spectral Resolution Lidar (HSRL) and Raman Measurement Study campaign in the summer of 2015 at the Southern Great Plains site in northern Oklahoma. Measurements of the hygroscopic properties of aerosols are crucial for accurately representing their relationship with clouds, which can be a significant source of uncertainty in assessing direct and indirect radiative effects. The ability for lidar to retrieve measurements of the vertically resolved f (RH), that is, the aerosol extinction at some wet RH normalized by the aerosol extinction at a dry reference RH, is investigated here and compared with nephelometer‐measured f (RH) at the surface. We introduce a modified approach to fitting the lidar measurements of aerosol extinction and our comparisons reveal that lidar and nephelometer measurements of f (RH) are consistent, both with each other and with reported values in the literature. The implications for this work present a path forward for global‐scale retrievals of remotely sensed aerosol hygroscopic properties. Most importantly, the efforts in this study could lead to closing the gap on uncertainties associated with the aerosol indirect radiative effect when combined with inversion retrievals of aerosol microphysical properties.

The U.S. Department of Energy Atmospheric Radiation Measurement (ARM) West Antarctic Radiation Experiment (AWARE) performed comprehensive meteorological and aerosol measurements and ground-based atmospheric remote sensing at two Antarctic stations using the most advanced instrumentation available. A suite of cloud research radars, lidars, spectral and broadband radiometers, aerosol chemical and microphysical sampling equipment, and meteorological instrumentation was deployed at McMurdo Station on Ross Island from December 2015 through December 2016. A smaller suite of radiometers and meteorological equipment, including radiosondes optimized for surface energy budget measurement, was deployed on the West Antarctic Ice Sheet between 4 December 2015 and 17 January 2016. AWARE provided Antarctic atmospheric data comparable to several well-instrumented high Arctic sites that have operated for many years and that reveal numerous contrasts with the Arctic in aerosol and cloud microphysical properties. These include persistent differences in liquid cloud occurrence, cloud height, and cloud thickness. Antarctic aerosol properties are also quite different from the Arctic in both seasonal cycle and composition, due to the continent's isolation from lower latitudes by Southern Ocean storm tracks. Antarctic aerosol number and mass concentrations are not only non-negligible but perhaps play a more important role than previously recognized because of the higher sensitivities of clouds at the very low concentrations caused by the large-scale dynamical isolation. Antarctic aerosol chemical composition, particularly organic components, has implications for local cloud microphysics. The AWARE dataset, fully available online in the ARM Program data archive, offers numerous case studies for unique and rigorous evaluation of mixed-phase cloud parameterization in climate models.

Observational knowledge about polar cloud processes requires information about the hydrometeor phase structure of the clouds, preferentially at high resolutions. Therefore, there are various attempts to classify ground-based radar observations using different techniques. In this letter, we examine the potential of detecting air-volumes containing liquid water in polar clouds using the Ka-band zenith-pointing radar (KAZR). We utilized the measurements gathered at Barrow, Alaska, in 2015, to produce comprehensive statistics about the Doppler-radar moments and the Doppler spectra. We find that the cloud-top liquid-bearing cloud layers (LBCLs) can potentially be reliably detected at high percentages with the KAZR when the signal is above the radar noise floor. However, embedded LBCLs are significantly more challenging to detect and could potentially be reliably separated in bulk processing only in exceptional cases, which account for not more than a few tens of percent of these cloud layer occurrences.

apid climate change on the West Antarctic Ice Sheet (WAIS) has challenged previous explanations of Antarctic climate change that focused on strengthening of circumpolar westerlies.A recent study linked surface melting conditions on the WAIS to atmospheric blocking over the Amundsen Sea region and to a negative phase of the southern annular mode, both of which correlate with El Niño in the tropical Pacific.There is a need to quantify the role of these changing air masses in the surface energy balance (SEB), and to improve the accuracy of global climate model simulations, which tend to perform poorly over the Antarctic and the Southern Ocean.The relative scarcity of cloud information at southern high latitudes has also inhibited progress.Surface melt during summer is important in WAIS mass loss-which is closely tied to global sea

Aerosol retrieval using ozone lidars in the ultraviolet spectral region is challenging but necessary for correcting aerosol interference in ozone retrieval and for studying the ozone–aerosol correlations. This study describes the aerosol retrieval algorithm for a tropospheric ozone lidar, quantifies the retrieval error budget, and intercompares the aerosol retrieval products at 299 nm with those at 532 nm from a high spectral resolution lidar (HSRL) and with those at 340 nm from an AErosol RObotic NETwork radiometer. After the cloud-contaminated data are filtered out, the aerosol backscatter or extinction coefficients at 30 m and 10 min resolutions retrieved by the ozone lidar are highly correlated with the HSRL products, with a coefficient of 0.95 suggesting that the ozone lidar can reliably measure aerosol structures with high spatiotemporal resolution when the signal-to-noise ratio is sufficient. The actual uncertainties of the aerosol retrieval from the ozone lidar generally agree with our theoretical analysis. The backscatter color ratio (backscatter-related exponent of wavelength dependence) linking the coincident data measured by the two instruments at 299 and 532 nm is 1.34±0.11, while the Ångström (extinction-related) exponent is 1.49±0.16 for a mixture of urban and fire smoke aerosols within the troposphere above Huntsville, AL, USA.