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Over 900 event-based precipitation samples were collected in 2019–2021 in the Tien Shan and its foothills and analysed using cavity ring-down spectroscopy. δD and δ18O values were highest in summer and lowest in winter, and annual cycles of deuterium excess (d-excess) varied between sites, reflecting local conditions. The δ18O and δD values increased from north to south in all seasons except autumn, and latitude was a statistically significant predictor of δ18O and δD in the overall data set, along with elevation in winter and elevation and longitude in autumn. Elevation was a significant predictor of d-excess in all seasons, and local air temperature was a more important control over δ18O and δD than precipitation depth. Local meteoric water lines were derived using seven regression methods applied to non-weighted and weighted precipitation. Non-weighted ordinary least squares regression and reduced major axis regression methods are recommended overall, except for summer when the precipitation-weighted least squares regression should be used, particularly in the south. Atmospheric back-trajectory and mixing-model analyses were applied in combination to identify air mass source regions and their relative contribution to precipitation. Recycled moisture from irrigated land in the Amu Darya and Syr Darya basins and from the study catchments accounted for 29 %–71 % of precipitation, depending on the site and season. In the Chon Kyzyl-Suu catchment, local re-evaporation from Issyk-Kul accounted for up to 85 % of precipitation. These findings highlight the importance of moisture from terrestrial sources, especially irrigated land, for the formation of precipitation in the Tien Shan.

Wildfires and agricultural burning generate seemingly increasing smoke aerosol emissions, impacting societal and natural ecosystems. To understand smoke's effects on climate and public health, we analyzed the spatiotemporal distribution of smoke aerosols, focusing on two major light-absorbing components, namely black carbon (BC) and brown carbon (BrC) aerosols. Using NASA's Earth Polychromatic Imaging Camera (EPIC) instrument aboard NOAA's Deep Space Climate Observatory (DSCOVR) spacecraft, we inferred BC and BrC volume fractions and particle mass concentrations based on spectral absorption provided by the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm with 1–2 h temporal resolution and ∼ 10 km spatial resolution over North America and central Africa. Our analyses of regional smoke properties reveal distinct characteristics for aerosol optical depth (AOD) at 443 nm, spectral single-scattering albedo (SSA), aerosol layer height (ALH), and BC and BrC amounts. Smoke aerosols in North America showed extremely high AOD up to 6, with elevated ALH (6–7 km) and significant BrC components up to 250 mg m−2 along the transport paths, whereas the smoke aerosols in central Africa exhibited stronger light absorption (i.e., lower SSA) and lower AOD, resulting in higher-BC mass concentrations and similar BrC mass concentrations than the cases in North America. Seasonal burning source locations in central Africa, following the seasonal shift in the Intertropical Convergence Zone and diurnal variations in smoke amounts, were also captured. A comparison of retrieved AOD443, SSA443, SSA680, and ALH with collocated AERONET and CALIOP measurements shows agreement with RMSE values of 0.2, 0.03–0.04, 0.02–0.04, and 0.8–1.3 km, respectively. An analysis of the spatiotemporal average reveals distinct geographical characteristics in smoke properties closely linked to burning types and meteorological conditions. Forest wildfires over western North America generated smoke with a small-BC volume fraction of 0.011 and a high ALH with large variability (2.2 ± 1.2 km), whereas smoke from wildfires and agricultural burning over Mexico region shows more absorption and low ALH. Smoke from savanna fires over central Africa had the most absorption, with a high-BC volume fraction (0.015) and low ALH with a small variation (1.8 ± 0.6 km) among the analyzed regions. Tropical forest smoke was less absorbing and had a high variance in ALH. We also quantify the estimation uncertainties related to the assumptions of BC and BrC refractive indices. The MAIAC EPIC smoke properties with BC and BrC volume and mass fractions and assessment of the layer height provide observational constraints for radiative forcing modeling and air quality and health studies.

Cloud condensation nuclei (CCN) are mediators of aerosol–cloud interactions (ACIs), contributing to the largest uncertainties in the understandings of global climate change. We present a novel remote-sensing-based algorithm that quantifies the vertically resolved CCN number concentrations (NCCN) using aerosol optical properties measured by a multiwavelength lidar. The algorithm considers five distinct aerosol subtypes with bimodal size distributions. The inversion used the lookup tables developed in this study, based on the observations from the Aerosol Robotic Network, to efficiently retrieve optimal particle size distributions from lidar measurements. The method derives dry aerosol optical properties by implementing hygroscopic enhancement factors in lidar measurements. The retrieved optically equivalent particle size distributions and aerosol-type-dependent particle composition are utilized to calculate critical diameters using κ-Köhler theory and NCCN at six supersaturations ranging from 0.07 % to 1.0 %. Sensitivity analyses indicate that uncertainties in extinction coefficients and relative humidity greatly influence the retrieval error in NCCN. The potential of this algorithm is further evaluated by retrieving NCCN using airborne lidar from the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) campaign and is validated against simultaneous measurements from the CCN counter. The independent validation with robust correlation demonstrates promising results. Furthermore, the NCCN has been retrieved for the first time using a proposed algorithm from spaceborne lidar – Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) – measurements. The application of this new capability demonstrates the potential for constructing a 3D CCN climatology at a global scale, which helps to better quantify ACI effects and thus reduce the uncertainty in aerosol climate forcing.

The iron-oxide content of dust in the atmosphere and most notably its apportionment between hematite (α-Fe2O3) and goethite (α-FeOOH) are key determinants in quantifying dust's light absorption, its top of atmosphere ultraviolet (UV) radiances used for dust monitoring, and ultimately shortwave dust direct radiative effects (DREs). Hematite and goethite column mass concentrations and iron-oxide mass fractions of total dust mass concentration were retrieved from the Deep Space Climate Observatory (DSCOVR) Earth Polychromatic Imaging Camera (EPIC) measurements in the ultraviolet–visible (UV–Vis) channels. The retrievals were performed for dust-identified aerosol plumes over land using aerosol optical depth (AOD) and the spectral imaginary refractive index provided by the Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm over six continental regions (North America, North Africa, West Asia, Central Asia, East Asia, and Australia). The dust particles are represented as an internal mixture of non-absorbing host and absorbing hematite and goethite. We use the Maxwell Garnett effective medium approximation with carefully selected complex refractive indices of hematite and goethite that produce mass fractions of iron-oxide species consistent with in situ values found in the literature to derive the hematite and goethite volumetric/mass concentrations from MAIAC EPIC products. We compared the retrieved hematite and goethite concentrations with in situ dust aerosol mineralogical content measurements, as well as with published data. Our data display variations within the published range of hematite, goethite, and iron-oxide mass fractions for pure-mineral-dust cases. A specific analysis is presented for 15 sites over the main dust-source regions. Sites in the central Sahara, Sahel, and Middle East exhibit a greater temporal variability of iron oxides relative to other sites. The Niger site (13.52∘ N, 2.63∘ E) is dominated by goethite over the Harmattan season with a median of ∼ 2 weight percentage (wt %) of iron oxide. The Saudi Arabia site (27.49∘ N, 41.98∘ E) over the Middle East also exhibited a surge of goethite content with the beginning of the shamal season. The Sahel dust is richer in iron oxide than Saharan and northern China dust except in summer. The Bodélé Depression area shows a distinctively lower iron-oxide concentration (∼ 1 wt %) throughout the year. Finally, we show that EPIC data allow the constraining of the hematite refractive index. Specifically, we select 5 out of 13 different hematite refractive indices that are widely variable in published laboratory studies by constraining the iron-oxide mass ratio to the known measured values. The provided climatology of hematite and goethite mass fractions across the main dust regions of Earth will be useful for dust shortwave DRE studies and climate modeling.

The large uncertainty in the mineral dust direct radiative effect (DRE) hinders projections of future climate change due to anthropogenic activity. Resolving modeled dust mineral speciation allows for spatially and temporally varying refractive indices consistent with dust aerosol composition. Here, for the first time, we quantify the range in dust DRE at the top of the atmosphere (TOA) due to current uncertainties in the surface soil mineralogical content using a dust mineral-resolving climate model. We propagate observed uncertainties in soil mineral abundances from two soil mineralogy atlases along with the optical properties of each mineral into the DRE and compare the resultant range with other sources of uncertainty across six climate models. The shortwave DRE responds region-specifically to the dust burden depending on the mineral speciation and underlying shortwave surface albedo: positively when the regionally averaged annual surface albedo is larger than 0.28 and negatively otherwise. Among all minerals examined, the shortwave TOA DRE and single scattering albedo at the 0.44–0.63 µm band are most sensitive to the fractional contribution of iron oxides to the total dust composition. The global net (shortwave plus longwave) TOA DRE is estimated to be within −0.23 to +0.35 W m−2. Approximately 97 % of this range relates to uncertainty in the soil abundance of iron oxides. Representing iron oxide with solely hematite optical properties leads to an overestimation of shortwave DRE by +0.10 W m−2 at the TOA, as goethite is not as absorbing as hematite in the shortwave spectrum range. Our study highlights the importance of iron oxides to the shortwave DRE: they have a disproportionally large impact on climate considering their small atmospheric mineral mass fractional burden (∼2 %). An improved description of iron oxides, such as those planned in the Earth Surface Mineral Dust Source Investigation (EMIT), is thus essential for more accurate estimates of the dust DRE.

We conceptualize aerosol radiative transfer processes arising from the hypothetical coupling of a global aerosol transport model and a global numerical weather prediction model by applying the US Naval Research Laboratory Navy Aerosol Analysis and Prediction System (NAAPS) and the Navy Global Environmental Model (NAVGEM) meteorological and surface reflectance fields. A unique experimental design during the 2013 NASA Studies of Emissions and Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field mission allowed for collocated airborne sampling by the high spectral resolution Lidar (HSRL), the Airborne Multi-angle SpectroPolarimetric Imager (AirMSPI), up/down shortwave (SW) and infrared (IR) broadband radiometers, as well as NASA A-Train support from the Moderate Resolution Imaging Spectroradiometer (MODIS), to attempt direct aerosol forcing closure. The results demonstrate the sensitivity of modeled fields to aerosol radiative fluxes and heating rates, specifically in the SW, as induced in this event from transported smoke and regional urban aerosols. Limitations are identified with respect to aerosol attribution, vertical distribution, and the choice of optical and surface polarimetric properties, which are discussed within the context of their influence on numerical weather prediction output that is particularly important as the community propels forward towards inline aerosol modeling within global forecast systems.