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NASA NTRS1992

Remote sensing of cloud, aerosol, and water vapor properties from the moderate resolution imaging spectrometer (MODIS)

The authors describe the status of MODIS-N and its companion instrument MODIS-T (tilt), a tiltable cross-track scanning spectrometer with 32 uniformly spaced channels between 0.410 and 0.875 micron. They review the various methods being developed for the remote sensing of atmospheric properties using MODIS, placing primary emphasis on the principal atmospheric applications of determining the optical, microphysical, and physical properties of clouds and aerosol particles from spectral reflection and thermal emission measurements. In addition to cloud and aerosol properties, MODIS-N will be used for determining the total precipitable water vapor and atmospheric stability. The physical principles behind the determination of each of these atmospheric products are described, together with an example of their application to aircraft and/or satellite measurements.

King, Michael D.↗
NASA NTRS2000

What we Hope to Learn about Global Mineral Dust Aerosols from EOS Multi-Angle Imaging SpectroRadiometer (MISR)

On global scales, just a few broad atmospheric aerosol compositional groups are commonly observed. Of these, "mineral dust" is the only group which both contains non-spherical particles, and typically has size distributions with enough large particles for particle shape to affect its visible-light-scattering properties. The MISR instrument is scheduled for launch into a 10:30 AM sun-synchronous, polar orbit aboard the EOS Terra satellite in 1999. MISR will measure the upwelling visible radiance from Earth in 4 spectral bands centered at 446, 558, 672, and 866 nm, at each of 9 emission angles spread out in the forward and aft directions along the flight path at +/-70.5 deg, +/-60.0 deg, +/-45.6 deg, +/-26.1deg, and nadir. Over a period of 7 minutes, as the spacecraft flies along, a 360 km wide swath of Earth will successively be viewed by each of the cameras, allowing MISR to sample a very large range of scattering angles; in mid latitudes, the instrument will observe scattering angles between about 60 deg and 160 deg. Global coverage will be acquired about once in 9 days at the equator; the nominal mission lifetime is 6 years. The distinction in single scattering phase function between natural distributions of spherical and randomly oriented, non-spherical particles, with a broad range of aspect ratios, shows up strongly for scattering angles ranging from about 90 deg to near 180 deg. For non-spherical particle distributions, single scattering phase functions tend to be much flatter in this region than for spherical particles. Since MISR samples the relevant range of scattering angles very well, we expect to be able to make critical distinctions between natural distributions of spherical and randomly oriented, non-spherical particles with MISR data. We anticipate that the new multiangle, multispectral data from MISR will also contain other information about particle properties, a major step beyond current spacecraft remote sensing retrievals, which obtain aerosol optical depth based on entirely assumed particle microphysical properties. According to simulations over cloud-free, calm ocean, for pure particles with natural ranges of optical depth, particle size, and indices of refraction, MISR should retrieve column optical depth for all but the darkest particles, to an uncertainty of at most 0.05 or 20%, whichever is larger, even if the particle properties are poorly known. For one common particle type, soot, constraints on the optical depth over dark ocean are very poor. The simulated measurements also should allow us to separate two to four compositional groups based on indices of refraction, and to identify three to four distinct size groups between 0.1 and 2.0 microns characteristic radius at most latitudes. The technique is most sensitive to particle microphysical properties in the "accumulation mode" sizes. where particle scattering undergoes the transition from Rayleigh to large-particle regimes for the MISR wavelengths. Based on these results, we expect to distinguish air masses containing different aerosol types, routinely and globally, with multiangle remote sensing data. Such data complements in situ and field data, which can provide details about aerosol size and composition locally that are needed to assess the radiative effects of aerosols quantitatively. Both field data and correlations in space and time with likely source and sink regions will also be helpful in developing a global picture of mineral dust aerosol budgets. Further work on the expected sensitivity of MISR to natural mixtures of pure particles, including climatologically likely mineral dust components, is currently underway.

Kahn, Ralph↗
DOE OSTI2021

Impact of dry intrusion events on the composition and mixing state of particles during the winter Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA)

Abstract. Long-range transport of continental emissions has a far-reaching influence over remote regions, resulting in substantial change in the size, morphology, and composition of the local aerosol population and cloud condensation nuclei (CCN) budget. Here, we investigate the physicochemical properties of atmospheric particles collected on board a research aircraft flown over the Azores during the winter 2018 Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA) campaign. Particles were collected within the marine boundary layer (MBL) and free troposphere (FT) after long-range atmospheric transport episodes facilitated by dry intrusion (DI) events. Chemical and physical properties of individual particles were investigated using complementary capabilities of computer-controlled scanning electron microscopy and X-ray spectromicroscopy to probe particle external and internal mixing state characteristics. Furthermore, real-time measurements of aerosol size distribution, cloud condensation nuclei (CCN) concentration, and back-trajectory calculations were utilized to help bring into context the findings from offline spectromicroscopy analysis. While carbonaceous particles were found to be the dominant particle type in the region, changes in the percent contribution of organics across the particle population (i.e., external mixing) shifted from 68 % to 43 % in the MBL and from 92 % to 46 % in FT samples during DI events. This change in carbonaceous contribution is counterbalanced by the increase in inorganics from 32 % to 57 % in the MBL and 8 % to 55 % in FT. The quantification of the organic volume fraction (OVF) of individual particles derived from X-ray spectromicroscopy, which relates to the multi-component internal composition of individual particles, showed a factor of 2.06 ± 0.16 and 1.11 ± 0.04 increase in the MBL and FT, respectively, among DI samples. We show that supplying particle OVF into the κ-Köhler equation can be used as a good approximation of field-measured in situ CCN concentrations. We also report changes in the κ values in the MBL from κMBL, non-DI=0.48 to κMBL, DI=0.41, while changes in the FT result in κFT, non-DI=0.36 to κFT, DI=0.33, which is consistent with enhancements in OVF followed by the DI episodes. Our observations suggest that entrainment of particles from long-range continental sources alters the mixing state population and CCN properties of aerosol in the region. The work presented here provides field observation data that can inform atmospheric models that simulate sources and particle composition in the eastern North Atlantic.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1992

Remote sensing of cloud, aerosol and water vapor properties from the Moderate Resolution Imaging Spectrometer (MODIS)

The Moderate Resolution Imaging Spectrometer (MODIS) is an Earth-viewing sensor being developed as a facility instrument for the Earth Observing System (EOS) to be launched in the late 1990s. MODIS consists of two separate instruments that scan a swath width sufficient to provide nearly complete global coverage every two days from a polar-orbiting, Sun-synchronous, platform at an altitude of 705 km. Of primary interest for studies of atmospheric physics is the MODIS-N (nadir) instrument which will provide images in 36 spectral bands between 0.415 and 14.235 micrometers with spatial resoulutions of 250 m (2 bands), 500 m (5 bands) and 1000 m (29 bands). These bands have been carefully selected to enable advanced studies of land, ocean and atmosperhic processes. The intent of this lecture is to describe the current status of MODIS-N and its companion instrument MODIS-T (tilt), a tiltable cross-track scanning radiometer with 32 uniformly spaced channels between 0.410 and 0.875 micrometers, and to describe the physical principles behind the development of MODIS for the remote sensing of atmospheric properties. Primary emphasis will be placed on the main atmospheric applications of determining the optical, microphysical and physical properties of clouds and aerosol particles form spectral-reflection and thermal-emission measurements. In addition to cloud and aerosol properties, MODIS-N will be utilized for the determination of the total precipitable water vapor over land and atmospheric stability. The physical principles behind the determination of each of these atmospheric products will be described herein.

King, M. D.↗
NASA NTRS1991

Optical properties of aerosol emissions from biomass burning in the tropics, BASE-A

Ground-based and airborne measurements of biomass-burning smoke particle optical properties, obtained with a view to aerosol-absorption properties, are presented as a function of time and atmospheric height. The wavelength dependence of the optical thickness can be explained by a log-normal size distribution, with particles' effective radius varying between 0.1 and 0.2 microns. The strong correlation noted between aerosol particle profile and CO profile indicates that smoke particulates constitute a good tracer for emission trace gases from tropical biomass burning.

Holben, Brent N.↗
DOE OSTI2024

Chemical properties and single-particle mixing state of soot aerosol in Houston during the TRACER campaign

Abstract. A high-resolution soot particle aerosol mass spectrometer (SP-AMS) was used to selectively measure refractory black carbon (rBC) and its associated coating material using both the ensemble size-resolved mass spectral mode and the event trigger single particle (ETSP) mode in Houston, Texas, in summer 2022. This study was conducted as part of the Department of Energy Atmospheric Radiation Measurement (ARM) program's TRacking Aerosol Convection interactions ExpeRiment (TRACER) field campaign. The study revealed an average (±1σ) rBC concentration of 103 ± 176 ng m−3. Additionally, the coatings on the BC particles were primarily composed of organics (59 %; 219 ± 260 ng m−3) and sulfate (26 %; 94 ± 55 ng m−3). Positive matrix factorization (PMF) analysis of the ensemble mass spectra of BC-containing particles resolved four distinct types of soot aerosol, including an oxidized organic aerosol (OOABC,PMF) factor associated with processed primary organic aerosol, an inorganic sulfate factor (SO4,BC,PMF), an oxidized rBC factor (O-BCPMF), and a mixed mineral dust–biomass burning aerosol factor with significant contribution from potassium (K-BBBC,PMF). Additionally, K-means clustering analysis of the single-particle mass spectra identified eight different clusters, including soot particles enriched in hydrocarbon-like organic aerosol (HOABC,ETSP), sulfate (SO4,BC,ETSP), two types of rBC, OOA (OOABC,ETSP), chloride (ClBC,ETSP), and nitrate (NO3,BC,ETSP). The single-particle measurements demonstrate substantial variation in BC coating thickness with coating-to-rBC mass ratios ranging from 0.1 to 100. The mixing state index (χ), which denotes the degree of homogeneity of the soot aerosol, varied from 4 % to 94 % with a median of 40 %, indicating that the aerosol population lies in between internal and external mixing but has large temporal and source type variability. In addition, a significant fraction of BC-containing particles, a majority enriched with oxidized organics and sulfate, exhibit sufficiently high κ values and diameters conducive to activation as cloud nuclei under atmospherically relevant supersaturation conditions. This finding bears significance in comprehending the aging processes of rBC-containing particles and their activation into cloud droplets. Our analysis highlights the complex nature of soot aerosol and underscores the need to comprehend its variability across different environments for accurate assessment of climate change.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2019

3+2+X: What Is the Most Useful Depolarization Input for Inverting Lidar Measurements of Non-Spherical Particles to Microphysical Properties?

The typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β ) at 355, 532, and 1064 nm and two extinction coefficients (α ) at 355 and 532 nm. This data combination is referred to as 3β +2α or 3+2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter to the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of δ that exceed 0.10 at 532 nm, i.e. in the presence of non-spherical particles such as desert dust, volcanic ash, and under special circumstances biomass-burning smoke.We use experimental data collected with instruments that are capable of measuring δ at all three lidar wavelengths with an inversion routine that uses the theory of light scattering by randomly oriented spheroids to replicate scattering properties of non-spherical particles. This is the first systematic test of the effect of using all theoretically possible combinations of δ taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information at least at one wavelength already provides useful information in the in version of optical data that describe light-scattering by nonspherical particles. However, any choice of δ(λ) will give lower values of the single-scattering albedo than the traditional 3+2 data set. We find that input data sets that include 355 give a non-spherical fraction that closely resembles the dust ratio we obtain from using β(532) and δ(532) in a methodology applied in aerosol-type separation. The use of 355 in data sets of two or three reduces the fraction of non-spherical particles that is retrieved when using δ(532) and δ(1064). Use of the latter two without accounting for 355 generally leads to high fractions of non-spherical particles that we consider not trustworthy. The use of three δ(λ) instead of two δ(λ) including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3+2+δ(355). Because of the technical challenges involved with accurately measuring δ(1064) we conclude that — depending on measurement capability — the future standard input for inversion using spheroid kernels might be 3+2+δ(355) or 3+2+δ(355)+δ(532).

Tesche, M.↗
DOE OSTI2022

Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories

Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utgiavik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr –1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Quantifying the effects of mixing state on aerosol optical properties

Abstract. Calculations of the aerosol direct effect on climate rely on simulated aerosol fields. The model representation of aerosol mixing state potentially introduces large uncertainties into these calculations, since the simulated aerosol optical properties are sensitive to mixing state. In this study, we systematically quantified the impact of aerosol mixing state on aerosol optical properties using an ensemble of 1800 aerosol populations from particle-resolved simulations as a basis for Mie calculations for optical properties. Assuming the aerosol to be internally mixed within prescribed size bins caused overestimations of aerosol absorptivity and underestimations of aerosol scattering. Together, these led to errors in the populations' single scattering albedo of up to −22.3 % with a median of −0.9 %. The mixing state metric χ proved useful in relating errors in the volume absorption coefficient, the volume scattering coefficient and the single scattering albedo to the degree of internally mixing of the aerosol, with larger errors being associated with more external mixtures. At the same time, a range of errors existed for any given value of χ. We attributed this range to the extent to which the internal mixture assumption distorted the particles' black carbon content and the refractive index of the particle coatings. Both can vary for populations with the same value of χ. These results are further evidence of the important yet complicated role of mixing state in calculating aerosol optical properties.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Ambient Aerosol Is Physically Larger on Cloudy Days in Bondville, Illinois

Particle chemical composition affects aerosol optical and physical properties in ways important for the fate, transport, and impact of atmospheric particulate matter. For example, hygroscopic constituents take up water to increase the physical size of a particle, which can alter the extinction properties and atmospheric lifetime. At the collocated AERosol RObotic NETwork (AERONET) and Interagency Monitoring of PROtected Visual Environments (IMPROVE) network monitoring stations in rural Bondville, Illinois, we employ a novel cloudiness determination method to compare measured aerosol physicochemical properties on predominantly cloudy and clear sky days from 2010 to 2019. On cloudy days, aerosol optical depth (AOD) is significantly higher than on clear sky days in all seasons. Measured angstrom ngstro''m exponents are significantly smaller on cloudy days, indicating physically larger average particle size for the sampled populations in all seasons except winter. Mass concentrations of fine particulate matter that include estimates of aerosol liquid water (ALW) are higher on cloudy days in all seasons but winter. More ALW on cloudy days is consistent with larger particle sizes inferred from angstrom ngstro''m exponent measurements. Aerosol chemical composition that affects hygroscopicity plays a determining impact on cloudy versus clear sky differences in AOD, angstrom ngstro''m exponents, and ALW. This work highlights the need for simultaneous collocated, high-time-resolution measurements of both aerosol chemical and physical properties, in particular at cloudy times when quantitative understanding of tropospheric composition is most uncertain.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2016

How We Can Constrain Aerosol Type Globally

In addition to aerosol number concentration, aerosol size and composition are essential attributes needed to adequately represent aerosol-cloud interactions (ACI) in models. As the nature of ACI varies enormously with environmental conditions, global-scale constraints on particle properties are indicated. And although advanced satellite remote-sensing instruments can provide categorical aerosol-type classification globally, detailed particle microphysical properties are unobtainable from space with currently available or planned technologies. For the foreseeable future, only in situ measurements can constrain particle properties at the level-of-detail required for ACI, as well as to reduce uncertainties in regional-to-global-scale direct aerosol radiative forcing (DARF). The limitation of in situ measurements for this application is sampling. However, there is a simplifying factor: for a given aerosol source, in a given season, particle microphysical properties tend to be repeatable, even if the amount varies from day-to-day and year-to-year, because the physical nature of the particles is determined primarily by the regional environment. So, if the PDFs of particle properties from major aerosol sources can be adequately characterized, they can be used to add the missing microphysical detail the better sampled satellite aerosol-type maps. This calls for Systematic Aircraft Measurements to Characterize Aerosol Air Masses (SAM-CAAM). We are defining a relatively modest and readily deployable, operational aircraft payload capable of measuring key aerosol absorption, scattering, and chemical properties in situ, and a program for characterizing statistically these properties for the major aerosol air mass types, at a level-of-detail unobtainable from space. It is aimed at: (1) enhancing satellite aerosol-type retrieval products with better aerosol climatology assumptions, and (2) improving the translation between satellite-retrieved aerosol optical properties and species-specific aerosol mass and size that are tracked in aerosol transport and climate models used to assess aerosol forcing and its anthropogenic components. This presentation will summarize where we stand on the development of the SAM-CAAM concept.

DARF↗
DOE OSTI2021

Observations of Aerosol, Cloud, Turbulence, and Radiation Properties at the Top of the Marine Boundary Layer over the Eastern North Atlantic Ocean: The ACORES Campaign

We report on the Azores Stratocumulus Measurements of Radiation, Turbulence and Aerosols (ACORES) campaign, which took place around Graciosa and Pico Islands/Azores in July 2017. The main objective was to investigate the vertical distribution of aerosol particles, stratocumulus microphysical and radiative properties, and turbulence parameters in the eastern North Atlantic. The vertical exchange of mass, momentum, and energy between the free troposphere (FT) and the cloudy marine boundary layer (MBL) was explored over a range of scales from submeters to kilometers. To cover these spatial scales with appropriate measurements, helicopter-borne observations with unprecedented high resolution were realized using the Airborne Cloud Turbulence Observation System (ACTOS) and Spectral Modular Airborne Radiation Measurement System–Helicopter-Borne Observations (SMART-HELIOS) instrumental payloads. Here, the helicopter-borne observations were combined with ground-based aerosol measurements collected at two continuously running field stations on Pico Mountain (2,225 m above sea level, in the FT), and at the Atmospheric Radiation Measurement (ARM) station on Graciosa (at sea level). First findings from the ACORES observations we are discussing in the paper are as follows: (i) we have observed a high variability of the turbulent cloud-top structure on horizontal scales below 100 m with local temperature gradients of up to 4 K over less than 1 m vertical distance, (ii) we have collected strictly collocated radiation measurements supporting the relevance of small-scale processes by revealing significant inhomogeneities in cloud-top brightness temperature to scales well below 100 m, and (iii) we have concluded that aerosol properties are completely different in the MBL and FT with often-complex stratification and frequently observed burst-like new particle formation.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2017

Developing and Diagnosing Climate Change Indicators of Regional Aerosol Optical Properties

Given the importance of aerosol particles to radiative transfer via aerosol-radiation interactions, a methodology for tracking and diagnosing causes of temporal changes in regional-scale aerosol populations is illustrated. The aerosol optical properties tracked include estimates of total columnar burden (aerosol optical depth, AOD), dominant size mode (Ångström exponent, AE), and relative magnitude of radiation scattering versus absorption (single scattering albedo, SSA), along with metrics of the structure of the spatial field of these properties. Over well-defined regions of North America, there are generally negative temporal trends in mean and extreme AOD, and SSA. These are consistent with lower aerosol burdens and transition towards a relatively absorbing aerosol, driven primarily by declining sulfur dioxide emissions. Conversely, more remote regions are characterized by increasing mean and extreme AOD that is attributed to increased local wildfire emissions and long-range (transcontinental) transport. Regional and national reductions in anthropogenic emissions of aerosol precursors are leading to declining spatial autocorrelation in the aerosol fields and increased importance of local anthropogenic emissions in dictating aerosol burdens. However, synoptic types associated with high aerosol burdens are intensifying (becoming more warm and humid), and thus changes in synoptic meteorology may be offsetting aerosol burden reductions associated with emissions legislation.

Ryan C Sullivan↗
NASA NTRS2000

What we can Learn About Aerosols from EOS-MISR Multi-Angle Remote Sensing Observations

Multiangle, multispectral remote sensing observations, such as those anticipated from the Earth Observing System (EOS) Multiangle Imaging SpectroRadiometer (MISR), promise to significantly improve our ability to constrain aerosol properties from space. Recent advances in modeling the Earth's climate have brought us to a point where the contributions made by aerosols to the global radiation budget noticeably affect the results. Knowledge of both aerosol optical depth and the microphysical properties of particles is needed to adequately model aerosol effects. This talk explores the ability of multiangle, multi-spectral remote sensing observations anticipated from the EOS MISR instrument, to retrieve aerosol optical depth and information about mixes of particle types, globally, at 17.6 km spatial resolution. The instrument is scheduled for launch into a 10:30 AM, sun-synchronous polar orbit in 1999.

Kahn, Ralph↗
DOE OSTI2026

Hygroscopic growth of UO 2 F 2 nanoparticles

Hygroscopicity is an important physicochemical property of aerosol that describes the ability of a particle to uptake water. The hygroscopic properties of uranyl fluoride (UO 2 F 2 ) aerosol generated from a UF 6 hydrolysis reactor was investigated for the first time using a custom-built Humidified Tandem Differential Mobility Analyzer (HTDMA). The HTDMA is capable of measuring UO 2 F 2 nanoparticle growth determined by mobility size over a wide range of atmospheric humidity from dry conditions at <10% relative humidity (RH) to 85% RH. The hygroscopic properties were determined for nanoparticles as small as 3.5 nm in this study. Although the largest size of UO 2 F 2 nanoparticles was 80 nm, monodisperse aerosol with a mobility diameter of up to approximately 500 nm can be investigated using the HTDMA. Anhydrous UO 2 F 2 nanoparticles with a mobility diameter of 3.5 nm were shown to be highly hygroscopic with a deliquescence relative humidity (DRH) of 10%. Hydrates with a larger mobility diameter from 10 to 80 nm were non-hygroscopic with no observable DRH and limited water uptake up to 85% RH. Here, these results demonstrate the hygroscopic properties of UO 2 F 2 nanoparticles are highly variable and based on both the mobility size and hydration state. Hygroscopicity affects the physicochemical properties of UO 2 F 2 nanoparticles, including the aerosol phase state and viscosity, with impacts on aerosol growth, coagulation, and deposition that is critical for understanding the fate and transport of UO 2 F 2 nanoparticles in the atmosphere.

Hygroscopicity↗
DOE OSTI2023

Annual cycle of aerosol properties over the central Arctic during MOSAiC 2019–2020 – light-extinction, CCN, and INP levels from the boundary layer to the tropopause

Abstract. The MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition was the largest Arctic field campaign ever conducted. MOSAiC offered the unique opportunity to monitor and characterize aerosols and clouds with high vertical resolution up to 30 km height at latitudes from 80 to 90∘ N over an entire year (October 2019 to September 2020). Without a clear knowledge of the complex aerosol layering, vertical structures, and dominant aerosol types and their impact on cloud formation, a full understanding of the meteorological processes in the Arctic, and thus advanced climate change research, is impossible. Widespread ground-based in situ observations in the Arctic are insufficient to provide these required aerosol and cloud data. In this article, a summary of our MOSAiC observations of tropospheric aerosol profiles with a state-of-the-art multiwavelength polarization Raman lidar aboard the icebreaker Polarstern is presented. Particle optical properties, i.e., light-extinction profiles and aerosol optical thickness (AOT), and estimates of cloud-relevant aerosol properties such as the number concentration of cloud condensation nuclei (CCN) and ice-nucleating particles (INPs) are discussed, separately for the lowest part of the troposphere (atmospheric boundary layer, ABL), within the lower free troposphere (around 2000 m height), and at the cirrus level close to the tropopause. In situ observations of the particle number concentration and INPs aboard Polarstern are included in the study. A strong decrease in the aerosol amount with height in winter and moderate vertical variations in summer were observed in terms of the particle extinction coefficient. The 532 nm light-extinction values dropped from >50 Mm−1 close to the surface to <5 Mm−1 at 4–6 km height in the winter months. Lofted, aged wildfire smoke layers caused a re-increase in the aerosol concentration towards the tropopause. In summer (June to August 2020), much lower particle extinction coefficients, frequently as low as 1–5 Mm−1, were observed in the ABL. Aerosol removal, controlled by in-cloud and below-cloud scavenging processes (widely suppressed in winter and very efficient in summer) in the lowermost 1–2 km of the atmosphere, seems to be the main reason for the strong differences between winter and summer aerosol conditions. A complete annual cycle of the AOT in the central Arctic could be measured. This is a valuable addition to the summertime observations with the sun photometers of the Arctic Aerosol Robotic Network (AERONET). In line with the pronounced annual cycle in the aerosol optical properties, typical CCN number concentrations (0.2 % supersaturation level) ranged from 50–500 cm−3 in winter to 10–100 cm−3 in summer in the ABL. In the lower free troposphere (at 2000 m), however, the CCN level was roughly constant throughout the year, with values mostly from 30 to 100 cm−3. A strong contrast between winter and summer was also given in terms of ABL INPs which control ice production in low-level clouds. While soil dust (from surrounding continents) is probably the main INP type during the autumn, winter, and spring months, local sea spray aerosol (with a biogenic aerosol component) seems to dominate the ice nucleation in the ABL during the summer months (June–August). The strong winter vs. summer contrast in the INP number concentration by roughly 2–3 orders of magnitude in the lower troposphere is, however, mainly caused by the strong cloud temperature contrast. A unique event of the MOSAiC expedition was the occurrence of a long-lasting wildfire smoke layer in the upper troposphere and lower stratosphere. Our observations suggest that the smoke particles frequently triggered cirrus formation close to the tropopause from October 2019 to May 2020.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2004

Enabling Technologies for High-accuracy Multiangle Spectropolarimetric Imaging from Space

Satellite remote sensing plays a major role in measuring the optical and radiative properties, environmental impact, and spatial and temporal distribution of tropospheric aerosols. In this paper, we envision a new generation of spaceborne imager that integrates the unique strengths of multispectral, multiangle, and polarimetric approaches, thereby achieving better accuracies in aerosol optical depth and particle properties than can be achieved using any one method by itself. Design goals include spectral coverage from the near-UV to the shortwave infrared; global coverage within a few days; intensity and polarimetric imaging simultaneously at multiple view angles; kilometer to sub-kilometer spatial resolution; and measurement of the degree of linear polarization for a subset of the spectral complement with an uncertainty of 0.5% or less. The latter requirement is technically the most challenging. In particular, an approach for dealing with inter-detector gain variations is essential to avoid false polarization signals. We propose using rapid modulation of the input polarization state to overcome this problem, using a high-speed variable retarder in the camera design. Technologies for rapid retardance modulation include mechanically rotating retarders, liquid crystals, and photoelastic modulators (PEMs). We conclude that the latter are the most suitable.

photoelastic modulators (PEMs)↗