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At least 19 records

Humidified single-scattering albedometer (H-CAPS-PM SSA ): Design, data analysis, and validation

In this work, we report the development and validation of a new humidified aerosol single-scattering albedometer to quantify the effects of water uptake on submicrometer particle optical properties. The instrument simultaneously measures in situ aerosol light extinction ( σ ep ) and scattering ( σ sp ) using a cavity-attenuated phase shift-single scattering albedo particulate matter (PM) monitor (CAPS-PM SSA , Aerodyne Research, Inc., Billerica, MA, USA). It retrieves by difference aerosol light absorption ( σ ap ) and directly quantifies aerosol single-scattering albedo (SSA), the aerosol “brightness.” We custom built a relative humidity (RH) control system using a water vapor-permeable membrane humidifier and coupled it to the CAPS-PM SSA to enable humidified aerosol observations. Our humidified instrument (H-CAPS-PM SSA ) overcomes problems with noise caused by mirror purge-flow humidification, heating, and characterizing cell RH. Careful angular truncation corrections in scattering, particularly for larger particles, were combined with empirical observations. Results show that the optimal operational size to be D p < 400 nm. The H-CAPS-PM SSA was evaluated with several pure single-component aerosols including ammonium sulfate ((NH 4 ) 2 SO 4 ), absorbing nigrosin, and levoglucosan, an organic biomass smoke tracer. The measured σ ep , σ sp , and the derived optical hygroscopicity parameter ( κ ) for size-selected ammonium sulfate are in good agreement with literature values. For dry size-selected nigrosin in the 100 < D p < 400 nm range, SSA values increased from ~0.3 to 0.65 with increasing D p . The enhancement in nigrosin σ ap at RH = 80% was a factor of 1.05–1.20 relative to dry conditions, with the larger particles showing greater enhancement. SSA increased with RH with the largest fractional enhancement measured for the smallest particles. For polydisperse levoglucosan, we measured an optical κ of 0.26 for both light extinction and scattering and negligible absorption. Our new instrument enables reliable observations of the effects of ambient humidity on mixed aerosol optical properties, particularly for light-absorbing aerosols whose climate forcing is uncertain due to measurement gaps.

54 ENVIRONMENTAL SCIENCES↗

CAPS PMssa Aerosol Extinction and SSA Data

We collected rapid (1 second time response) measurements of aerosol extinction and scattering (Mm-1) using an Aerodyne CAPS PMssa deployed during LASIC (as part of the LASIC SSA-constraint study) to measure ambient SSA at 530 nm wavelength to compare with other optical measurement methods. Measured from August 4 to September 22, 2017. Sampled from both PM1 and PM10 inlets. CAPS PMssa monitors have been tested extensively for PM2.5 and smaller particle sizes, but not for particles greater than 2,500 nm in diameter (i.e., PM10). The data were collected in order to provide an independent measurement of aerosol single scattering albedo at 530 nm wavelength to compare with ARM standard methods.

54 ENVIRONMENTAL SCIENCES↗

Algorithmic construction of SSA-compatible extreme rays of the subadditivity cone and the N = 6 solution

We compute the set of all extreme rays of the 6-party subadditivity cone that are compatible with strong subadditivity. In total, we identify 208 new (genuine 6-party) orbits, 52 of which violate at least one known holographic entropy inequality. For the remaining 156 orbits, which do not violate any such inequalities, we construct holographic graph models for 150 of them. For the final 6 orbits, it remains an open question whether they are holographic. Consistent with the strong form of the conjecture in [1], 148 of these graph models are trees. However, 2 of the graphs contain a “bulk cycle”, leaving open the question of whether equivalent models with tree topology exist, or if these extreme rays are counterexamples to the conjecture. The paper includes a detailed description of the algorithm used for the computation, which is presented in a general framework and can be applied to any situation involving a polyhedral cone defined by a set of linear inequalities and a partial order among them to find extreme rays corresponding to down-sets in this poset.

AdS-CFT correspondence↗

News and Notes: SSA Task Force on Diversity, Equity, and Inclusion: Toward a Changing, Inclusive Future in Earthquake Science

In the United States, a wide variety of studies show that the geoscience community does not reflect the broader societal makeup (e.g., Velasco and Jaurrieta de Velasco, 2010; Dutt, 2020; Howley, 2020). In fact, only about 10% of all Science, Technology, Engineering, Mathematics (STEM) Ph.D. degrees are awarded to people of color, although they represent more than a third of the population (Dutt, 2020). These numbers have changed little over the past 40 years (e.g., Bernard and Cooperdock, 2018; Dutt, 2020). Recent events in the United States have again raised awareness of this discrepancy in many fields; similar divergences may be present throughout the world. How this discrepancy represents a tremendous loss of talent and contributes to ongoing bias and racism is discussed.

58 GEOSCIENCES↗

TRACER-CAT-LANL Aerosol Optics and Chemical Speciation - CAPS-SSA

Aerosol size distribution, optical properties, and speciation data collected in La Port TX, during TRACER-CAT-LANL, July 2022, with basic trace gas measurements. All sampling was conducted with an identical aerosol inlet as the standard ARM-AOS systems. The TRacking Aerosol Convection interactions ExpeRiment Carbonaceous Aerosols Thrust by Los Alamos National Laboratory (TRACER-CAT-LANL, July 2022) was designed to complement the larger ARM TRACER science goals to understand convective cloud lifecycles and aerosol-convection interactions. TRACER-CAT-LANL is focused on understanding the relationship between particle composition and light absorption and the influence of water uptake on this relationship. This aerosol and trace gas data can be used to understand the relationship between particle composition and light absorption and the influence of water uptake on this relationship. Instruments Include: Picarro GHG Photoacoustic Soot Spectrometer (PASS-3) Humidified-cavity attenuated phase shift-single scattering albedo particulate matter monitor (H-CAPS-PMSSA) Soot Particle Aerosol Mass Spectrometer (SPAMS) Single-Particle Soot Photometer (SP2) Cloud Condensation Nuclei Counter (CCNc) Aerodynamic Particle Sizer (APS) Scanning Mobility Particle Sizer (SMPS)

54 ENVIRONMENTAL SCIENCES↗

Chemical Composition and Mixing State of Wintertime Aerosol from the European Arctic Site of Ny-Ålesund, Svalbard

The Arctic is rapidly warming, and aerosols play an increasingly important role by scattering and absorbing sunlight and by participating in cloud formation. Their optical and cloud-forming properties depend on the mixing state and chemical composition, but observations of these features remain limited. This study comprehensively characterizes 25,254 individual particles collected at Ny-Ålesund, Svalbard (November −December 2020), using microspectroscopy techniques to investigate their size, morphology, mixing state, and chemical composition. Fresh sea salt aerosols (SSA) were identified as the most abundant (∼85%), of the total observed aerosol population, with potential sources from sea spray and blowing snow. Air masses originating from the Arctic Ocean surrounding Svalbard likely contribute to increased concentrations of sub-micrometer “Fresh SSA” particles. “Aged SSA” particles (7.4%) are enriched in sulfur and nitrogen, compared to “Fresh SSA”. These elevated ratios may result from various atmospheric aging processes including the uptake of sulfuric and nitric acids. Here, our results suggest that aged SSA, with sizes larger than 300 nm, likely underwent chlorine depletion by sulfuric and nitric acids during transport. Additionally, elemental analysis reveals that both fresh and aged SSA can mix with dust particles, regardless of the SSA size (49.9% in sub-micrometer size and 50.1% in super-micrometer size, respectively). Dust particles are efficient ice-nucleating particles (INPs), and SSA is known to act as cloud condensation nuclei (CCN), and therefore, their mixtures may inherit both properties. The non-negligible number (4.4%) of SSA-dust mixtures underscores the importance of these particles as potential sources of CCN and INP in the Arctic atmosphere.

Arctic↗

Seasonal variations in fire conditions are important drivers in the trend of aerosol optical properties over the south-eastern Atlantic

Abstract. From June to October, southern Africa produces one-third of the global biomass burning (BB) emissions by widespread fires. BB aerosols are transported westward over the south-eastern Atlantic with the mid-tropospheric winds, resulting in significant radiative effects. Ascension Island (ASI) is located midway between Africa and South America. From June 2016 to October 2017, a 17-month in situ observation campaign on ASI found a low single-scattering albedo (SSA) as well as a high mass absorption cross-section of black carbon (MACBC), demonstrating the strong absorbing marine boundary layer in the south-eastern Atlantic. Here we investigate the monthly variations of critical optical properties of BB aerosols, i.e. SSA and MACBC, during the BB seasons and the driving factors behind these variations. Both SSA and MACBC increase from June to August and decrease in September and October. The average SSA during the BB seasons is 0.81 at 529 nm wavelength, with the highest mean ∼ 0.85 in October and the lowest ∼ 0.78 in August. The absorption enhancement (Eabs) derived from the MACBC shows similar trends with SSA, with the average during the whole of the BB seasons at ∼ 1.96 and ∼ 2.07 in 2016 and 2017, respectively. As the Eabs is higher than the ∼ 1.5 commonly adopted value by climate models, this result suggests the marine boundary layer in the south-eastern Atlantic is more absorbing than model simulations. We find the enhanced ratio of BC to CO (ΔBC/ΔCO, equal to BC/ΔCO as the BC background concentration is considered to be 0) is well correlated with SSA and MACBC, providing a simple way to estimate the aerosol optical characteristics in the south-eastern Atlantic. The exponential function we proposed can approximate SSA and MACBC with BC/ΔCO, and when BC/ΔCO is small it can capture the rapid growth of SSA as BC/ΔCO decreases. BC/ΔCO is influenced by combustion conditions and aerosol scavenging. From the analysis of the location of BB, the primary source fuel, the water content in the fuel, combined with the mean cloud cover and precipitation in the transport areas of the BB plume, we conclude that the increase in BC/ΔCO from June to August is likely to be caused by burning becoming more flaming. The reduction in the water content of fuels may be responsible for the change in the burning conditions from June to August. The decrease in BC/ΔCO in September and October may be caused by two factors, one being a lower proportion of flaming conditions, possibly associated with a decrease in mean surface wind speed in the burning area, and the other being an increase in precipitation in the BB transport pathway, leading to enhanced aerosol scavenging, which ultimately results in an increase in SSA and MACBC.

54 ENVIRONMENTAL SCIENCES↗

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗

Impacts of sea ice leads on sea salt aerosols and atmospheric chemistry in the Arctic

Abstract. The processes contributing to Arctic cold-season (November–April) sea salt aerosols (SSAs) remain uncertain. Observations from coastal Alaska suggest that emissions from open leads in sea ice, which are not included in climate models, may play a dominant role. Their Arctic-wide significance has not yet been quantified. Here, we create an emission parameterization of SSAs from leads by combining satellite data of lead area (the Advanced Microwave Scanning Radiometer–Earth Observation System (AMSR-E) product) and a chemical transport model (GEOS-Chem) to quantify pan-Arctic SSA emissions from leads during the cold season from 2002 to 2008 and to predict their impacts on atmospheric chemistry, evaluating the results of our simulated SSAs against in situ observations. The AMSR-E product detects large leads with certainty (> 3 km in size), and, hence, our study is limited to quantifying emissions from large leads. Lead emissions vary seasonally and interannually. Simulated total monthly SSA emissions increase by 1.1 %–1.8 % (≥60° N latitude) and 5.6 %–7.5 % (≥75° N) for the 2002–2008 cold seasons. SSA concentrations primarily increase at the location of leads, where standard model concentrations are low. GEOS-Chem overestimates SSA concentrations at Arctic sites compared to ground observations, even when lead emissions are not included, suggesting underestimation of SSA sinks and/or uncertainties in SSA emissions from blowing snow and the open ocean. Multi-year monthly mean surface bromine atom (Br) concentrations increase by 2.8 %–8.8 % due to SSAs from leads for the 2002–2008 cold seasons. Changes in ozone concentrations are negligible. While leads contribute < 10 % to Arctic-wide SSA emissions in the years 2002–2008, these emissions occur in regions of low background aerosol concentrations. Leads may increase in frequency under future climate change, which could increase SSA emissions from leads.

Emme, Erin J. (ORCID:0000000268406352)↗

Sea spray aerosol production flux retrieval based on Doppler lidar measurements

Supermicron sea spray aerosols (SSA) play a crucial role in stratocumulus cloud microphysics and drizzle formation. However, our understanding of SSA's spatiotemporal distribution, production mechanisms, and fluxes in the marine boundary layer remains limited. This study introduces a novel approach to determine supermicron SSA production flux and number concentration at various heights above the ocean surface. Our method leverages Doppler lidar data, specifically attenuated backscatter and vertical velocity, collected at a 105 m range gate during the Eastern Pacific Clouds and Aerosols for Precipitation Experiment (EPCAPE) at Scripps Pier, La Jolla, California. To focus on nascent SSA, we analyzed data from periods with wind directions between 225° and 315° and wind speeds exceeding 4 m s −1 . Cloud and precipitation events were excluded using relative humidity, backscatter thresholds, and 2D Video Disdrometer observations. Results show that calculated supermicron SSA number concentrations at 105 m ranged from 0.26 to 2.93 cm −3 for surface wind speeds between 4 and 6 ms −1 . When exceeding the method's Limit of Detection, estimated production fluxes ranged from 0.20 to 1.53 cm −2 s −1 . This methodology has potential for application in various oceanic locations, likely enhancing our understanding of SSA's role in atmospheric processes and climate interactions.

54 ENVIRONMENTAL SCIENCES↗

Ice-nucleating agents in sea spray aerosol identified and quantified with a holistic multimodal freezing model

Sea spray aerosol (SSA) is a widely recognized important source of ice-nucleating particles (INPs) in the atmosphere. However, composition-specific identification, nucleation processes, and ice nucleation rates of SSA-INPs have not been well constrained. Microspectroscopic characterization of ambient and laboratory-generated SSA confirms that water-borne exudates from planktonic microorganisms composed of a mixture of proteinaceous and polysaccharidic compounds act as ice-nucleating agents (INAs). These data and data from previously published mesocosm and wave channel studies are subsequently used to further develop the stochastic freezing model (SFM) producing ice nucleation rate coefficients for SSA-INPs. The SFM simultaneously predicts immersion freezing and deposition and homogeneous ice nucleation by SSA particles under tropospheric conditions. Predicted INP concentrations agree with ambient and laboratory measurements. In addition, this holistic freezing model is independent of the source and exact composition of the SSA particles, making it well suited for implementation in cloud and climate models.

54 ENVIRONMENTAL SCIENCES↗

Shoreline wave breaking strongly enhances the coastal sea spray aerosol population: Climate and air quality implications

Sea spray aerosol (SSA) emission is a major source of atmospheric aerosols, influencing global climate and coastal air quality. Much of our knowledge about SSA derives from coastal observations near shorelines, but whether and when these observations accurately represent open oceans remain unclear. Here, we show that strong nearshore SSA production during high-wave periods greatly enhances downwind cloud condensation nuclei (CCN) and aerosol mass concentrations. Strong shoreline wave breaking is widespread globally, and swell waves, which are decoupled from local winds, play a dominant role in many coastal regions. Therefore, extrapolating results based on coastal measurements to open oceans may significantly overestimate SSA concentration and its contribution to CCN and, by extension, the impact of SSA on clouds and climate. Additionally, the strong enhancement of coastal aerosol population by shoreline wave breaking and its environmental impact on coastal communities cannot be captured by current regional models, which do not parameterize nearshore SSA generation using wave energy or completely neglect it.

54 ENVIRONMENTAL SCIENCES↗

Marine aerosol generation experiments in the High Arctic during summertime

The rapidly warming Arctic has transitioned to thinner sea ice which fractures, producing leads. Few studies have investigated Arctic sea spray aerosol (SSA) produced from open ocean, leads, and melt ponds, which vary in salinity and organic and microbial community composition. A marine aerosol reference tank was deployed aboard an icebreaker to the Arctic Ocean during August–September 2018 to study SSA generated from locally collected surface waters. Aerosol generation experiments were carried out using water collected from the marginal ice zone, a human-made hole in sea ice near the North Pole, and both lead and melt pond water during an ice floe drift period. Salinity, chlorophyll a, organic carbon, nitrogen, and microbial community composition were measured. Eukaryotic plankton and bacterial abundance were elevated in experimental water from the marginal ice zone, but the relative contributions from major eukaryotic taxonomic groups varied little across the experiments. The chemical composition of individual SSA particles was analyzed using Raman microspectroscopy and computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy. Individual sea salt aerosol, primary organic aerosol, and mineral dust particles were observed. Sea salt aerosol constituted 44–95% of individual submicrometer and 68–100% of supermicrometer particles, by number, generated during each experiment. Carbon was detected in 85%, by number, of the individual sea salt particles, with visible organic coatings. Carbohydrates were detected in 72% of particles, by number, with smaller contributions from long-chain fatty acids (13%) and siliceous material (15%). SSA generated from melt pond water contained only long-chain fatty acids and siliceous material. Quantification of the ice-nucleating activity showed that locally produced SSA may define the High Arctic background ice-nucleating particle population, but cannot account for the peak atmospheric concentrations observed. As the Arctic warms, the increasing SSA emissions have a complex dependence on changing biological and physical processes.

54 ENVIRONMENTAL SCIENCES↗

On the relation between the subadditivity cone and the quantum entropy cone

Given a multipartite quantum system, what are the possible ways to impose mutual independence among some subsystems, and the presence of correlations among others, such that there exists a quantum state which satisfies these demands? This question and the related notion of a pattern of marginal independence (PMI) were introduced in [1], and then argued in [2] to be central in the derivation of the holographic entropy cone. Here we continue the general information theoretic analysis of the PMIs allowed by strong subadditivity (SSA) initiated in [1]. We show how the computation of these PMIs simplifies when SSA is replaced by a weaker constraint, dubbed Klein’s condition (KC), which follows from the necessary condition for the saturation of subadditivity (SA). Formulating KC in the language of partially ordered sets, we show that the set of PMIs compatible with KC forms a lattice, and we investigate several of its structural properties. One of our main results is the identification of a specific lower dimensional face of the SA cone that contains on its boundary all the extreme rays (beyond Bell pairs) that can possibly be realized by quantum states. We verify that for four or more parties, KC is strictly weaker than SSA, but nonetheless the PMIs compatible with SSA can easily be derived from the KC-compatible ones. For the special case of 1-dimensional PMIs, we conjecture that KC and SSA are in fact equivalent. To make the presentation self-contained, we review the key ingredients from lattice theory as needed.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗