Abstract Reconstructing the source regions of past atmospheric dust preserved in ice remains a challenge in Antarctic glaciology. Until now, different dust properties were obtained by separate techniques and could not be directly correlated at single particle level limiting the dust characterization. Here we apply a novel technique (single particle Inductively Coupled Plasma-Time of Flight Mass Spectrometry) to characterize millions of individual particles in low-volume (< 2 mL) ice samples. We analyzed more than 2,000,000 individual particles smaller than 2.5 µm in 28 discrete samples from Taylor Glacier, coastal East Antarctica, spanning 44—9 kyr BP. We show a glacial-interglacial shift in particle number and mass concentrations, as well as in the elemental and mineralogical compositions. Our observations suggest a common potential dust source area for central and coastal East Antarctica during the Last Glacial Period, followed by a transition to different dominant sources in coastal sites during the Holocene. These changes likely reflect large-scale variations in dust sources, and environmental conditions in the Southern Hemisphere. We have also identified and measured the elemental composition of thousands of volcanic particles < 2.5 µm, indicating occasional tephra deposition from one of the Victoria Land volcanoes around 14.8 kyr BP.

Biomass-burning aerosol (BBA) is emitted by combustion through wildfires and prescribed burns. As BBA contains chromophoric brown carbon, this aerosol increases radiative forcing and drives particle-phase photochemistry such as generation of singlet oxygen (1O2) via photosensitization. By generating 1O2, BBA could contribute to oxidation of atmospheric aerosol constituents and facilitate photobleaching of its brown carbon. Little is known regarding the quantum yield for 1O2 production in the aqueous dissolved fraction of BBA, or the variability of 1O2 production between biomass fuel types and other factors. In this study, the quantum yield of 1O2 photosensitization in aqueous BBA extracts during UVA light exposure was determined using the molecular probe furfuryl alcohol. Quantum yields of 1O2 formation ranged from 1.2-3.4%, and BBA generated by wax myrtle was found to have a significantly higher quantum yield than five other biomass fuels, indicating a possible significant dependence on fuel type in some cases. These values lie in a similar range observed for aquatic dissolved organic matter (DOM), where 1O2 production plays an important role in the fate of aquatic contaminants. No dependence on fuel type was observed in measured BBA steady-state 1O2 concentrations or rates of light absorption. The quantum yield of 1O2 was negatively correlated with absorption at 254 and 300 nm, but no other optical index was found to correlate with 1O2 production. Additionally, dynamic changes to the UV-vis absorption spectrum indicated that optical indices used to predict size and aromaticity of aqueous DOM do not apply to BBA extracts. These results emphasize the importance of BBA photosensitization as an aerosol-phase source of 1O2 decoupled from gas-phase atmospheric oxidants. BBA thus plays a role similar to DOM photosensitization in the aqueous environment, despite differences in their formation, chemical composition, and photochemical properties.

While spICP-MS has been used mainly to measure nanoparticles, it can also be used to measure microparticles. The transport efficiency of nanoparticles is typically independent of their size. However, the transport efficiency of microparticles can be particle size (mass) dependent as well as being dependent on the sample uptake rate and sample introduction system used. To measure both nanoparticles and microparticles a very large linear dynamic range (where signal intensity is linearly proportional to the measured analyte(s) mass within a very short measurement time (∼300 to 500 µs, the width of signals produced by an individual particle)) is needed. Deviations from linearity could occur due to incomplete particle vaporization or from signals that are beyond the instrument's ion detection system linear dynamic range. To characterize and determine the cause of nonlinearity we measured sets of nearly monodisperse engineered SiO2 particles with diameters from 500 to 5000 nm and Au particles with diameters from 60 to 1500 nm. We found that by reducing the sensitivity (up to a factor of 269×) the upper end of the linear dynamic range, in particle size that produced signal intensities that were linearly proportional to the particle (analyte) mass, could be greatly extended. Not surprisingly, reducing the sensitivity increased the minimum size detectable particle. The results are consistent with SiO2 particles as large as 5000 nm being completely vaporized in the ICP.

This study introduces a new method for constructing subdaily land surface temperatures (LSTs) in northern high-latitude areas. The method is based on 1) an integration of observations from multiple satellites-sensors, including Moderate Resolution Imaging Spectroradiometer (MODIS) and Visible Infrared Imaging Radiometer Suite (VIIRS); and 2) the use of swath data to more comprehensively utilize the information content available from overlapping events from each platform within a day. The initial validation phase demonstrated a comparably high performance for LSTs among different products with a root mean square error (RMSE) at approximately 3 degrees C. Subsequently, the results confirmed that more than 23 observations per day at 70 degrees N could be achieved, almost quadrupling the observation frequency achieved with twice-daily LST products combining MODIS and VIIRS. At one of the sample sites, the subdaily LST was clearly identified as a near-hourly temporal variation, and the gaps in the early morning and late afternoon were effectively filled.

It is generally assumed that acidic submicron atmospheric aerosol particles do not constitute a significant sink for nitrous acid (HONO), as this weak acid would remain protonated and volatile, yet the uptake of HONO to larger less acidic particles is unexplored. Experiments on optically tweezed aerosol did not observe HONO gas uptake but instead revealed rapid oxidation of HONO to HNO3 in droplets of initial pH between 0 and 7.75. This oxidation was spontaneous at room temperature with no oxidant added and occurred over a subminute time scale. The reaction is accelerated under acidic conditions of pH < 2. We hypothesize that protonated HONO is restricted to the interfacial region while NO2 - is not, and HONO is therefore oxidized to HNO3 following a second-order rate dependence on the HONO concentration. The oxidation of HONO can thus be self-catalyzed in weakly buffered aerosol. Less acidic droplets (pH > 5.0) displayed an approximately 2 orders of magnitude lower conversion rate of HONO to HNO3, likely due to deprotonation and then slower oxidation of NO2 - directly to NO3 - with a first-order dependence on the NO2 - concentration. Production of HNO3 can drive a liquid-liquid phase separation of secondary organic aerosol, but an organic shell phase did not prevent oxidation of HONO to HNO3. This rapid conversion of HONO to HNO3 at the droplet interface due to an acidity-based transition in the reaction mechanism could represent a significant new sink for HONO and a source of strong inorganic acids in the atmosphere that are more readily removed through deposition.

Ice nucleating particles (INP) capable of nucleating ice crystals via immersion freezing at temperatures above approximately −35°C may strongly influence cloud glaciation, with implications for global precipitation and climate feedback. In addition to mineral dust, soil dust, and marine organics, laboratory and field measurements suggest biomass burning aerosols (BBA) can act as immersion‐mode INP between around −30°C and −15°C. However, the contribution of BBA to the global INP budget remains poorly understood due to poor knowledge of which fuels yield INPs, uncertainties in global coverage of those fuels, and unknown size distributions of the INPs in the BBA. Nonetheless, with some understanding of these uncertainties from sensitivity studies, the relative importance of ice nucleation activity of BBA compared to other INP sources can be quantified. In this work, we investigate the potential global importance of BBA as INP using a global aerosol‐climate model, specifically the UK Met Office Unified Model (UM). We evaluate the model using field campaign data sets. We examine potential uncertainties in fuel types and particle sizes on BBA‐based INP concentrations. Averaged over June–September between 15°S and 50°S, BBA is a more important INP than dust and marine INP about 30% of the time at altitudes with temperatures between −30°C and −20°C. Our simulations therefore suggest BBA INPs may be at least as important as mineral dust and marine INP over the atmospheric regions and seasons where grassland fires are frequent.

Processes mediating the coupling of terrestrial, aquatic, biospheric, and atmospheric systems influence weather, climate, and ecosystem dynamics via transfer of energy, momentum, water, and carbon (or other species). These exchange processes are quantified by measurements of near-surface turbulent fluxes. Understanding processes at these interfaces provides insight toward understanding and predicting current and future states within the Earth system. The Atmospheric Radiation Measurement (ARM) user facility has been conducting measurements of near-surface turbulent fluxes since the early 1990s at long-term fixed locations and shorter-term mobile deployments across the Earth. ARM has utilized two established methods for conducting these measurements: energy balance Bowen ratio (EBBR) and eddy covariance (EC). Primary measurements from the former include sensible and latent heat flux, while the latter also measures fluxes of momentum and carbon (primarily carbon dioxide, with methane fluxes measured at two locations to date). The EBBR systems have been deployed at 22 locations, and, to date, the EC systems have been deployed at over 50 sites, with plans for additional novel site locations in the future. Herein, the history, evolution, and key aspects of these instrument systems are documented, along with information on data quality assurance and post-processing, as well as best use practices. Additionally, three data validation experiments were recently conducted, and their key findings are summarized. Finally, ancillary datasets acquired by ARM, which can contextualize and aid interpretation of the near-surface turbulent flux measurements, are discussed. The datasets described herein include the eddy correlation flux measurement system: 30ECOR (10.5439/1879993, Sullivan et al., 1997), 30QCECOR (10.5439/1097546, Gaustad, 2003), ECORSF (10.5439/1494128, Sullivan et al., 2019a), and associated AmeriFlux and Methane Value-Added Product, AMCMETHANE (10.5439/1508268, Billesbach, 2011); the energy balance Bowen ratio system: 30EBBR (10.5439/1023895, Sullivan et al., 1993) and 30BAEBBR (10.5439/1027268, Gaustad and Xie, 1993); and the carbon dioxide flux measurement system: CO2FLX (10.5439/1287574, 10.5439/1287575, 10.5439/1287576, Koontz et al., 2015a, b, c; 10.5439/1989774, 10.5439/1989776, 10.5439/1992202, Biraud and Chan, 2002a, b, c). These data can be found by searching the above data stream names at https://adc.arm.gov/discovery/#/results/ (last access: 8 September 2025).

Carbon-based adsorbents used to remove recalcitrant water contaminants, including perfluoroalkyl substances (PFAS), are often regenerated using energy-intensive treatments that can form harmful byproducts. We explore mechanisms for sorbent regeneration using hydrated electrons (e(aq) -) from sulfite ultraviolet photolysis (UV/sulfite) in water. We studied the UV/sulfite treatment on three carbon-based sorbents with varying material properties: granular activated carbon (GAC), carbon nanotubes (CNTs), and polyethylenimine-modified lignin (lignin). Reaction rates and defluorination of dissolved and adsorbed model perfluorocarboxylic acids (PFCAs), perfluorooctanoic acid (PFOA) and perfluorobutanoic acid (PFBA), were measured. Monochloroacetic acid (MCAA) was employed to empirically quantify e(aq) - formation rates in heterogeneous suspensions. Results show that dissolved PFCAs react rapidly compared to adsorbed ones. Carbon particles in solution decreased aqueous reaction rates by inducing light attenuation, e(aq) - scavenging, and sulfite consumption. The magnitude of these effects depended on adsorbent properties and surface chemistry. GAC lowered PFOA destruction due to strong adsorption. CNT and lignin suspensions decreased e(aq )- formation rates by attenuating light. Lignin showed high e(aq) - quenching, likely due to its oxygenated functional groups. These results indicate that desorbing PFAS and separating the adsorbent before initiating PFAS degradation reactions will be the best engineering approach for adsorbent regeneration using UV/sulfite.

Per- and polyfluoroalkyl substances (PFAS) are a class of ultra-persistent anthropogenic contaminants. PFAS are ubiquitous in environmental and built systems, but very few online methods exist for their characterization in atmospheric gases and aerosols. Iodide time-of-flight chemical ionization mass spectrometry (iodide-ToF-CIMS) is a promising technology for online characterization of PFAS in the atmosphere. Previous work using iodide-ToF-CIMS was successful in measuring gas-phase perfluoroalkyl carboxylic acids and fluorotelomer alcohols, but those are just two of the myriad classes of PFAS that are atmospherically relevant. Therefore, our first objective was to test other sample introduction methods coupled to iodide-TOF-CIMS to evaluate its ability to measure a wider suite of PFAS in both gas and aerosol phases. Using a variety of sample introduction techniques, we successfully measured gas-phase fluorotelomer alcohols (FTOHs), gas and aerosol-phase perfluoroalkyl carboxylic acids (PFCAs), and aerosol-phase perfluoroalkyl sulfonic acids and polyfluoroalkyl phosphoric acid diesters (PFSAs and diPAPs). We also determined iodide-ToF-CIMS response factors for these compounds by introducing known quantities using a Filter Inlet for Gases and AEROsols (FIGAERO). These response factors ranged from 400 to 6 × 104 ions per nanogram, demonstrating low limits of detection. Furthermore, PFAS are a poorly understood diverse class of molecules that exhibit unusual and often unexpected physicochemical properties due to their highly fluorinated nature. Since detection of PFAS with iodide-ToF-CIMS relies on the analyte molecule to either undergo proton transfer or adduct formation with iodide, understanding PFAS behavior during chemical ionization gives rise to a more fundamental understanding of these compounds. Through voltage scanning experiments and DFT calculations, we found that PFCAs and FTOHs readily form iodide adducts, while PFSAs and diPAPs preferentially undergo proton transfer to iodide. Generally, binding energy increased with increasing linear chain length, and PFCAs had stronger binding than FTOHs. Overall, our results suggest that iodide-ToF-CIMS can be used to measure even nonvolatile PFAS such as PFSAs and diPAPs in the aerosol phase in a semi-continuous online fashion.

The science of mountainous hydrology spans the atmosphere through the bedrock and inherently crosses physical and disciplinary boundaries: land-atmosphere interactions in complex terrain enhance clouds and precipitation, while watersheds retain and release water over a large range of spatial and temporal scales. Limited observations in complex terrain challenge efforts to improve predictive models of the hydrology in the face of rapid changes. The Upper Colorado River exemplifies these challenges, especially with ongoing mismatches between precipitation, snowpack, and discharge. Consequently, the U.S. Department of Energy's (DOE) Atmospheric Radiation Measurement (ARM) user facility has deployed an observatory to the East River Watershed near Crested Butte, Colorado, between September 2021 and June 2023 to measure the main atmospheric drivers of water resources, including precipitation, clouds, winds, aerosols, radiation, temperature, and humidity. This effort, called the Surface Atmosphere Integrated Field Laboratory (SAIL), is also working in tandem with DOE-sponsored surface and subsurface hydrologists and other federal, state, and local partners. SAIL data can be benchmarks for model development by producing a wide range of observational information on precipitation and its associated processes, including those processes that impact snowpack sublimation and redistribution, aerosol direct radiative effects in the atmosphere and in the snowpack, aerosol impacts on clouds and precipitation, and processes controlling surface fluxes of energy and mass. Preliminary data from SAIL's first year showcase the rich information content in SAIL's many datastreams and support testing hypotheses that will ultimately improve scientific understanding and predictability of Upper Colorado River hydrology in 2023 and beyond.

Abstract Wetlands are responsible for 20%–31% of global methane (CH4) emissions and account for a large source of uncertainty in the global CH4 budget. Data‐driven upscaling of CH4 fluxes from eddy covariance measurements can provide new and independent bottom‐up estimates of wetland CH4 emissions. Here, we develop a six‐predictor random forest upscaling model (UpCH4), trained on 119 site‐years of eddy covariance CH4 flux data from 43 freshwater wetland sites in the FLUXNET‐CH4 Community Product. Network patterns in site‐level annual means and mean seasonal cycles of CH4 fluxes were reproduced accurately in tundra, boreal, and temperate regions (Nash‐Sutcliffe Efficiency ∼0.52–0.63 and 0.53). UpCH4 estimated annual global wetland CH4 emissions of 146 ± 43 TgCH4 y−1 for 2001–2018 which agrees closely with current bottom‐up land surface models (102–181 TgCH4 y−1) and overlaps with top‐down atmospheric inversion models (155–200 TgCH4 y−1). However, UpCH4 diverged from both types of models in the spatial pattern and seasonal dynamics of tropical wetland emissions. We conclude that upscaling of eddy covariance CH4 fluxes has the potential to produce realistic extra‐tropical wetland CH4 emissions estimates which will improve with more flux data. To reduce uncertainty in upscaled estimates, researchers could prioritize new wetland flux sites along humid‐to‐arid tropical climate gradients, from major rainforest basins (Congo, Amazon, and SE Asia), into monsoon (Bangladesh and India) and savannah regions (African Sahel) and be paired with improved knowledge of wetland extent seasonal dynamics in these regions. The monthly wetland methane products gridded at 0.25° from UpCH4 are available via ORNL DAAC (https://doi.org/10.3334/ORNLDAAC/2253).

Epidemiological data from Europe and North America suggest that 1-1.5% of the adult population 10 has heart failure with reduced left ventricular ejection fraction (HFrEF). Development of edema 11 (pulmonary or systemic) is a major hallmark of heart failure (HF) and a key driver of symptoms, such 12 as exertional dyspnea and fatigue, reduced quality of life, morbidity and mortality (1). 13 Timely identification and treatment of edema are critical strategies in HF management, but are both 14 difficult, for many reasons. A certain degree of peripheral edema is frequent in the elderly, but it 15 might be due to poor mobility or use of treatments such as dihydropyridine calcium channel blockers, The authors declare that the research was conducted in the absence of any commercial or financial 73 relationships that could be construed as a potential conflict of interest. 74

Pollution by chemicals and waste impacts human and ecosystem health on regional, national, and global scales, resulting, together with climate change and biodiversity loss, in a triple planetary crisis. Consequently, in 2022, countries agreed to establish an intergovernmental science-policy panel (SPP) on chemicals, waste, and pollution prevention, complementary to the existing intergovernmental science-policy bodies on climate change and biodiversity. To ensure the SPP's success, it is imperative to protect it from conflicts of interest (COI). Here, we (i) define and review the implications of COI, and its relevance for the management of chemicals, waste, and pollution; (ii) summarize established tactics to manufacture doubt in favor of vested interests, i.e., to counter scientific evidence and/or to promote misleading narratives favorable to financial interests; and (iii) illustrate these with selected examples. This analysis leads to a review of arguments for and against chemical industry representation in the SPP's work. We further (iv) rebut an assertion voiced by some that the chemical industry should be directly involved in the panel's work because it possesses data on chemicals essential for the panel's activities. Finally, (v) we present steps that should be taken to prevent the detrimental impacts of COI in the work of the SPP. In particular, we propose to include an independent auditor's role in the SPP to ensure that participation and processes follow clear COI rules. Among others, the auditor should evaluate the content of the assessments produced to ensure unbiased representation of information that underpins the SPP's activities.

The prevalence of heart failure (HF) with reduced (r) and preserved (p) ejection fraction (EF) continues to rise globally despite current advances in diagnostics and improvements to medical management [...].

Severe viral respiratory diseases, such as SARS-CoV-2, are transmitted through aerosol particles produced by coughing, talking, and breathing. Medical procedures including tracheal intubation, extubation, dental work, and any procedure involving close contact with a patient's airways can increase exposure to infectious aerosol particles. This presents a significant risk for viral exposure of nearby healthcare workers during and following patient care. Previous studies have examined the effectiveness of plastic enclosures for trapping aerosol particles and protecting health-care workers. However, many of these enclosures are expensive or are burdensome for healthcare workers to work with. In this study, a low-cost plastic enclosure was designed to reduce aerosol spread and viral transmission during medical procedures, while also alleviating issues found in the design and use of other medical enclosures to contain aerosols. This enclosure is fabricated from clear polycarbonate for maximum visibility. A large single-side cutout provides health care providers with ease of access to the patient with a separate cutout for equipment access. A survey of medical providers in a local hospital network demonstrated their approval of the enclosure's ease of use and design. The enclosure with appropriate plastic covers reduced total escaped particle number concentrations (diameter > 0.01 μm) by over 93% at 8 cm away from all openings. Concentration decay experiments indicated that the enclosure without active suction should be left on the patient for 15-20 minutes following a tracheal manipulation to allow sufficient time for >90% of aerosol particles to settle upon interior surfaces. This decreases to 5 minutes when 30 LPM suction is applied. This enclosure is an inexpensive, easily implemented additional layer of protection that can be used to help contain infectious or otherwise potentially hazardous aerosol particles while providing access into the enclosure.

Volcanic ash nucleates ice when immersed in supercooled water droplets, giving it the potential to influence weather and climate from local to global scales. This ice nucleation activity (INA) is likely derived from a subset of the crystalline mineral phases in the ash. The INA of other mineral-based dusts can change when exposed to various gaseous and aqueous chemical species, many of which also interact with volcanic ash in the eruption plume and atmosphere. However, the effects of aqueous chemical aging on the INA of volcanic ash have not been explored. We show that the INA of two mineralogically distinct ash samples from Fuego and Astroni volcanoes is variably reduced following immersion in water or aqueous sulfuric acid for minutes to days. Aging in water decreases the INA of both ash samples by up to two orders of magnitude, possibly due to a reduction in surface crystallinity and cation availability accompanying leaching. Aging in sulfuric acid leads to minimal loss of INA for Fuego ash, which is proposed to reflect a quasi-equilibrium between leaching that removes ice-active sites and dissolution that reveals or creates new sites on the pyroxene phases present. Conversely, exposure to sulfuric acid reduces the INA of Astroni ash by one to two orders of magnitude, potentially through selective dissolution of ice-active sites associated with surface microtextures on some Kfeldspar phases. Analysis of dissolved element concentrations in the aged ash leachates shows supersaturation of certain mineral species which could have precipitated and altered the INA of the ash. These results highlight the key role that leaching, dissolution, and precipitation likely play in the aqueous aging of volcanic ash with respect to its INA. Finally, we discuss the implications for understanding the nature and reactivity of ice-active sites on volcanic ash and its role in influencing cloud properties in the atmosphere.

A suite of generally applicable statistical methods based on empirical bootstrapping is presented for calculating uncertainty and testing the significance of quantitative differences in temperature and/or ice active site densities between ice nucleation temperature spectra derived from droplet freezing experiments. Such experiments are widely used to determine the heterogeneous ice nucleation properties and ice nucleation particle concentration spectra of different particle samples, as well as in studies of homogeneous freezing. Our methods avoid most of the assumptions and approximations inherent to existing approaches, and when sufficiently large sample sizes are used (approximately > 150 droplets and >=1000 bootstrap samples in our system), can capture the full range of random variability and error in ice nucleation spectra. Applications include calculation of accurate confidence intervals and confidence bands, quantitative statistical testing of differences between observed freezing spectra, accurate subtraction of the background filtered water freezing signal, and calculation of a range of statistical parameters using data from a single droplet array freezing experiment if necessary. By providing additional statistical tools to the community, this work will improve the quality and accuracy of statistical tests and representations of uncertainty in future ice nucleation research, and will allow quantitative comparisons of the ice nucleation ability of different particles and surfaces.

Despite the importance of high-latitude surface energy budgets (SEBs) for land-climate interactions in the rapidly changing Arctic, uncertainties in their prediction persist. Here, we harmonize SEB observations across a network of vegetated and glaciated sites at circumpolar scale (1994–2021). Our variance-partitioning analysis identifies vegetation type as an important predictor for SEB-components during Arctic summer (June-August), compared to other SEB-drivers including climate, latitude and permafrost characteristics. Differences among vegetation types can be of similar magnitude as between vegetation and glacier surfaces and are especially high for summer sensible and latent heat fluxes. The timing of SEB-flux summer-regimes (when daily mean values exceed 0 Wm −2 ) relative to snow-free and -onset dates varies substantially depending on vegetation type, implying vegetation controls on snow-cover and SEB-flux seasonality. Our results indicate complex shifts in surface energy fluxes with land-cover transitions and a lengthening summer season, and highlight the potential for improving future Earth system models via a refined representation of Arctic vegetation types.

In heart failure with reduced ejection fraction (HFrEF), cardiogenic edema develops from impaired cardiac function, pathological remodeling, chronic inflammation, endothelial dysfunction, neurohormonal activation, and altered nitric oxide-related pathways. Pre-clinical HFrEF studies have shown that treatment with sodium–glucose cotransporter-2 inhibitors (SGLT-2i) stimulates natriuretic and osmotic/diuretic effects, improves overall cardiac function, attenuates maladaptive cardiac remodeling, and reduces chronic inflammation, oxidative stress, and endothelial dysfunction. Here, we review the mechanisms and effects of SGLT-2i therapy on cardiogenic edema in various models of HFrEF. Overall, the data presented suggest a high translational importance of these studies, and pre-clinical studies show that SGLT-2i therapy has a marked effect on suppressing the progression of HFrEF through multiple mechanisms, including those that affect the development of cardiogenic edema.