Individual atmospheric particles can contain mixtures of primary organic aerosol (POA), secondary organic aerosol (SOA), and secondary inorganic aerosol (SIA). To predict the role of such complex multicomponent particles in air quality and climate, information on the number and types of phases present in the particles is needed. However, the phase behavior of such particles has not been studied in the laboratory, and as a result, remains poorly constrained. Here, we show that POA+SOA+SIA particles can contain three distinct liquid phases: a low-polarity organic-rich phase, a higher-polarity organic-rich phase, and an aqueous inorganic-rich phase. Based on our results, when the elemental oxygen-to-carbon (O:C) ratio of the SOA is less than 0.8, three liquid phases can coexist within the same particle over a wide relative humidity range. In contrast, when the O:C ratio of the SOA is greater than 0.8, three phases will not form. We also demonstrate, using thermodynamic and kinetic modeling, that the presence of three liquid phases in such particles impacts their equilibration timescale with the surrounding gas phase. Three phases will likely also impact their ability to act as nuclei for liquid cloud droplets, the reactivity of these particles, and the mechanism of SOA formation and growth in the atmosphere. These observations provide fundamental information necessary for improved predictions of air quality and aerosol indirect effects on climate.

Tornadoes cause damage, injury, and death when intense winds impact structures. Quantifying the strength and extent of such winds is critical to characterizing tornado hazards. Ratings of intensity and size are based nearly entirely on postevent damage surveys [R. Edwards et al., Bull. Am. Meteorol. Soc. 94, 641–653 (2013)]. It has long been suspected that these suffer low bias [C. A. Doswell, D. W. Burgess, Mon. Weather Rev. 116, 495–501 (1988)]. Here, using mapping of low-level tornado winds in 120 tornadoes, we prove that supercell tornadoes are typically much stronger and wider than damage surveys indicate. Our results permit an accurate assessment of the distribution of tornado intensities and sizes and tornado wind hazards, based on actual wind-speed observations, and meaningful comparisons of the distribution of tornado intensities and sizes with theoretical predictions. We analyze data from Doppler On Wheels (DOW) radar measurements of 120 tornadoes at the time of peak measured intensity. In striking contrast to conventional damage-based climatologies, median tornado peak wind speeds are ∼60 m⋅s⁻¹, capable of causing significant, Enhanced Fujita Scale (EF)-2 to -3, damage, and 20% are capable of the most intense EF-4/EF-5 damage. National Weather Service (NWS) EF/wind speed ratings are 1.2 to 1.5 categories (∼20 m⋅s⁻¹) lower than DOW observations for tornadoes documented by both the NWS and DOWs. Median tornado diameter is 250 to 500 m, with 10 to 15% >1 km. Wind engineering tornado-hazard-model predictions and building wind resistance standards may require upward adjustment due to the increased wind-damage risk documented here.

During the formation of terrestrial planets, volatile loss may occur through nebular processing, planetesimal differentiation, and planetary accretion. We investigate iron meteorites as an archive of volatile loss during planetesimal processing. The carbon contents of the parent bodies of magmatic iron meteorites are reconstructed by thermodynamic modeling. Calculated solid/molten alloy partitioning of C increases greatly with liquid S concentration, and inferred parent body C concentrations range from 0.0004 to 0.11 wt%. Parent bodies fall into two compositional clusters characterized by cores with medium and low C/S. Both of these require significant planetesimal degassing, as metamorphic devolatilization on chondrite-like precursors is insufficient to account for their C depletions. Planetesimal core formation models, ranging from closed-system extraction to degassing of a wholly molten body, show that significant open-system silicate melting and volatile loss are required to match medium and low C/S parent body core compositions. Greater depletion in C relative to S is the hallmark of silicate degassing, indicating that parent body core compositions record processes that affect composite silicate/iron planetesimals. Degassing of bare cores stripped of their silicate mantles would deplete S with negligible C loss and could not account for inferred parent body core compositions. Devolatilization during small-body differentiation is thus a key process in shaping the volatile inventory of terrestrial planets derived from planetesimals and planetary embryos.

Organic matter constitutes a key reservoir in global elemental cycles. However, our understanding of the dynamics of organic matter and its accumulation remains incomplete. Seemingly disparate hypotheses have been proposed to explain organic matter accumulation: the slow degradation of intrinsically recalcitrant substrates, the depletion to concentrations that inhibit microbial consumption, and a dependency on the consumption capabilities of nearby microbial populations. Here, using a mechanistic model, we develop a theoretical framework that explains how organic matter predictably accumulates in natural environments due to biochemical, ecological, and environmental factors. Our framework subsumes the previous hypotheses. Changes in the microbial community or the environment can move a class of organic matter from a state of functional recalcitrance to a state of depletion by microbial consumers. The model explains the vertical profile of dissolved organic carbon in the ocean and connects microbial activity at subannual timescales to organic matter turnover at millennial timescales. The threshold behavior of the model implies that organic matter accumulation may respond nonlinearly to changes in temperature and other factors, providing hypotheses for the observed correlations between organic carbon reservoirs and temperature in past earth climates.

Fires are a major contributor to atmospheric budgets of greenhouse gases and aerosols, affect soils and vegetation properties, and are a key driver of land use change. Since the 1990s, global burned area (BA) estimates based on satellite observations have provided critical insights into patterns and trends of fire occurrence. However, these global BA products are based on coarse spatial-resolution sensors, which are unsuitable for detecting small fires that burn only a fraction of a satellite pixel. We estimated the relevance of those small fires by comparing a BA product generated from Sentinel-2 MSI (Multispectral Instrument) images (20-m spatial resolution) with a widely used global BA product based on Moderate Resolution Imaging Spectroradiometer (MODIS) images (500 m) focusing on sub-Saharan Africa. For the year 2016, we detected 80% more BA with Sentinel-2 images than with the MODIS product. This difference was predominately related to small fires: we observed that 2.02 Mkm² (out of a total of 4.89 Mkm²) was burned by fires smaller than 100 ha, whereas the MODIS product only detected 0.13 million km² BA in that fire-size class. This increase in BA subsequently resulted in increased estimates of fire emissions; we computed 31 to 101% more fire carbon emissions than current estimates based on MODIS products. We conclude that small fires are a critical driver of BA in sub-Saharan Africa and that including those small fires in emission estimates raises the contribution of biomass burning to global burdens of (greenhouse) gases and aerosols.

Natural aerosols in pristine regions form the baseline used to evaluate the impact of anthropogenic aerosols on climate. Sea spray aerosol (SSA) is a major component of natural aerosols. Despite its importance, the abundance of SSA is poorly constrained. It is generally accepted that wind-driven wave breaking is the principle governing SSA production. This mechanism alone, however, is insufficient to explain the variability of SSA concentration at given wind speed. The role of other parameters, such as sea surface temperature (SST), remains controversial. Here, we show that higher SST promotes SSA mass generation at a wide range of wind speed levels over the remote Pacific and Atlantic Oceans, in addition to demonstrating the wind-driven SSA production mechanism. The results are from a global scale dataset of airborne SSA measurements at 150 to 200 m above the ocean surface during the NASA Atmospheric Tomography Mission. Statistical analysis suggests that accounting for SST greatly enhances the predictability of the observed SSA concentration compared to using wind speed alone. Our results support implementing SST into SSA source functions in global models to better understand the atmospheric burdens of SSA.

Terrestrial vegetation and soils hold three times more carbon than the atmosphere. Much debate concerns how anthropogenic activity will perturb these surface reservoirs, potentially exacerbating ongoing changes to the climate system. Uncertainties specifically persist in extrapolating point-source observations to ecosystem-scale budgets and fluxes, which require consideration of vertical and lateral processes on multiple temporal and spatial scales. To explore controls on organic carbon (OC) turnover at the river basin scale, we present radiocarbon (¹⁴C) ages on two groups of molecular tracers of plant-derived carbon—leaf-wax lipids and lignin phenols—from a globally distributed suite of rivers. We find significant negative relationships between the ¹⁴C age of these biomarkers and mean annual temperature and precipitation. Moreover, riverine biospheric-carbon ages scale proportionally with basin-wide soil carbon turnover times and soil ¹⁴C ages, implicating OC cycling within soils as a primary control on exported biomarker ages and revealing a broad distribution of soil OC reactivities. The ubiquitous occurrence of a long-lived soil OC pool suggests soil OC is globally vulnerable to perturbations by future temperature and precipitation increase. Scaling of riverine biospheric-carbon ages with soil OC turnover shows the former can constrain the sensitivity of carbon dynamics to environmental controls on broad spatial scales. Extracting this information from fluvially dominated sedimentary sequences may inform past variations in soil OC turnover in response to anthropogenic and/or climate perturbations. In turn, monitoring riverine OC composition may help detect future climate-change–induced perturbations of soil OC turnover and stocks.