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At least 613 records · Page 34

Distinct Fracture Mineralogy That is Out of Equilibrium With Modern Groundwaters Provides Important Context for Subsurface Life

Rock fracture surfaces in the crust are essential habitat for microorganisms. Fracture‐groundwater interfaces provide physical substrates for biofilm growth and are sources of carbon, nutrients, and electron donors and acceptors. To better understand geochemical processes impacting fracture surfaces and the subsurface microbiome, we identified fractures in archived rock cores from the Soudan formation, which is known to host saline groundwaters and isolated microbial communities dependent on rock‐water interactions. Cores with open fractures were thin sectioned and studied via electron microprobe and synchrotron X‐ray fluorescence microprobe. Most fracture surfaces had mineralogy distinct from that of the bulk rock. Chlorite minerals were abundant on fracture surfaces and had elemental compositions suggesting deposition during late‐stage hydrothermal alteration. Fracture‐lining chlorites likely limit access to iron oxide and sulfide minerals that are active in subsurface biogeochemical cycles. Calcium‐rich rinds were also observed along fracture edges. These rinds were too thin and poorly ordered to be identified via light microscopy or X‐ray diffraction; however, Ca K‐edge micro‐X‐ray absorption near‐edge structure spectroscopy identified them as carbonates, minerals not observed in the bulk rock. Thermodynamic modeling shows that carbonate precipitation is largely unfavorable in Soudan groundwaters, indicating that fracture edge conditions differed from those in modern water samples. Because of the low carbon concentrations in Soudan groundwaters, carbonate rinds likely play an important role in subsurface carbon cycling and may mark fracture surfaces that once hosted biofilms. Overall, this study suggests that fracture alteration can both play an active role in and suppress rock‐water interactions essential to subsurface life.

36 MATERIALS SCIENCE↗

Co-treating flue gas desulfurized effluent and produced water enables novel waste management and recovery of critical minerals

Herein this study reports a novel approach of resource recovery from co-managing two geographically co-located and chemically complementary wastewaters using a pilot-scale treatment process. Designed to treat flue gas desulfurized (FGD) effluent from combustion powerplants and produced water (PW) from energy industries, the process consists of soda-ash softening, nanofiltration (NF), and reverse osmosis (RO). Recovered products are barite, calcite, and low-salinity water. Using field-collected waters, the results show that softening at pH 8.5 produces calcite (yield: 30 kg/m 3 treated water), a chemical used as SO ₂(g) scrubbers. NF treatment under an applied pressure of 3.5 MPa yields a permeate stream laden with monovalent ions (water recovery 60%) and a concentrate stream with a sulfate concentration 1.8 times of the feedwater concentration. Mixing the NF concentrate and PW at a volumetric ratio of 1.0 precipitates a high-density barite material (4.1 g/cm 3 , yield: ~7.5 kg/m 3 mixture) – a critical mineral commonly used as a weighting agent in drilling. The RO treatment recovers >64% water as the permeate, which can be readily used as cooling make-up water at the powerplants. The RO concentrate stream can be further processed in a thermal evaporative system for additional water recovery and brine production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The reaction between metakaolin and limestone and its effect in porosity refinement and mechanical properties

In limestone calcined clay cements (LC{sup 3}), more hemicarboaluminate and monocarboaluminate is observed, as compared to other blended cements, from the reaction of metakaolin with limestone. In this study, it is shown that the formation of these carboaluminate phases, predominantly occurs during a “third” hydration peak, after the main alite and aluminate peaks. The influence of the metakaolin content, level of sulfate addition and the water to binder ratio on the position and magnitude of this peak were investigated. This precipitation of hemi and monocarboaluminate has a significant effect on porosity refinement and strength development. It was also observed that alumina from metakaolin can contribute to the precipitation of ettringite if sufficient sulfate is available.

36 MATERIALS SCIENCE↗

Linking water quality, fouling layer composition, and performance of reverse osmosis membranes

Fouling of polyamide membranes during reverse osmosis (RO) is a major challenge for adopting membrane technologies to treat highly contaminated waters, especially those containing organic foulants (e.g., natural organic matter (NOM), polysaccharides) and dominant cations (e.g., sodium, magnesium, calcium). Here, this work combines bench-scale membrane fouling experiments with detailed characterization of feedwater chemistry and fouling layer composition/morphology to reveal fundamental mechanisms of (in)organic fouling during RO. Divalent cations are shown to promote fouling by hydrophobic NOM containing aromatic and carboxyl groups, while NOM fouling in the presence of a monovalent cation, sodium, occurs by smaller fulvic acids containing larger fractions of carboxyl groups and other oxygen-rich moieties. Calcium-carboxyl bridging occurs in solution and near the membrane surface to induce NOM aggregation on nanometer length scales. In complex waters containing foulant mixtures, co-fouling by calcium-carboxyl bridging and CaCO 3 precipitation influence membrane performance at longer timeframes. However, the flux decline observed for the co-fouling mechanism was less significant than the sum of its parts, suggesting both synergistic and antagonistic fouling mechanisms should be considered in membrane design/operation. These results encourage the design of pretreatment processes to reduce concentrations of multivalent ions and hydrophobic NOM in RO feedwaters, and of membrane materials to limit attachment/deposition of aggregates to/on polyamide surfaces.

42 ENGINEERING↗

Snow Reconciles Observed and Simulated Phase Partitioning and Increases Cloud Feedback

The surprising increase of Earth's climate sensitivity in the most recent coupled model intercomparison project (CMIP) models has been largely attributed to extratropical cloud feedback, which is thought to be driven by greater supercooled water in present-day cloud phase partitioning (CPP). Here, we report that accounting for precipitation in the Goddard Institute for Space Studies ModelE3 radiation scheme, neglected in more than 60% of CMIP6 and 90% of CMIP5 models, systematically changes its apparent CPP and substantially increases its cloud feedback, consistent with results using CMIP models. Including precipitation in the comparison with cloud–aerosol lidar and infrared pathfinder satellite observations (CALIPSO) measurements and in model radiation schemes is essential to faithfully constrain cloud amount and phase partitioning, and simulate cloud feedbacks. Our findings suggest that making radiation schemes precipitation-aware (missing in most CMIP6 models) should strengthen their positive cloud feedback and further increase their already high mean climate sensitivity.

54 ENVIRONMENTAL SCIENCES↗

AmeriFlux US-UR1 Boulder - UCRB

This is the AmeriFlux version of the carbon flux data for the site US-UR1 Boulder - UCRB. Site Description - This site is located in Boulder, Wyoming, in a high-altitude grassland ecosystem. The region experiences cold winters and mild summers, with relatively low precipitation throughout the year. Snowfall is common during the winter months, contributing to the seasonal water availability. The landscape is primarily covered by grass vegetation, with some areas supported by a center pivot irrigation system, which helps sustain plant growth in the dry environment.

Neale, C. U. [Daugherty Water for Food Global Inst↗

Predictability and feedbacks of the ocean-soil-plant-atmosphere water cycle: deep learning water conductance in Earth System Model

This white paper responds to Focal Area 2. We seek to build predictive models of leaf and surface conductance of water by implementing deep learning (DL) data assimilation techniques. These new models would then be implemented in existing Land Surface Models (LSMs) and Earth System models (ESMs), generating novel water cycle feedbacks. In doing so, we would improve predictability of expected changes in land precipitation, soil moisture, and vegetation dynamics in the long-term, and the role of land cover on the impacts and feedbacks of extreme weather events in the short-term

54 ENVIRONMENTAL SCIENCES↗

Storm and Annual Time Scale Hydrological Data for the Russian River Watershed 1996-2022

These files contains observed and simulated hydrological data (discharge, precipitation) that have been aggregated to the storm-event scale and to the annual time scale for the Russian River Watershed (RRW), California. Observed data are obtained from 12 different USGS hydrological stations located throughout the watershed, and discharge is simulated using the GR5H hourly hydrological model. Precipitation data are obtained from the NASA NLDAS NOAH Community Land Surface Model. All simulated and observed discharge are aggregated to the storm and annual time scales. We investigated changes in watershed hydrological conditions in the Russian River Watershed, a Mediterranean, drought prone, wildfire-adapted ecosystem, following eleven wildfires that occurred from 2017-2020. We ask two research questions: 1) How do interacting wildfire events, drought, and atmospheric rivers impact hydrological conditions of the watershed and in particular streamflow?, and 2) What percentage of new and/or cumulative wildfire disturbance is required to initiate hydrological change? We hypothesize that sub-watersheds of the RRW Mediterranean ecoregion have not burned beyond an intrinsic, and still unknown, threshold required to initiate change. Using a series of paired burned/unburned catchments nested within the larger watershed, we examined temporal and spatial patterns of pre-and-post wildfire water hydrology using a rainfall runoff hydrological model compared with data.

54 ENVIRONMENTAL SCIENCES↗

Electrically Powered High-Salinity Brine Separation Using Dimethyl Ether

Dewatering highly saline aqueous streams, from mining and geothermal leachates to industrial wastewater, is essential for effective resource recovery and safe disposal. Membraneless water extraction (MWE) uses a low-polarity solvent to separate water from concentrated aqueous solutions. In this study, we design a new MWE that uses dimethyl ether (DME) to selectively extract water from high-salinity brines, leveraging the volatility of DME to achieve rapid solvent recovery. By separating water and dissolved salts at a liquid–liquid interface, MWE minimizes the deleterious effects of scaling on vulnerable membrane and heat exchanger surfaces, reducing the need for extensive pretreatment and expensive materials. We begin by developing a computational framework for a multistage counterflow liquid–liquid contactor, which extracts water into DME, coupled with a multistage solvent regenerator that uses vapor compression to efficiently separate the desalinated water from the DME extractant. Excess Gibbs free energy and equation of state frameworks are used to model fluid phase equilibria in water–DME–sodium chloride (NaCl) mixtures, with interaction parameters estimated from experimental data. Incorporating equilibrium calculations into a system-scale computational model, we examine the performance of MWE using DME for the first time. Our analysis demonstrates that MWE can concentrate seawater desalination brine (>1.0 mol NaCl kg –1 ) to zero-liquid discharge salinities, with an energy consumption of under 50 kW h per m 3 of water extracted with a solvent recovery ratio greater than 99.9%. We highlight the importance of staging the vapor compression process to simultaneously minimize energy consumption while enabling brine concentration and product water solvent contamination. Finally, the thermodynamic framework developed here allows for the robust evaluation of new MWE solvents and systems for critical brine concentration and fractional precipitation applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Data for: Spatial access and resource limitations control carbon mineralization in soils

This dataset contains data and code used for the paper "Spatial access and resource limitations control carbon mineralization in soils", https://doi.org/10.1016/j.soilbio.2021.108427. Core-scale soil carbon fluxes are ultimately regulated by pore-scale dynamics of substrate availability and microbial access. These are constrained by physicochemical and biochemical phenomena (e.g. spatial access and hydrologic connectivity, physical occlusion, adsorption-desorption with mineral surfaces, nutrient and resource limitations). We conducted an experiment to determine how spatial access and resource limitations influence core-scale water-soluble soil organic matter (SOM) mineralization, and how these are regulated by antecedent moisture conditions. Intact soil cores were incubated at field-moist vs. drought conditions, after which they were saturated from above (to simulate precipitation) or below (to simulate groundwater recharge). Soluble carbon (acetate) and nitrogen (nitrate) forms were added to some cores during the rewetting process to alleviate potential nutrient limitations. Soil respiration was measured during the incubation, after which pore water was extracted from the saturated soils and analyzed for water soluble organic carbon concentrations and characterization. Our results showed that carbon (C) amendments increased the cumulative carbon dioxide (CO2) evolved from the soil cores, suggesting that the soils were C-limited. Drought and rewetting increased soil respiration, and there was a greater abundance of complex aromatic molecules in pore waters sampled from these soils. This newly available substrate appeared to alleviate nutrient limitations on respiration, because there were no further respiration increases with subsequent C and N amendments. We had hypothesized that respiration would be influenced by wetting direction, as simulated precipitation would mobilize C from the surface. However, as a main effect, this response was seen only in the C-amended soils, indicating that surface-C may not have been bioavailable. At the pore scale (pore water samples), drought and the C, N amendments caused a net loss of identified molecules when the soils were rewet from below, whereas wetting from above caused a net increase in identified molecules, suggesting that fresh inputs stimulated the C-and N-limited microbial populations present deeper in the soil profile. Our experiment highlights the complex and interactive role of antecedent moisture conditions, wetting direction, and resource limitations in driving core-scale C fluxes.This dataset contains a compressed (.zip) archive of the data and R scripts used for this manuscript. The dataset includes files in .csv format, which can be accessed and processed using MS Excel or R. This archive can also be accessed on GitHub at https://github.com/kaizadp/TES_spatial_access_2021 (DOI: 10.5281/zenodo.5522938).

54 ENVIRONMENTAL SCIENCES↗

Science Area 1: Standard Award: Model-Data Fusion to Examine Multiscale Dynamical Controls on Snow Cover and Critical Zone Moisture Inputs (Final Report)

In many mountain watersheds of the world, seasonal snowpacks play an important role as natural reservoirs of water. Seasonal snowpacks accumulate water during cold, wet winter months that subsequently melts. Downstream communities depend on water from melting seasonal snowpacks to support agricultural, industrial, and municipal water needs. Rapidly melting snowpacks can also present a flooding hazard, particularly if snowpacks melt at rates faster than anticipated and where adequate reservoir capacity is unavailable to buffer river flows associated with melt. The spatial and temporal dynamics of snow accumulation and melt also play an important role in supporting upland ecosystems in mountain landscapes. Snowmelt provides soil moisture that enable terrestrial ecosystem productivity and exert control on soil microorganisms that play important roles in global carbon cycles. Climate warming is gradually decreasing the amount of precipitation in mountain watersheds arriving as snow, presenting potentially profound disruptions to mountain ecosystems, as well as downstream delivery of water. The overarching goal of this project was to understand how interactions between the near-surface atmosphere and surface topography control the input, accumulation, retention, and release of water from mountain snowpacks. Over a 5-year period, this project pursued an approach combining high-resolution regional climate modeling, satellite and airborne remote sensing data, and ground-based observations to develop and analyze benchmark datasets to address overarching science questions and hypotheses. Key products include a continuous, long-term, high spatiotemporal resolution (1 km/1 hr) dataset characterizing key climate variables in the Upper Colorado River Basin. The dataset included historical estimates of precipitation, temperature, humidity, solar and longwave radiation, and wind speeds. Additionally, the project developed a 20+ year long, 30 m spatial, daily temporal multi-sensor dataset characterizing snow presence/absence in the East/Taylor River watersheds in the Central Rocky Mountains of Colorado. The project supported training of 1 postdoctoral scholar, 1 Ph.D. student, and 1 M.S. student.

54 ENVIRONMENTAL SCIENCES↗

Redox-Based Electrochemical Affinity Sensor for Detection of Aqueous Pertechnetate Anion

Rapid, selective, in-situ detection of TcO4- in multicomponent matrices consisting of interfering anions such as the ubiquitous NO3- and Cl- or the isostructural and isoelectronic CrO42- is challenging. Present sensors mostly lack the selectivity to exclude these interferences, or the sensitivity to meet the detection limits that are lower than the drinking water standards across the globe. This work presents an affinity based electrochemical sensor for TcO4- detection that relies on selective reductive precipitation of aqueous TcO4- induced by a capture probe immobilized on an electrode platform. This results in a direct decrease of the electron transfer current, the magnitude of the decrease being proportional to the amount of TcO4- added. Using this approach, we were able to achieve a detection limit of 1x10-10 M, which is lower than the drinking water standard of 5.2x10-10 M set by United States Environmental Protection Agency. Our proposed approach also allowed us to detect TcO4- from a multicomponent groundwater sample obtained from a well at the Hanford site in Washington (well 299-W19-36) that also contained NO3- , Cl- and CrO42-, without discernably affecting the detection limits.

Chatterjee, Sayandev↗

Dispersible Colloid Facilitated Release of Organic Carbon From Two Contrasting Riparian Sediments

In aqueous systems, including groundwater, nano-colloids (1–100 nm diameter) and small colloids (<450 nm diameter) provide a vast store of surfaces to which organic carbon (OC) can sorb, precluding its normal bioavailability. Because nanomaterials are ubiquitous and abundant throughout Earth systems, it is reasonable that they would play a significant role in biogeochemical cycles. As such, mineral nano-colloids (MNC) and small colloids, formed through mineral weathering and precipitation processes, are both an unaccounted-for reservoir and unquantified vector for transport of OC and nutrients and contaminants within watersheds. Water extractions and leaching experiments were conducted under (1) aerobic (ambient) and (2) anaerobic (environmental chamber) conditions for each of two contrasting riparian sediments from (1) Columbia River, Washington and (2) Tims Branch, South Carolina. Water dispersible colloid-adsorbed OC was as high as 48% of OC for Tims Branch anaerobic batch water extraction and as low as 0% for Columbia River aerobic batch water extractions. Anaerobic leaching from column experiments yielded higher colloid and OC release rates. Transmission electron microscopy with electron dispersive spectroscopy mapping revealed organic carbon associated with aggregations of nano-particulate silicate minerals and Mossbauer identified nano-particulate goethite. This exploratory study demonstrates that mineral facilitated release of OC in riparian sediments is both significant and variable between locations.

Rod, Kenton A.↗

Upwind Moisture Controls on Interannual Variations of Precipitation and Vegetation in China's Drylands

Dryland precipitation depends on upwind and local moisture sources via moisture recycling. How upwind moisture variations affect interannual variations of downwind precipitation and vegetation in China's drylands remains unclear. We used high-resolution moisture tracking data sets and found terrestrial moisture (93%) was the dominant moisture source for China's drylands, especially from drylands themselves (46%). In most dryland grids, we observed strong correlations between precipitation and upwind moisture sources from 2003 to 2022 (median r = 0.55), with a more significant effect in drier areas. These demonstrated the upwind moisture control on interannual variations of dryland precipitation, in which internal moisture from drylands exceeds the influence of external terrestrial sources. The upwind moisture variations, especially the recycled moisture of drylands, propagate to influence downwind vegetation greenness in precipitation-sensitive dryland areas. Our findings revealed that upwind moisture variations induced by climate or land-cover changes have important implications for water and food security in China's drylands.

54 ENVIRONMENTAL SCIENCES↗

Chemical and isotopic evolution of flowback fluids from the Utica Gas Shale Play, Eastern Ohio USA

For this work, hydraulic fracturing flowback fluids were collected from two Utica/Point Pleasant well pads in eastern Ohio. One site was in the wet gas zone (UPPW), while the site ~50 km south consisted of four wells on the same pad in the dry gas zone (UPPS). Samples of input fluids also were collected before and during hydraulic fracturing. Flowback fluids are Na-Ca-Cl brines with total dissolved salt (TDS) concentrations that increase over several months from ~100 to 200 g/L. The slightly higher TDS of the dry gas fluids are in part due to recycled flowback used as input fluids, and in part due to lower volume of water used in hydraulic fracturing. Concentrations of most major ions (Ca 2+ , Mg 2+ , Na + , Sr2 + , Fe, Mn, Cl – , Br – ) are similar for the five wells sampled, although small but systematic changes occur in the major element ratios over time. Most notably, an increase in the Sr/Cl ratio corresponds to an increase in the 87 Sr/ 86 Sr ratio in the fluids, suggesting interactions with a more radiogenic Sr source in the subsurface. Dissolved Ba concentrations and Ra activities were different between the two sites, reflecting a high SO 4 2– fluid used at the UPPW site, and water-rock reactions occurring during hydraulic fracturing at the UPPS site. Water oxygen (δ 18 O) and hydrogen (δD) isotopes for input fluids used in the UPPW4 well and fresh water used for the UPPS wells fall on the Global Meteoric waterline (GMWL). Flowback fluids from both sites are relatively enriched in δ 18 O and δD compared to the input, but do not appear to follow a simple mixing trend, suggesting reaction and isotopic exchange with carbonates and fractionation due to imbibition in the rock. Cl isotopes, δ 37 Cl in the FP fluids varied from ~ –0.43 to +0.13‰, the largest variation was observed in the earlier stages of flowback, while in the later stages δ 37 Cl exhibited a small but systematic increase over time, suggesting diffusion control of isotopic composition. Some of the trace species measured (dissolved Fe, Mn, thiosulfate and organic acids) do not follow the same trends as the major ions, suggesting contributions from input fluids, or microbially mediated reactions are exerting control on their concentrations. Input water chemistry exerts an important control on the Sr and Ba concentrations in flowback water. High SO 4 2– in the input fluids used for hydraulically fracturing the wet gas well leads to precipitation of barite-celestite in flowback fluids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tree water uptake patterns across the globe

Plant water uptake from the soil is a crucial element of the global hydrological cycle and essential for vegetation drought resilience. Yet, knowledge of how the distribution of water uptake depth (WUD) varies across species, climates, and seasons is scarce relative to our knowledge of aboveground plant functions. With a global literature review, we found that average WUD varied more among biomes than plant functional types (i.e. deciduous/evergreen broadleaves and conifers), illustrating the importance of the hydroclimate, especially precipitation seasonality, on WUD. By combining records of rooting depth with WUD, we observed a consistently deeper maximum rooting depth than WUD with the largest differences in arid regions – indicating that deep taproots act as lifelines while not contributing to the majority of water uptake. The most ubiquitous observation across the literature was that woody plants switch water sources to soil layers with the highest water availability within short timescales. Hence, seasonal shifts to deep soil layers occur across the globe when shallow soils are drying out, allowing continued transpiration and hydraulic safety. While there are still significant gaps in our understanding of WUD, the consistency across global ecosystems allows integration of existing knowledge into the next generation of vegetation process models.

54 ENVIRONMENTAL SCIENCES↗

Peatland hydrology across scale: a probabilistic framework for confronting variability, heterogeneity, and uncertainty (Final Report)

Our project aimed to guide the representations of peatland hydrology and water-carbon feedbacks within Earth System Models, by improving process understanding and developing parsimonious models that elucidate the effects of hydroclimatic variability and spatial heterogeneity. Our research questions centered on the three key drivers of peatland hydrology: (1) seasonal and interannual hydroclimatic fluctuations, (2) spatial heterogeneity of peatland microtopography, and (3) hydrological connectivity across landscape units within a peatland watershed. Our analyses and model testing used existing long-term datasets within the Marcell Experimental Forest (MEF), with new data collected whenever necessary. To date, we have demonstrated the strong influence of water table elevations on the temperature sensitivity of CH 4 emissions, using a newly developed eddy covariance dataset spanning eleven years at MEF. Specifically, higher water tables dampen the increase in CH 4 emissions in the spring as well as their decrease in the fall, resulting in hysteresis. These results imply that any hydroclimatological changes in peatlands that shift seasonal water availability from winter to summer will increase annual CH 4 emissions, even if soil temperature remains unchanged. To further investigate water table elevation change within the peatland microtopography, we installed automated water table gauges across four bog-forest transects (the “lagg”) in two peatland watersheds at MEF, which are hotspots of intense biogeochemical activity. These measurements will give us new information about the extent of lagg expansion and contraction during snowmelt and high intensity rainfall events, as well as the directionality of water and nutrient flow into the bog from the surrounding forests. Finally, we investigated the hydrological connectivity across the peatland watershed complex during early spring – a critical period where water table is elevated from snowmelt – using extended hydrological records from MEF (e.g., snow and frost depths, water table elevations, streamflow). The importance of thermal and wintertime processes within the Energy Exascale Earth System Model (E3SM) was determined through sensitivity analyses. Results from data analyses show that (i) streamflow has decreased over decades likely due to increased evapotranspiration rates (despite no detectable trends in precipitation), (ii) spring streamflow generation is controlled by a sequence of fill-and-spill pathways from the snowpack to the stream through peatland water stores, and (iii) frost depth is a key explanatory variable for the timing and magnitude of streamflow. These results suggest that frost plays an important role in connecting surface water storage in peatlands to stream outlets, and that the hydrological connectivity across the peatland watershed complex can mediate the sensitivity of hydrological responses to climate variations.

54 ENVIRONMENTAL SCIENCES↗

Isolating the effect of biomass burning aerosol emissions on 20th century hydroclimate in South America and Southeast Asia

Abstract Biomass burning is a significant source of aerosol emissions in some regions and has a considerable impact on regional climate. Earth system model simulations indicate that increased biomass burning aerosol emissions contributed to statistically significant decreases in tropical precipitation over the 20th century. In this study, we use the Community Earth System Model version 1 Large Ensemble (CESM1-LENS) experiment to evaluate the mechanisms by which biomass burning aerosol contributed to decreased tropical precipitation, with a focus on South America and Southeast Asia. We analyze the all-but-one forcing simulations in which biomass burning aerosol emissions are held constant while other forcings (e.g., greenhouse gas concentrations) vary throughout the 20th century. This allows us to isolate the influence of biomass burning aerosol on processes that contribute to decreasing precipitation, including cloud microphysics, the radiative effects of absorbing aerosol particles, and alterations in regional circulation. We also show that the 20th century reduction in precipitation identified in the CESM1-LENS historical and biomass burning experiments is consistent across Coupled Model Intercomparison Project Phase 5 models with interactive aerosol schemes and the CESM2 single-forcing experiment. Our results demonstrate that higher concentrations of biomass burning aerosol increases the quantity of cloud condensation nuclei and cloud droplets, limiting cloud droplet size and precipitation formation. Additionally, absorbing aerosols (e.g., black carbon) contribute to a warmer cloud layer, which promotes cloud evaporation, increases atmospheric stability, and alters regional circulation patterns. Corresponding convectively coupled circulation responses, particularly over the tropical Andes, contribute to further reducing the flow of moisture and moisture convergence over tropical land. These results elucidate the processes that affect the water cycle in regions prone to biomass burning and inform our understanding of how future changes in aerosol emissions may impact tropical precipitation over the 21st century.

Environmental Sciences & Ecology↗