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DOE OSTI2024

Vacancy-Mediated Increases in Brine–Salt Surface Energies

Salt formations have been explored for the permanent isolation of spent nuclear fuel based on their high thermal conductivity, self-healing nature, and low hydraulic permeability to brine flow. Vacancy defect concentrations in salt complicate fracture mechanics not driven by dislocation dynamics and can influence the resulting surface structure. Classical molecular dynamic simulations were used to simulate tensile testing of salt crystals (halite) with vacancy defect concentrations of up to 0.5 defects/nm 3 . Increasing defect concentrations resulted in a decrease in ultimate tensile strength and fracture surface energies, driven by increased surface roughness rather than changes in the amount of surface area. Brine–salt surface energies of the fractured surfaces were 0.22 to 0.26 J/m 2 , significantly higher than values reported for atomically flat (100) surfaces at the same brine composition. This change in surface energy increased the brine–salt dihedral angle by ~27°. The dihedral angle threshold for percolation in salt is 60°, and a 27° increase due to rough fracture surfaces identifies a reduction in porosity percolation and a decrease in salt permeability. Therefore, bedded salt and salt domes may be even more stable than those previously predicted from dihedral angle calculations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Excitonic Spin-Coherence Lifetimes in CdSe Nanoplatelets Increase Significantly with Core/Shell Morphology

Here, we report spin-polarized transient absorption for colloidal CdSe nanoplatelets as functions of thickness (2–6 monolayer thickness) and core/shell motif. Using electro-optical modulation of co- and cross-polarization pump–probe combinations, we sensitively observe spin-polarized transitions. Core-only nanoplatelets exhibit few-picosecond spin lifetimes that weakly increase with layer thickness. The spectral content of differenced spin-polarized signals indicate biexciton binding energies that decrease with increasing thickness and smaller values than previously reported. Shell growth of CdS with controlled thicknesses, which partially delocalize the electron from the hole, significantly increases the spin lifetime to ~49 ps at room temperature. Implementation of ZnS shells, which do not alter delocalization but do alter surface termination, increased spin lifetimes up to ~100 ps, bolstering the interpretation that surface termination heavily influences spin coherence, likely due to passivation of dangling bonds. Spin precession in magnetic fields both confirms long coherence lifetime at room temperature and yields the excitonic g factor.

2D semiconductor↗

DOE OSTI2026

Synergistic Interactions During Co-Hydrothermal Liquefaction of Food Waste and Biomass Model Compounds for Increased Sustainable Aviation Fuel Production

Hydrothermal liquefaction (HTL) of lignocellulosic biomass is plagued with low biocrude yields owing to the tendency of highly reactive oxygenated intermediates to condense to form biochars. By contrast, the high protein content in food waste is comprised of substantial nitrogen species, which are known to interact strongly with oxygenates through Maillard, amide, and peptide bond formation reactions. Co-feeding food waste and lignocellulose opens new reaction pathways for biocrude formation but is currently poorly understood. This work evaluated the molecular level interactions between food waste and lignocellulose model compounds and the corresponding effect on product yields and quality. Food waste–cellulose and food waste–xylan feedstock blends achieved maximum biocrude carbon yield improvements of 12.2% and 10.1%, respectively, relative to a simple linear model that interpolates between the yields of the pure feedstocks. Increases in biocrude yield were balanced by corresponding decreases in char yield, indicating synergistic interactions between the feeds during HTL. Biocrude volatility analysis revealed that increased biocrude yield preferentially benefitted the jet fuel fraction, which comprised up to 22.6% of the total carbon yield for food waste–cellulose blends. Biocrude and char were analyzed using GC–MS and FT-IR spectroscopy to investigate the source of synergistic trends and provide greater mechanistic understanding. Key cofeeding effects included the promotion of retro-aldol condensation reactions and trans-esterification of fatty acids, sequestering carbon in the biocrude phase via the inhibition of char formation while increasing biocrude volatility toward jet fuel-range compounds. These results indicate the potential for judicious selection of HTL cofeeds to increase both biocrude yield and selectivity to desired fuel precursors, including sustainable aviation fuel.

Maillard reaction↗

DOE OSTI2019

Salmonella Membrane Structural Remodeling Increases Resistance to Antimicrobial Peptide LL-37

Gram-negative bacteria are protected from their environment by an outer membrane that is primarily composed of lipopolysaccharides (LPSs). Under stress, pathogenic serotypes of Salmonella enterica remodel their LPSs through the PhoPQ two-component regulatory system that increases resistance to both conventional antibiotics and antimicrobial peptides (AMPs). Acquired resistance to AMPs is contrary to the established narrative that AMPs circumvent bacterial resistance by targeting the general chemical properties of membrane lipids. However, the specific mechanisms underlying AMP resistance remain elusive. Here we report a 2-fold increase in bacteriostatic concentrations of human AMP LL-37 for S. enterica with modified LPSs. LPSs with and without chemical modifications were isolated and investigated by Langmuir films coupled with grazing-incidence X-ray diffraction (GIXD) and specular X-ray reflectivity (XR). The initial interactions between LL-37 and LPS bilayers were probed using all-atom molecular dynamics simulations. These simulations suggest that initial association is nonspecific to the type of LPS and governed by hydrogen bonding to the LPS outer carbohydrates. GIXD experiments indicate that the interactions of the peptide with monolayers reduce the number of crystalline domains but greatly increase the typical domain size in both LPS isoforms. Here, electron densities derived from XR experiments corroborate the bacteriostatic values found in vitro and indicate that peptide intercalation is reduced by LPS modification. We hypothesize that defects at the liquid-ordered boundary facilitate LL-37 intercalation into the outer membrane, whereas PhoPQ-mediated LPS modification protects against this process by having innately increased crystallinity. Since induced ordering has been observed with other AMPs and drugs, LPS modification may represent a general mechanism by which Gram-negative bacteria protect against host innate immunity.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2011

Pollution from China increases cloud droplet number, suppresses rain over the East China Sea

Rapid economic growth over the last 30 years in China has led to a significant increase in aerosol loading, which is mainly due to the increased emissions of its precursors such as SO 2 and NO x . Here we show that these changes significantly affect wintertime clouds and precipitation over the East China Sea downwind of major emission sources. Satellite observations show an increase of cloud droplet number concentration from less than 200 cm -3 in the 1980s to more than 300 cm -3 in 2005. In the same time period, precipitation frequency reported by voluntary ship observers was reduced from more than 30% to less than 20% of the time. A back trajectory analysis showed the pollution in the investigation area to originate from the Shanghai-Nanjing and Jinan industrial areas. A model sensitivity study was performed, isolating the effects of changes in emissions of the aerosol precursors SO 2 and NO x on clouds and precipitation using a state-of-the-art mesocale model including chemistry and aerosol indirect effects. Similar changes in cloud droplet number concentration over the East China Sea were obtained when the current industrial emissions in China were reduced to the 1980s levels. Simulated changes in precipitation were somewhat smaller than the observed changes but still significant. Citation: Bennartz, R., J. Fan, J. Rausch, L. R. Leung, and A. K. Heidinger (2011), Pollution from China increases cloud droplet number, suppresses rain over the East China Sea, Geophys. Res. Lett., 38, L09704, doi:10.1029/ 2011GL047235.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2012

Unexpected increasing AOT trends over northwest Bay of Bengal in the early postmonsoon season

The main point of our study is that aerosol trends can be created by changes in meteorology without changes in aerosol source strength. Over the 10 year period 2000–2009, in October, Moderate Resolution Imaging Spectroradiometer (MODIS) showed strong increasing aerosol optical thickness (AOT) trends of approximately 14% yr-1 over northwest Bay of Bengal (BoB) in the absence of AOT trends over the east of the Indian subcontinent. This was unexpected because sources of anthropogenic pollution were located over the Indian subcontinent and aerosol transport from the Indian subcontinent to northwest BoB was carried out by prevailing winds. In October, winds over the east of the Indian subcontinent were stronger than winds over northwest BoB, which resulted in wind convergence and accumulation of aerosol particles over northwest BoB. Moreover, there was an increasing trend in wind convergence over northwest BoB. This led to increasing trends in the accumulation of aerosol particles over northwest BoB and, consequently, to strong AOT trends over this area. In contrast to October, November showed no increasing AOT trends over northwest BoB or the nearby Indian subcontinent. The lack of AOT trends over northwest BoB corresponds to a lack of trends in wind convergence in that region. Finally, December domestic heating by the growing population resulted in positive AOT trends of similar magnitude over land and sea. Our findings illustrate that in order to explain and predict trends in regional aerosol loading, meteorological trends should be taken into consideration together with changes in aerosol source strength.

AOT↗

DOE OSTI2019

Why Does Amazon Precipitation Decrease When Tropical Forests Respond to Increasing CO 2 ?

Earth system models predict a zonal dipole of precipitation change over tropical South America, with decreases over the Amazon and increases over the Andes. Much of this has been attributed to the physiological response of the rainforest to elevated CO 2 , which describes a basin-wide reduction in stomatal conductance and transpiration. While robust in Earth system model experiments, details of the underlying atmospheric mechanism—specifically how it evolves in the context of land-atmosphere interaction and the diurnal cycle—are unresolved. We investigate this using idealized model simulations and find that within 24 hr of a CO 2 increase, changes occur over the Amazon that engender synoptic timescale feedbacks. Decreased evapotranspiration from the rainforest throttles near-surface moisture, inducing a drier, warmer, and deeper boundary layer. Above this, enhanced turbulent diffusivity increases vapor in the lower free troposphere. Together, these processes reduce convective activity and cause immediate decreases in Amazon rainfall. Over the synoptic timescale, these changes leave behind lower tropospheric moisture, which is advected westward by the background jet and increases Andean precipitation. This produces a dipole of precipitation change consistent across global and regional models as well as parameterized and resolved convection, though details are sensitive to model topography and boundary layer formulation. The mechanism reported here stresses the importance of fast timescale processes affecting stability over a period of hours that can influence longer-term vegetation-climate interactions. These results help clarify the Amazon's physiological response to rising CO 2 and provide insight into possible causes of historical model biases and end-of-century uncertainty in this region.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Wildfire‐Smoke Aerosols Lead to Increased Light Use Efficiency Among Agricultural and Restored Wetland Land Uses in California's Central Valley

Abstract There are few observational studies measuring the ecosystem‐scale productivity effects of changes in incident diffuse photosynthetically active radiation (PAR diffuse ), especially related to wildfire smoke. Climate change‐induced increases to the duration and intensity of fire conditions have made smoke a common occurrence across western North America, with largely unquantified ecosystem feedbacks. Under equivalent amounts of radiation, increased atmospheric particulate matter could lead to a boost in productivity as scattering redistributes photons throughout multilayer canopies. In this work, we leverage a meso‐network of eddy covariance measurement sites across a unique array of managed and restored C 3 and C 4 canopy types to understand how recent wildfire smoke affected ecosystem productivity during the summer of 2018, an especially smoky year in the agriculturally productive Central Valley. We find that diffuse PAR diffuse increased by more than a third compared to the previous growing season, while total PAR was only slightly diminished. These conditions caused nearly a doubling of light use efficiency over the range of diffuse fraction observed, with the highest sensitivity to diffuse fraction exhibited by corn and alfalfa crops. We utilized an empirical model to assess the trade‐off between enhanced diffuse fraction and reduced total PAR. Under mean radiation conditions, daily integrated gross ecosystem productivity increased by 1.2–4.2% compared to the previous growing season. Finally, we explore the potential negative effect of heightened ozone, a copollutant often associated with wildfire. In addition to the effects of wildfire smoke, the results of this natural experiment can help validate future predictions of aerosol‐productivity feedbacks.

Hemes, Kyle S.↗

DOE OSTI2020

Sensitivity of Atmospheric River Vapor Transport and Precipitation to Uniform Sea Surface Temperature Increases

Abstract Filaments of intense vapor transport called atmospheric rivers (ARs) are responsible for the majority of poleward vapor transport in the midlatitudes. Despite their importance to the hydrologic cycle, there remain many unanswered questions about changes to ARs in a warming climate. In this study we perform a series of escalating uniform SST increases (+2, +4, and +6K, respectively) in the Community Atmosphere Model version 5 in an aquaplanet configuration to evaluate the thermodynamic and dynamical response of AR vapor content, transport, and precipitation to warming SSTs. We find that AR column integrated water vapor (IWV) is especially sensitive to SST and increases by 6.3–9.7% per degree warming despite decreasing relative humidity through much of the column. Further analysis provides a more nuanced view of AR IWV changes: Since SST warming is modest compared to that in the midtroposphere, computing fractional changes in IWV with respect to SST results in finding spuriously large increases. Meanwhile, results here show that AR IWV transport increases relatively uniformly with temperature and at consistently lower rates than IWV, as modulated by systematically decreasing low‐level wind speeds. Similarly, changes in AR precipitation are related to a compensatory relationship between enhanced near‐surface moisture and damped vertical motions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The Mechanism of Increasing Summer Water Vapor Over the Tibetan Plateau

Rapid warming over the Tibetan Plateau (TP) has been associated with a wetting trend in atmospheric water vapor content, which is critical for recharging the Asian water tower. However, the mechanism associated with the wetting phenomenon remains unclear. Long-term changes in moisture balance and precipitation recycling processes are investigated using the ERA5 reanalysis from 1979 to 2019. The wetting trend over TP is mainly due to the summer water vapor trend with signi?cantly increases over the western TP. Based on the moisture balance analysis, it is found that precipitation, evaporation, and the convergence of moisture are all increasing over the western TP but decreasing over the eastern TP. Based on the dynamical precipitation recycling model, the results suggest that both internal and external cycles contributes to the wetting over TP, with 63.87% and 36.13% contributions respectively. Further analysis found that the atmospheric heating source is also increasing over the western TP, which could shift the moisture transportation from east to west at the southern boundary of TP. The increasing moisture convergence could enhance precipitation, and the enhanced latent heating in the mid-atmosphere can further induced moisture convergence, which forms a positive feedback. However, an opposite situation occurred over the eastern TP. The internal and external cycle of the recycling process can stimulate (suppress) each other through precipitation over the western (eastern) TP. This mechanism linked the changes in the precipitation recycling and atmospheric circulation, and induced the wetting trend over TP in summer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Future Hurricanes Will Increase Palm Abundance and Decrease Aboveground Biomass in a Tropical Forest

Hurricanes are expected to intensify throughout the 21st century, yet the impact of frequent major hurricanes on tropical ecosystems remains unknown. To investigate tropical forest damage and recovery under different hurricane regimes, we generate a suite of scenarios based on Coupled Model Intercomparison Project Phase 6 climate projections and increased hurricane recurrence and intensity for the Luquillo Experimental Forest, Puerto Rico. We then use the Ecosystem Demography model to predict changes in carbon stocks, forest structure and composition. In this work, our results indicate that frequent hurricane disturbances in the future would decrease the overall aboveground biomass, decrease the dominance of late-successional species, but increase the dominance of palm species. Warmer climates with increased CO 2 would have little effect on the functional-type composition but increase the aboveground biomass. However, the predicted climate and CO 2 fertilization effects would not compensate for the biomass loss due to more frequent severe-hurricane disturbances.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Dual Impacts of Space Heating Electrification and Climate Change Increase Uncertainties in Peak Load Behavior and Grid Capacity Requirements in Texas

Around 60% of households in Texas currently rely on electricity for space heating. As decarbonization efforts increase, non‐electrified households could adopt electric heat pumps, significantly increasing peak (highest) electricity demand in winter. Simultaneously, anthropogenic climate change is expected to increase temperatures, the potential for summer heat waves, and associated electricity demand for cooling. Uncertainty regarding the timing and magnitude of these concurrent changes raises questions about how they will jointly affect the seasonality of peak demand, firm capacity requirements, and grid reliability. This study investigates the net effects of residential space heating electrification and climate change on long‐term demand patterns and load shedding potential, using climate change projections, a predictive load model, and a direct current optimal power flow (DCOPF) model of the Texas grid. Results show that full electrification of residential space heating by replacing existing fossil fuel use with higher efficiency heat pumps could significantly improve reliability under hotter futures. Less efficient heat pumps may result in more severe winter peaking events and increased reliability risks. As heating electrification intensifies, system planners will need to balance the potential for greater resource adequacy risk caused by shifts in seasonal peaking behavior alongside the benefits (improved efficiency and reductions in emissions).

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2025

Aerosol Decline Accelerates the Increasing Extreme Precipitation in China

Extreme precipitation is becoming more intense and frequent. The increasing trends in extreme precipitation in China in warm season related to changes in aerosols and greenhouse gases (GHGs) are investigated using observations, reanalysis data and model simulations. A significant accelerating increase in extreme precipitation occurred around 2010, with the trend in accumulated extreme rainfall amount (R95pTOT) increasing from 2.88 mm per decade during 2000–2010 to 22.88 mm per decade during 2010–2023. The sudden acceleration of the increasing extreme precipitation is largely attributed to the reverse in aerosol trends associated with China’s clean air actions, which affects extreme precipitation through perturbing cloud microphysics and atmospheric dynamics, accounting for half of the change in R95pTOT trends. Future aerosol reduction to achieve carbon neutrality is shown to continue to intensify the extreme precipitation, which overweighs the effect induced by GHGs, highlighting the importance of aerosol changes in modulating future climate and weather extremes.

58 GEOSCIENCES↗

DOE OSTI2016

Elevated temperature increases carbon and nitrogen fluxes between phytoplankton and heterotrophic bacteria through physical attachment

Quantifying the contribution of marine microorganisms to carbon and nitrogen cycles and their response to predicted ocean warming is one of the main challenges of microbial oceanography. Here we present a single-cell NanoSIMS isotope analysis to quantify C and N uptake by free-living and attached phytoplankton and heterotrophic bacteria, and their response to short-term experimental warming of 4 °C. Elevated temperature increased total C fixation by over 50%, a small but significant fraction of which was transferred to heterotrophs within 12 h. Cell-to-cell attachment doubled the secondary C uptake by heterotrophic bacteria and increased secondary N incorporation by autotrophs by 68%. Warming also increased the abundance of phytoplankton with attached heterotrophs by 80%, and promoted C transfer from phytoplankton to bacteria by 17% and N transfer from bacteria to phytoplankton by 50%. Lastly, our results indicate that phytoplankton-bacteria attachment provides an ecological advantage for nutrient incorporation, suggesting a mutualistic relationship that appears to be enhanced by temperature increases.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Decadal biomass increment in early secondary succession woody ecosystems is increased by CO 2 enrichment

Increasing atmospheric CO 2 stimulates photosynthesis which can increase net primary production (NPP), but at longer timescales may not necessarily increase plant biomass. Here we analyse the four decade-long CO 2 -enrichment experiments in woody ecosystems that measured total NPP and biomass. CO 2 enrichment increased biomass increment by 1.05 ± 0.26 kg C m –2 over a full decade, a 29.1 ± 11.7% stimulation of biomass gain in these early-secondary-succession temperate ecosystems. This response is predictable by combining the CO 2 response of NPP (0.16 ± 0.03 kg C m –2 y –1 ) and the CO 2 -independent, linear slope between biomass increment and cumulative NPP (0.55 ± 0.17). Furthermore an ensemble of terrestrial ecosystem models fail to predict both terms correctly. Allocation to wood was a driver of across-site, and across-model, response variability and together with CO 2 -independence of biomass retention highlights the value of understanding drivers of wood allocation under ambient conditions to correctly interpret and predict CO 2 responses.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Tropical extreme droughts drive long-term increase in atmospheric CO 2 growth rate variability

The terrestrial carbon sink slows the accumulation of carbon dioxide (CO 2 ) in the atmosphere by absorbing roughly 30% of anthropogenic CO 2 emissions, but varies greatly from year to year. The resulting variations in the atmospheric CO 2 growth rate (CGR) have been related to tropical temperature and water availability. The apparent sensitivity of CGR to tropical temperature ( ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ ) has changed markedly over the past six decades, however, the drivers of the observation to date remains unidentified. Here, we use atmospheric observations, multiple global vegetation models and machine learning products to analyze the cause of the sensitivity change. We found that a threefold increase in ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ emerged due to the long-term changes in the magnitude of CGR variability (i.e., indicated by one standard deviation of CGR; STD CGR ), which increased 34.7% from 1960-1979 to 1985-2004 and subsequently decreased 14.4% in 1997-2016. We found a close relationship (r 2 = 0.75, p < 0.01) between STD CGR and the tropical vegetated area (23°S – 23°N) affected by extreme droughts, which influenced 6-9% of the tropical vegetated surface. A 1% increase in the tropical area affected by extreme droughts led to about 0.14 Pg C yr -1 increase in STD CGR . The historical changes in STD CGR were dominated by extreme drought-affected areas in tropical Africa and Asia, and semi-arid ecosystems. The outsized influence of extreme droughts over a small fraction of vegetated surface amplified the interannual variability in CGR and explained the observed long-term dynamics of ${{{{{{\rm{\gamma }}}}}}}_{{{{{{\rm{CGR}}}}}}}^{{{{{{\rm{T}}}}}}}$ .

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2026

Aerosol effective radiative forcing increases Earth’s energy imbalance in recent decades

Earth’s energy imbalance (EEI), a key driver of climate change, has risen markedly over the last two decades. Greenhouse gas forcing, aerosol forcing, and cloud feedback all contribute to this increase. However, the role of aerosol forcing, particularly effective radiative forcing through aerosol-cloud interactions (ERF ACI ), remains highly uncertain and closely intertwined with cloud feedback. Here, we estimate shortwave ERF ACI using satellite observations and show its importance as a contributor to the EEI increase between 2003 and 2023. ERF ACI exhibits a significant increasing trend of 0.33 Wm −2 /decade averaged over oceans between 60°S and 60°N. The increasing trend of ERF ACI stems from a global decline in cloud droplet number concentration driven by decreasing anthropogenic aerosol emissions. It is of similar magnitude as the combined instantaneous forcing trend from greenhouse gases and aerosol-radiation interactions. Our results may reduce the gap between the simulated and observed shortwave contribution to EEI trends while implying a weak shortwave cloud feedback. They also suggest a stronger aerosol forcing than the multi-model mean.

Yuan, Tianle [NASA Goddard Space Flight Center (GS↗

DOE OSTI2019

Increasing impacts of extreme droughts on vegetation productivity under climate change

Terrestrial gross primary production (GPP) is the basis of food production and vegetation growth globally1 and plays a critical role in regulating atmospheric CO2 through its impact on ecosystem carbon balance. Even though higher CO2 concentrations in future decades can increase GPP2, low soil water availability, heat stress and disturbances associated with droughts could reduce the benefits of such CO2 fertilization. Here we analysed outputs of 13 Earth system models to show an increasingly stronger impact on GPP by extreme droughts than by mild and moderate droughts over the twenty-first century. Due to a dramatic increase in the frequency of extreme droughts, the magnitude of globally averaged reductions in GPP associated with extreme droughts was projected to be nearly tripled by the last quarter of this century (2075–2099) relative to that of the historical period (1850–1999) under both high and intermediate GHG emission scenarios. By contrast, the magnitude of GPP reduction associated with mild and moderate droughts was not projected to increase substantially. Our analysis indicates a high risk of extreme droughts to the global carbon cycle with atmospheric warming; however, this risk can be potentially mitigated by positive anomalies of GPP associated with favourable environmental conditions.

Xu, Chonggang↗