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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3

Characterizing and quantifying uncertainty in projections of climate change impacts on air quality

Climate change can aggravate air pollution, with important public health and environmental consequences. While major sources of uncertainty in climate change projections - greenhouse gas (GHG) emissions scenario, model response, and internal variability - have been investigated extensively, their propagation to estimates of air quality impacts has not been systematically assessed. Here, we compare these uncertainties using a coupled modeling framework that includes a human activity model, an Earth system model of intermediate complexity, and a global atmospheric chemistry model. Uncertainties in projections of U.S. air quality under 21st century climate change are quantified based on a climate-chemistry ensemble that includes multiple initializations, representations of climate sensitivity, and climate policy scenarios, under constant air pollution emissions. We find that climate-related uncertainties are comparable at mid-century, making it difficult to distinguish the impact of variations in GHG emissions on ozone and particulate matter pollution. While GHG emissions scenario eventually becomes the dominant uncertainty based on the scenarios considered, all sources of uncertainty are significant through the end of the century. The results provide insights into intrinsically different uncertainties in projections of air pollution impacts and the potential for large ensembles to better capture them.

54 ENVIRONMENTAL SCIENCES↗

Shift in Peaks of PAH-Associated Health Risks From East Asia to South Asia and Africa in the Future

Lung cancer risk from exposure to ambient polycyclic aromatic hydrocarbons (PAHs) is expected to change significantly by 2050 compared to 2008 due to changes in climate and emissions. Integrating a global atmospheric chemistry model, a lung cancer risk model, and plausible future emissions trajectories of PAHs, we assess how global PAHs and their associated lung cancer risk will likely change in the future. Benzo(a)pyrene (BaP) is used as an indicator of cancer risk from PAH mixtures. From 2008 to 2050, the population-weighted global average BaP concentrations under all RCPs consistently exceeded the WHO-recommended limits, primarily attributed to residential biofuel use. Peaks in PAH-associated incremental lifetime cancer risk shift from East Asia (4 × 10 –5 ) in 2008 to South Asia (mostly India, 2–4 × 10 –5 ) and Africa (1–2 × 10 –5 ) by 2050. In the developing regions of Africa and South Asia, PAH-associated lung cancer risk increased by 30–64% from 2008 to 2050, due to increasing residential energy demand in households for cooking, heating, and lighting, the continued use of traditional biomass use, increases in agricultural waste burning, and forest fires, accompanied by rapid population growth in these regions. Due to more stringent air quality policies in developed countries, their PAH lung cancer risk substantially decreased by ~80% from 2008 to 2050. Climate change is likely to have minor effects on PAH lung cancer risk compared to the impact of emissions. Future policies, therefore, need to consider efficient combustion technologies that reduce air pollutant emissions, including incomplete combustion products such as PAH.

54 ENVIRONMENTAL SCIENCES↗

Observed humidity trends in dry regions contradict climate models

Arid and semi-arid regions of the world are particularly vulnerable to greenhouse gas–driven hydroclimate change. Climate models are our primary tool for projecting the future hydroclimate that society in these regions must adapt to, but here, we present a concerning discrepancy between observed and model-based historical hydroclimate trends. Over the arid/semi-arid regions of the world, the predominant signal in all model simulations is an increase in atmospheric water vapor, on average, over the last four decades, in association with the increased water vapor–holding capacity of a warmer atmosphere. In observations, this increase in atmospheric water vapor has not happened, suggesting that the availability of moisture to satisfy the increased atmospheric demand is lower in reality than in models in arid/semi-arid regions. This discrepancy is most clear in locations that are arid/semi-arid year round, but it is also apparent in more humid regions during the most arid months of the year. Here, it indicates a major gap in our understanding and modeling capabilities which could have severe implications for hydroclimate projections, including fire hazard, moving forward.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stochastic nucleation processes and substrate abundance explain time-dependent freezing in supercooled droplets

Atmospheric immersion freezing (IF), a heterogeneous ice nucleation process where an ice nucleating particle (INP) is immersed in supercooled water, is a dominant ice formation pathway impacting the hydrological cycle and climate. Implementation of IF derived from field and laboratory data in cloud and climate models is difficult due to the high variability in spatio-temporal scales, INP composition, and morphological complexity. We demonstrate that IF can be consistently described by a stochastic nucleation process accounting for uncertainties in the INP surface area. This approach accounts for time-dependent freezing, a wide range of surface areas and challenges phenomenological descriptions typically used to interpret IF. The results have an immediate impact on the current description, interpretation, and experiments of IF and its implementation in models. The findings are in accord with nucleation theory, and thus should hold for any supercooled liquid material that nucleates in contact with a substrate.

54 ENVIRONMENTAL SCIENCES↗

Simulations of ENSO Phase-locking in CMIP5 and CMIP6

The characteristics of El-Niño-Southern Oscillation (ENSO) phase-locking in observations and CMIP5 and CMIP6 models are examined in this study. Two metrics based on the peaking month histogram for all El Niño and La Niña events are adopted to delineate the basic features of ENSO phase-locking in terms of the preferred calendar month and strength of this preference. It turns out that most models are poor at simulating the ENSO phase-locking, either showing little peak strengths or peaking at the wrong seasons. By deriving ENSO’s linear dynamics based on the conceptual recharge oscillator (RO) framework through the seasonal linear inverse model (sLIM) approach, various simulated phase-locking behaviors of CMIP models are systematically investigated in comparison with observations. In observations, phase-locking is mainly attributed to the seasonal modulation of ENSO’s SST growth rate. In contrast, in a significant portion of CMIP models, phase-locking is co-determined by the seasonal modulations of both SST growth and phase-transition rates. Further study of the joint effects of SST growth and phase-transition rates suggests that for simulating realistic winter peak ENSO phase-locking with the right dynamics, climate models need to have four key factors in the right combination: (1) correct phase of SST growth rate modulation peaking at the fall; (2) large enough amplitude for the annual cycle in growth rate; (3) amplitude of semi-annual cycle in growth rate needs to be small; and (4) amplitude of seasonal modulation in SST phase-transition rate needs to be small.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Climate change penalty and benefit on surface ozone: a global perspective based on CMIP6 earth system models

Abstract This work presents an analysis of the effect of climate change on surface ozone discussing the related penalties and benefits around the globe from the global modelling perspective based on simulations with five CMIP6 (Coupled Model Intercomparison Project Phase 6) Earth System Models. As part of AerChemMIP (Aerosol Chemistry Model Intercomparison Project) all models conducted simulation experiments considering future climate (ssp370SST) and present-day climate (ssp370pdSST) under the same future emissions trajectory (SSP3-7.0). A multi-model global average climate change benefit on surface ozone of −0.96 ± 0.07 ppbv °C −1 is calculated which is mainly linked to the dominating role of enhanced ozone destruction with higher water vapour abundances under a warmer climate. Over regions remote from pollution sources, there is a robust decline in mean surface ozone concentration on an annual basis as well as for boreal winter and summer varying spatially from −0.2 to −2 ppbv °C −1 , with strongest decline over tropical oceanic regions. The implication is that over regions remote from pollution sources (except over the Arctic) there is a consistent climate change benefit for baseline ozone due to global warming. However, ozone increases over regions close to anthropogenic pollution sources or close to enhanced natural biogenic volatile organic compounds emission sources with a rate ranging regionally from 0.2 to 2 ppbv C −1 , implying a regional surface ozone penalty due to global warming. Overall, the future climate change enhances the efficiency of precursor emissions to generate surface ozone in polluted regions and thus the magnitude of this effect depends on the regional emission changes considered in this study within the SSP3_7.0 scenario. The comparison of the climate change impact effect on surface ozone versus the combined effect of climate and emission changes indicates the dominant role of precursor emission changes in projecting surface ozone concentrations under future climate change scenarios.

Zanis, Prodromos↗

Persisting volcanic ash particles impact stratospheric SO 2 lifetime and aerosol optical properties

Volcanic ash is often neglected in climate simulations because ash particles are assumed to have a short atmospheric lifetime, and to not participate in sulfur chemistry. After the Mt. Kelut eruption in 2014, stratospheric ash-rich aerosols were observed for months. Here we show that the persistence of super-micron ash is consistent with a density near 0.5 g cm -3 , close to pumice. Ash-rich particles dominate the volcanic cloud optical properties for the first 60 days. We also find that the initial SO 2 lifetime is determined by SO 2 uptake on ash, rather than by reaction with OH as commonly assumed. About 43% more volcanic sulfur is removed from the stratosphere in 2 months with the SO 2 heterogeneous chemistry on ash particles than without. This research suggests the need for re-evaluation of factors controlling SO 2 lifetime in climate model simulations, and of the impact of volcanic ash on stratospheric chemistry and radiation.

54 ENVIRONMENTAL SCIENCES↗

A Modular System for Increasing Predictiveness for Extreme Climate Predictions

We know that climate change is poised to reshape our world, but we lack clear enough predictions about precisely how. The preponderance of these changes is associated with human activity, specifically the emission of CO 2 and other greenhouse gases. Problematically, projections of climate change continue to be marred by unacceptably large uncertainties which hamper informed decision-making and cost society a chance to adapt proactively and effectively. These uncertainties stem from deficiencies in predictions of future greenhouse gas emissions, but also from inaccuracies in the representation of the physical models used to predict the climate response to such emissions. The uncertainties in projections associated with the inaccurate representation of climate physics, chemistry and biology are similar to those that plagued the first global climate models developed fifty years ago, despite more than a factor 10 8 increase in computer performance. Our transformational question is then, how can the accuracy of climate projections be dramatically improved by applying recent advances in the computational and data sciences to train the models with the wealth of data being constantly collected about the ongoing changes in the climate system?

54 ENVIRONMENTAL SCIENCES↗

Understanding the Applicability of Gas/Particle Partitioning Theory to SOA using Novel Chemically-Speciated Partitioning Measurements (Final Report)

The main objective of this research grant project was to investigate the physical-chemical processes and properties of particles and partitioning gases that influence gas/particle (G/P) partitioning and timescales for equilibration, to directly determine the conditions under which equilibrium G/P partitioning theory can be applied to secondary organic aerosol (SOA). SOA constitutes a major component of submicron particles in the atmosphere, which have important implications for air quality, human and ecosystem health, radiation balance, and climate; however SOA formation, evolution and losses are not well understood. Use of novel on-line measurements of chemically-speciated partitioning measurements of both gas-phase and particle-phase components was a central component to advancing these scientific goals. The key approach was to conduct environmental chamber studies with systems of increasing complexity to determine G/P partitioning rates and equilibrium states for chemically-speciated SOA components. The project builds on our previous work on gas-wall partitioning that must be understood in order to study G/P partitioning in chambers, and to help extrapolate the results to be atmospherically relevant. The goal was to employ measurements and modeling to systematically determine when G/P partitioning theory accurately describes the distribution of oxidized organic compounds in the gas and aerosol phases, and when and why it does not (e.g., aerosol phase-state kinetic limitations, non-ideal mixing, phase separation, oligomer formation,), for chemical and physical conditions typically found throughout the continental boundary layer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The future of Earth system prediction: Advances in model-data fusion

Predictions of the Earth system, such as weather forecasts and climate projections, require models informed by observations at many levels. Some methods for integrating models and observations are very systematic and comprehensive (e.g., data assimilation), and some are single purpose and customized (e.g., for model validation). We review current methods and best practices for integrating models and observations. We highlight how future developments can enable advanced heterogeneous observation networks and models to improve predictions of the Earth system (including atmosphere, land surface, oceans, cryosphere, and chemistry) across scales from weather to climate. As the community pushes to develop the next generation of models and data systems, there is a need to take a more holistic, integrated, and coordinated approach to models, observations, and their uncertainties to maximize the benefit for Earth system prediction and impacts on society.

54 ENVIRONMENTAL SCIENCES↗

A spatial evaluation of Arctic sea ice and regional limitations in CMIP6 historical simulations

The Arctic sea ice response to a warming climate is assessed in a subset of models participating in Phase 6 of the Coupled Model Intercomparison Project (CMIP6), using several metrics in comparison with satellite observations and results from the Pan-Arctic Ice Ocean Modeling and Assimilation System and the Regional Arctic System Model. Our study examines the historical representation of sea ice extent, volume, and thickness using spatial analysis metrics, such as the integrated ice-edge error, Brier score, and Spatial Probability Score. We find that the CMIP6 multi-model mean captures the mean annual cycle and 1979-2014 sea ice trends remarkably well. However, individual models experience a wide range of uncertainty in the spatial distribution of sea ice when compared against satellite measurements and reanalysis data. Our metrics expose common and individual regional model biases, which sea ice temporal analyses alone do not capture. We identify large ice edge and ice thickness errors in Arctic sub-regions, implying possible model specific limitations in or lack of representation of some key physical processes. We postulate that many of them could be related to the oceanic forcing, especially in the marginal and shelf seas, where seasonal sea ice changes are not adequately simulated. We therefore conclude that an individual model’s ability to represent the observed/reanalysis spatial distribution still remains a challenge. We propose the spatial analysis metrics as useful tools to diagnose model limitations, narrow down possible processes affecting them, and guide future model improvements critical to the representation and projections of Arctic climate change.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Role and Lifetime of Dissociative Heterogeneous Processes in Improving Simulated Ozone on Mars

Abstract Ozone simulated in Mars Global Climate Models (MGCMs) is used to assess the underlying chemistry occurring in the atmosphere. Currently, ozone total column abundance (TCA) is under‐predicted in MGCMs by up to 120%, implying missing or inaccurate chemistry in models. Heterogeneous reactions of hydroxyl radicals (HO X ) have been offered as an explanation for some of this bias, because they cause ozone to increase at locations where it's currently under‐predicted. We use four simulations to compare modeled ozone TCA with observations from the UVIS spectrometer aboard the ExoMars Trace Gas Orbiter to improve the representation of heterogeneous processes and their impact on ozone. We use a gas‐phase only run, a dissociative scheme, an adsorbed HO X retention scheme, and a hybrid scheme that combines the dissociative mechanism with the retention of HO X on water ice. We find retention of HO X is dependent on water ice sublimation, and ozone abundance increases when water ice persists for longer periods (1–20 sols). Over time, the loss of HO X causes a depletion in H 2 O 2 concentration (HO X reservoir), and thus allows ozone concentration to increase. When adsorbed HO X are desorbed and dissociate into other by‐products, HO X are not immediately available to destroy ozone. This results in larger ozone concentrations than if desorbed HO X are released directly back into their gaseous states. When using the hybrid scheme, ozone TCA is increased up to 50% where the ozone deficit is greatest, demonstrating the best agreement with observations, and implying that HO X radicals are both retained when adsorbed and dissociate.

Brown, M. A. J.↗

Improving the QBO Forcing by Resolved Waves With Vertical Grid Refinement in E3SMv2

Abstract The quasi‐biennial oscillation (QBO) is the dominate mode of variability in the tropical stratosphere and plays an important role in stratospheric dynamics and chemistry. The QBO is notably deficient in many climate models, including the Energy Exascale Earth System Model (E3SM) developed by the US Department of Energy. In this work, we refine the lower stratospheric vertical grid spacing from roughly 1 km to 500 m to facilitate more realistic equatorial wave activity in the lower stratosphere in E3SM version 2. The refinement results in a simulated QBO with a reasonable amplitude and easterly‐westerly transition in both directions, but still has a longer period than observed, slower easterly downward propagation speed, and shallower vertical depth. Similar refinement in the multi‐scale modeling framework configuration of E3SM yields similar improvements. By analyzing the forcing contributions from different wave types, we find that most of the QBO forcing still comes from parameterized gravity wave drag from convection. The improved QBO forcing contributions from resolved waves, especially equatorial Kelvin waves and resolved small scale waves, can be attributed to the grid refinement.

E3SM↗

Global net climate effects of anthropogenic reactive nitrogen

Anthropogenic activities have substantially enhanced the loadings of reactive nitrogen (Nr) in the Earth system since pre-industrial times, contributing to widespread eutrophication and air pollution. Increased Nr can also influence global climate through a variety of effects on atmospheric and land processes but the cumulative net climate effect is yet to be unravelled. Here we show that anthropogenic Nr causes a net negative direct radiative forcing of –0.34 [–0.20, –0.50] W m –2 in the year 2019 relative to the year 1850. This net cooling effect is the result of increased aerosol loading, reduced methane lifetime and increased terrestrial carbon sequestration associated with increases in anthropogenic Nr, which are not offset by the warming effects of enhanced atmospheric nitrous oxide and ozone. Future predictions using three representative scenarios show that this cooling effect may be weakened primarily as a result of reduced aerosol loading and increased lifetime of methane, whereas in particular N 2 O-induced warming will probably continue to increase under all scenarios. Our results indicate that future reductions in anthropogenic Nr to achieve environmental protection goals need to be accompanied by enhanced efforts to reduce anthropogenic greenhouse gas emissions to achieve climate change mitigation in line with the Paris Agreement.

54 ENVIRONMENTAL SCIENCES↗

Modeling Functional Organic Chemistry in Arctic Rivers: An Idealized Siberian System

Rivers of the Arctic will become ever more important for the global climate, since they carry a majority of continental dissolved organic carbon flux into the rapidly changing polar ocean. Aqueous organics comprise a wide array of functional groups, several of which are likely to impact coastal and open water biophysical properties. Light attenuation, interfacial films, aerosol formation, gas release and momentum exchange can all be cited. We performed Lagrangian kinetic modeling for the evolution of riverine organic chemistry as the molecules in question make their way from the highlands to Arctic outlets. Classes as diverse as the proteins, sugars, lipids, re-condensates, humics, bio-tracers and small volatiles are all included. Our reduced framework constitutes an idealized northward flow driving a major hydrological discharge rate and primarily representing the Russian Lena. Mountainous, high solute and tundra sources are all simulated, and they meet up at several points between soil and delta process reactors. Turnover rates are parameterized beginning with extrapolated coastal values imposed along a limited tributary network, with connections between different terrestrial sub-ecologies. Temporal variation of our total dissolved matter most closely resembles the observations when we focus on the restricted removal and low initial carbon loads, suggesting relatively slow transformation along the water course. Thus, channel combinations and mixing must play a dominant role. Nevertheless, microbial and photochemical losses help determine the final concentrations for most species. Chemical evolution is distinct for the various functionalities, with special contributions from pre- and post-reactivity in soil and delta waters. Several functions are combined linearly to represent the collective chromophoric dissolved matter, characterized here by its absorption. Tributaries carry the signature of lignin phenols to segregate tundra versus taiga sources, and special attention is paid to the early then marine behaviors of low molecular weight volatiles. Heteropolycondensates comprise the largest percentage of reactive carbon in our simulations due to recombination/accumulation, and they tend to be preeminent at the mouth. Outlet concentrations of individual structures such as amino acids and absorbers lie above threshold values for biophysical influence, on the monolayer and light attenuation. The extent of coastal spreading is examined through targeted regional box modeling, relying on salinity and color for calibration. In some cases, plumes reach the scale of peripheral arctic seas, and amplification is expected during upcoming decades. Conclusions are mapped from the Lena to other boreal discharges, and future research questions are outlined regarding the bonding type versus mass release as permafrost degrades. Dynamic aqueous organic coupling is recommended for polar system models, from headwaters to coastal diluent.

54 ENVIRONMENTAL SCIENCES↗

Aerosols overtake greenhouse gases causing a warmer climate and more weather extremes toward carbon neutrality

To mitigate climate warming, many countries have committed to achieve carbon neutrality in the mid-21 st century. Here, we assess the global impacts of changing greenhouse gases (GHGs), aerosols, and tropospheric ozone (O 3 ) following a carbon neutrality pathway on climate and extreme weather events individually using the Community Earth System Model version 1 (CESM1). The results suggest that the future aerosol reductions significantly contribute to climate warming and increase the frequency and intensity of extreme weathers toward carbon neutrality and aerosol impacts far outweigh those of GHGs and tropospheric O 3 . It reverses the knowledge that the changing GHGs dominate the future climate changes as predicted in the middle of the road pathway. Therefore, substantial reductions in GHGs and tropospheric O 3 are necessary to reach the 1.5 °C warming target and mitigate the harmful effects of concomitant aerosol reductions on climate and extreme weather events under carbon neutrality in the future.

54 ENVIRONMENTAL SCIENCES↗

Characterizing the contribution of bioaerosols diversity from complex aerosol particle samples.

Current global change scenarios expect to significantly increase the contribution of pollen to the total organic aerosol budget. In addition, pollen can burst into smaller fragments that are highly efficient as cloud condensation nuclei. However, current climate models still do not incorporate the effects of these particles due to detection and quantification challenges in complex aerosol mixtures. Chemical biomarkers (i.e. fructose) have commonly been used to trace pollen but this approximation can generate false positive results given the large number of shared compounds between different bioaerosols. A previous pilot EMSL experiment performed on pure pollen samples suggested that using a set of metabolites as a fingerprint of bioaerosols could serve to substantially increase detection accuracy over single biomarker approaches. In this proposal we developed novel bioinformatic strategies to characterize and quantify complex pollen mixtures present in the atmosphere. For that, we used diverse machine learning algorithms to analyze metabolic fingerprints from complex mixtures of different pollen acquired with high-resolution mass spectrometry (Orbitrap Q-Exactive). Our preliminary results demonstrated the potential to accurately discern and identify at specific relative abundances different pollen species in complex mixtures. Our research will lead to a significant advancement in the atmospheric chemistry and provide much needed data to improve the accuracy of climate models.

54 ENVIRONMENTAL SCIENCES↗

Analysis of secondary organic aerosol simulation bias in the Community Earth System Model (CESM2.1)

Organic aerosol (OA) has been considered as one of the most important uncertainties in climate modeling due to the complexity in presenting its chemical production and depletion mechanisms. To better understand the capability of climate models and probe into the associated uncertainties in simulating OA, we evaluate the Community Earth System Model version 2.1 (CESM2.1) configured with the Community Atmosphere Model version 6 (CAM6) with comprehensive tropospheric and stratospheric chemistry representation (CAM6-Chem) through a long-term simulation (1988–2019) with observations collected from multiple datasets in the United States. We find that CESM generally reproduces the interannual variation and seasonal cycle of OA mass concentration at surface layer with a correlation of 0.40 compared to ground observations and systematically overestimates (69%) in summer and underestimates (-19%) in winter. Through a series of sensitivity simulations, we reveal that modeling bias is primarily related to the dominant fraction of monoterpene-formed secondary organic aerosol (SOA), and a strong positive correlation of 0.67 is found between monoterpene emission and modeling bias in the eastern US during summer. In terms of vertical profile, the model prominently underestimates OA and monoterpene concentrations by 37%–99% and 82%–99%, respectively, in the upper air (>500 m) as validated against aircraft observations. Our study suggests that the current volatility basis set (VBS) scheme applied in CESM might be parameterized with monoterpene SOA yields that are too high, which subsequently results in strong SOA production near the emission source area. We also find that the model has difficulty in reproducing the decreasing trend of surface OA in the southeastern US probably because of employing pure gas VBS to represent isoprene SOA which is in reality mainly formed through multiphase chemistry; thus, the influence of aerosol acidity and sulfate particle change on isoprene SOA formation has not been fully considered in the model. This study reveals the urgent need to improve the SOA modeling in climate models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗