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DOE OSTI2025

Simulating Pyrocumulonimbus Clouds Using a Multiscale Wildfire Simulation Framework

Pyrocumulonimbus (pyroCb) clouds, driven by extreme fires under favorable meteorological conditions, can inject smoke into the stratosphere at magnitudes comparable to those of moderate volcanic eruptions, potentially altering the global radiative balance and atmospheric composition. However, simulating pyroCb is particularly challenging in Earth system models. Using the Energy Exascale Earth System Model (E3SM), we developed a novel global multiscale framework to model pyroCb events in California, which includes a high‐resolution fire radiative power time series, a one‐dimensional plume‐rise parameterization, a fire‐induced vertical water vapor transport scheme, and a surface wildfire sensible heat flux representation. Our simulation successfully reproduces many pyroCb features, including cloud height, spatiotemporal evolution, and convective intensity in comparison with satellite and ground‐based observations. Sensitivity experiments show that realistic pyroCb simulation depends on vertical water vapor transport. These advances provide a basis for future exploration of pyroCb impacts at regional and global scales within climate models.

E3SM↗

DOE OSTI2023

Warming decreases desert ecosystem functioning by altering biocrusts in drylands

Warming and precipitation fluctuations are changing desert ecosystems in global drylands. However, the effects of climate change on keystone species such as cryptogamic biocrust in drylands remain relatively under-investigated, even though biocrusts play a vital role in desert ecosystems. Here we conducted a long-term experiment (14 years) to simulate the responses of two main types of biocrusts to warming coupled with reduction in precipitation that was achieved by open-top chambers (OTCs) to simulate the predicted warming and precipitation decreasing under climate change scenario. We also conduct a structural analysis to evaluate the resulting changes in desert ecosystem functioning (carbon and nitrogen cycling). Neither warming and corresponding rainfall reduction treatments had a negative effect on lichen species richness, but both treatments reduced lichen cover and biomass. The negative effects of warming on moss-dominated crusts were much greater than those on lichen-dominated crusts. Although mosses and lichens had varying degree responses to warming, the loss of mosses and decreased lichen cover and biomass, as well as the shortening of the wet time, resulted in a reduction in carbon and nitrogen fixation, soil enzyme activity and water-holding capacity of biocrusts and topsoil. These impacts collectively change the water balance of drylands and weaken the hydrological and biogeochemical function of biocrusts. Synthesis and applications: Results from this long-term experiment suggest that the ecosystem C and N cycling and water balance of global drylands may be highly impacted by climate change, in part because of the response of biocrusts, which contribute an important implication for both dryland restoration and earth system dynamics.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Size-resolved process understanding of stratospheric sulfate aerosol following the Pinatubo eruption

Stratospheric sulfate aerosol produced by volcanic eruptions plays important roles in atmospheric chemistry and the global radiative balance of the atmosphere. The simulation of stratospheric sulfate concentrations and optical properties is highly dependent on the chemistry scheme and microphysical treatment. In this work, we implemented a sophisticated gas-phase chemistry scheme (full chemistry, FC) and a 5-mode version of the Modal Aerosol Module with Prognostic Stratospheric Aerosol (MAM5-PSA) for the interactive treatment of stratospheric sulfate aerosol in the Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2) model to better simulate the chemistry-aerosol feedback following the Pinatubo eruption, and to compare it against a simulation using simplified chemistry (SC) and the default 4-mode version of the Modal Aerosol Module (MAM4). MAM5-PSA experiments were found to better capture the stratospheric sulfate burden from the eruption of the volcano to the end of 1992 as compared to the High-resolution Infrared Sounder (HIRS) observations, and the formation of sulfate in MAM5-PSA with FC (with an additional OH replenishment reaction) was significantly faster than in MAM4 with FC. Analyses of microphysical processes indicate that more sulfate aerosol mass was generated in total in FC experiments than in SC experiments. MAM5-PSA performs better than MAM4 in simulation of aerosol optical depth (AOD); AOD anomalies from the MAM5-PSA experiment have better agreement with observations. The simulated largest changes in global mean net radiative flux at the top of the atmosphere following the eruption were about −3 W m −2 in MAM5-PSA experiments and roughly −1.5 W m −2 in MAM4 experiments.

AEROSOL↗

DOE OSTI2023

Microbial Models for Simulating Soil Carbon Dynamics: A Review

Abstract Soils store the largest amount of carbon (C) in the biosphere, and the C pool in soil is critical to the global C balance. Numerous microbial models have been developed over the last few decades to represent microbial processes that regulate the responses of soil organic carbon (SOC) to climate change. However, the representation of microbial processes varies, and how microbial processes are incorporated into SOC models has not been well explored. Here, we reviewed 71 microbial models to characterize the microbial processes incorporated into SOC models and analyzed variations in mechanistic complexity. We revealed that (a) four processes (microbial‐mediated decomposition, mineral interaction, microbial necromass recycling, and active and dormant microbial dynamics) are commonly incorporated in microbial models, (b) ∼48% of models simulate only one microbial process (i.e., microbial‐mediated decomposition) and 35% of models simulate two microbial processes: for example, microbial‐mediated decomposition and mineral interaction, (c) more than 80% microbial models use nonlinear equations, such as forward Michaelis‐Menten kinetics, to represent SOC decomposition, (d) the concept of persistence of SOC due to its intrinsic properties has been replaced by organo‐mineral interaction (∼39% of microbial models) that protects SOC from decomposition, and (e) various temperature and moisture modifiers and pH effects have been used to explain the environmental effect on microbial processes. In the future, to realistically incorporate microbial processes into Earth System Models, it is imperative to identify experimental evidence on rate limitation processes and firmly ground model structure on the field and laboratory data.

Environmental Sciences & Ecology↗

DOE OSTI2022

Upper troposphere dust belt formation processes vary seasonally and spatially in the Northern Hemisphere

Dust aerosols impact global energy balance substantially by acting as efficient ice nuclei to alter cold cloud properties. However, the estimate of dust indirect effect remains uncertain due to simulating dust distributions poorly and lacking reliable dust observations, especially in the upper-troposphere. Here, we characterize and understand upper-troposphere dust sources and transport with an improved dust dataset derived from A-train satellite lidar and radar measurements and an air parcel trajectory model. The distinct upper-troposphere dust belt over the northern hemisphere has seasonally varying base and top heights of 3.65 ± 2.84 and 8.35 ± 1.50 km above mean sea level and its column loading is strongest during spring (March-April-May). The out-of-phase annual cycles of mid-level dust concentration and westerly wind over source regions control the seasonal upper-tropospheric dust loading variations. African deserts contribute the most (46.3%) to the upper-troposphere dust belt in spring and the synoptic trough is the leading (49%) dust lifting mechanism.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Time-resolved quantification of key species and mechanistic insights in low-temperature tetrahydrofuran oxidation

Here, we investigate the kinetics and report the time-resolved concentrations of key chemical species in the oxidation of tetrahydrofuran (THF) at 7500 torr and 450–675 K. Experiments are carried out using high-pressure multiplexed photoionization mass spectrometry (MPIMS) combined with tunable vacuum ultraviolet radiation from the Berkely Lab Advanced Light Source. Intermediates and products are quantified using reference photoionization (PI) cross sections, when available, and constrained by a global carbon balance tracking approach at all experimental temperatures simultaneously for the species without reference cross sections. From carbon balancing, we determine time-resolved concentrations for the ROO˙ and ˙OOQOOH radical intermediates, butanedial, and the combined concentration of ketohydroperoxide (KHP) and unsaturated hydroperoxide (UHP) products stemming from the ˙QOOH + O 2 reaction. Furthermore, we quantify a product that we tentatively assign as fumaraldehyde, which arises from UHP decomposition via H 2 O or ˙OH + H loss. The experimentally derived species concentrations are compared with model predictions using the most recent literature THF oxidation mechanism of Fenard et al., (Combust. Flame, 2018, 191, 252–269). Our results indicate that the literature mechanism significantly overestimates THF consumption and the UHP + KHP concentration at our conditions. The model predictions are sensitive to the rate coefficient for the ROO˙ isomerization to ˙QOOH, which is the gateway for radical chain propagating and branching pathways. Comparisons with our recent results for cyclopentane (Demireva et al., Combust. Flame, 2023, 257, 112506) provide insights into the effect of the ether group on reactivity and highlight the need to determine accurate rate coefficients of ROO˙ isomerization and subsequent reactions.

Demireva, Maria↗

DOE OSTI2023

DC electric field generation and distribution in magnetized plasmas

Very large DC and AC electric fields cannot be sustained between conducting electrodes because of volume gas breakdown and/or surface field emission. However, very large potential fields are now routinely generated in plasma structures, such as laser generated wake in unmagnetized plasmas. In magnetized plasmas, large DC fields can also be sustained and controlled perpendicular to the magnetic field, but the metallic end plates limiting the plasma, terminating the magnetic field lines, and usually providing the voltage drop feed between the field lines impose severe restrictions on the maximum field. However, it is shown that very large radial DC voltage drops can be sustained by injecting waves of predetermined frequencies and wave vectors, traveling along the azimuthal direction of an axially magnetized plasma cylinder, or by injecting fast neutral particles beams along this azimuthal direction. The large conductivity along the magnetic field lines and the small conductivity between the field lines then distribute this voltage drop. Furthermore, the global power balance and control parameters of wave and beam generated large DC electric fields in magnetized plasmas are identified, described, and analyzed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Optimizing biological carbon uptake by regulating carbonate-bicarbonate equilibrium

Balancing the global carbon budget is a grand challenge and a critical research mission for sustaining life on Earth. Oceans absorb ca. 30% of global anthropogenic CO 2 emissions and dissolved CO 2 in the oceans forms carbonic acid that dissociates to generate H + , bicarbonate, and carbonate. By regulating the carbonate-bicarbonate equilibrium, rates of marine photosynthesis can be substantially enhanced, thereby capturing and condensing CO 2 into a readily utilizable form. The specific goal of this project was to demonstrate enhanced marine biomass production at the bench-scale towards advancing sustainable marine CO 2 removal. Our proof-of-concept experimental results are highly promising and we have filed a PNNL invention disclosure. In consideration of which, no further details are included in this document.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Exploring Multilayer Network Models to Build a Scientific Basis for Integrated Deterrence: Final Report

The emerging multipolar international security environment represents a fundamental restructuring of global nuclear balance of power to include two nuclear peer competitors, growing non-peer nuclear threats, and concerns of nuclear latency from both allies and adversaries. Conflicts in the grey zone, cyber operations, mis- and disinformation campaigns, and emerging disruptive technologies like drones, and hypersonic missiles are becoming more prevalent. These present a risk of cross-domain and multi-domain conflicts that may not follow known escalatory patterns. In order to prepare for the new deterrence environment, it is critical to have quantitative and qualitative understandings of these cross-domain conflicts, their potential for escalation, and which systems they may impact. To that end, our team created a Multi-Layer Network (MLN) model of ‘integrated deterrence’ where instruments of national power are modeled as individual network graph layers that include efforts from all domains. We then evaluate the potential for escalation against escalation scenarios. Analysis of the escalation scenarios is then used to identify insights of potential risk and escalation within integrated deterrence.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2022

Water balance model (WBM) v.1.0.0: a scalable gridded global hydrologic model with water-tracking functionality

Abstract. This paper describes the University of New Hampshire Water Balance Model, WBM, a process-based gridded global hydrologic model that simulates the land surface components of the global water cycle and includes water extraction for use in agriculture and domestic sectors. The WBM was first published in 1989; here, we describe the first fully open-source WBM version (v.1.0.0). Earlier descriptions of WBM methods provide the foundation for the most recent model version that is detailed here. We present an overview of the model functionality, utility, and evaluation of simulated global river discharge and irrigation water use. This new version adds a novel suite of water source tracking modules that enable the analysis of flow-path histories on water supply. A key feature of WBM v.1.0.0 is the ability to identify the partitioning of sources for each stock or flux within the model. Three different categories of tracking are available: (1) primary inputs of water to the surface of the terrestrial hydrologic cycle (liquid precipitation, snowmelt, glacier melt, and unsustainable groundwater); (2) water that has been extracted for human use and returned to the terrestrial hydrologic system; and (3) runoff originating from user-defined spatial land units. Such component tracking provides a more fully transparent model in that users can identify the underlying mechanisms generating the simulated behavior. We find that WBM v.1.0.0 simulates global river discharge and irrigation water withdrawals well, even with default parameter settings, and for the first time, we are able to show how the simulation arrives at these fluxes by using the novel tracking functions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Projections of Hourly Meteorology by Balancing Authority Based on the IM3/HyperFACETS Thermodynamic Global Warming (TGW) Simulations

This dataset contains 40 years (1980-2019) of historical hourly meteorology and 80 years (2020-2099) of projected hourly meteorology for 54 Balancing Authorities (BAs) in the conterminous United States. Details about the scenarios and variables included in this dataset are in the readme.pdf file. This dataset is derived from the IM3/HyperFACETS Thermodynamic Global Warming (TGW) simulations (https://doi.org/10.57931/1885756). More details on the TGW approach can be found at: https://tgw-data.msdlive.org/. If you use this dataset please also cite the raw TGW dataset (Jones, A. D., Rastogi, D., Vahmani, P., Stansfield, A., Reed, K., Thurber, T., Ullrich, P., & Rice, J. S. (2022). IM3/HyperFACETS Thermodynamic Global Warming (TGW) Simulation Datasets (v1.0.0) [Data set]. MSD-LIVE Data Repository. https://doi.org/10.57931/1885756). To go from the TGW data to these BA-level aggregated data we first averaged the raw gridded data by county in the United States. That intermediate data step is also stored in MSD-LIVE (https://doi.org/10.57931/1960548). We then population-weight the county-level hourly data in order to create population-weighted meteorology time series for each BA. Historical populations are from the United States Census Bureau and the evolving future populations are based on Shared Socioeconomic Pathways (SSPs) 3 and 5. The four climate scenarios crossed with the two SSPs yield eight different future projections for each BA: rcp45cooler_ssp3, rcp45cooler_ssp5, rcp45hotter_ssp3, rcp45hotter_ssp5, rcp85cooler_ssp3, rcp85cooler_ssp5, rcp85hotterssp3, rcp85hotterssp5. For the historical period and each of the eight future scenarios the dataset has hourly estimates of the population-weighted average of five meteorological variables: Temperature, specific humidity, shortwave radiation, longwave radiation, and wind speed. All times are in Coordinated Universal Time (UTC). The code to go from the raw TGW data to county-level and then BA-level projections is available at: https://github.com/IMMM-SFA/im3components/tree/main/im3components/wrf_to_tell.

Balancing Authority↗

DOE OSTI2022

Renewable Energy and Efficiency Technologies in Scenarios of U.S. Decarbonization in Two Types of Models: Comparison of GCAM Modeling and Sector-Specific Modeling

Energy system projections from quantitative models inform actions ranging from short-term and local decisions, such as those about technology and infrastructure deployment, and global and long-term negotiations and targets. Computational limits require model designers to balance coverage and resolution (i.e., breadth versus depth). Some models, such as the Global Change Analysis Model (GCAM), represent all energy sources and uses with less resolution than models that focus on a single sector's energy use. GCAM balances global supply and demand of all energy carriers projecting prices using internal calculations for energy sources and costs of greenhouse gas mitigation while capturing interlinkages between the energy system, water, agriculture and land use, the economy, and the climate. This globally comprehensive model was used to frame the Long-Term Strategy of the United States: Pathways to Net-Zero Greenhouse Gas Emissions by 2050, which the White House released in 2021 and has been used to inform national and global economy-wide climate change mitigation discussions and strategy development for decades. Unlike GCAM, sectoral models focus on a portion of the energy sector and with greater detail and resolution. The Regional Energy Deployment System (ReEDS) electricity-sector model, for example, projects electricity system capacity expansion and operation with high-fidelity representation of emerging technologies for deep decarbonization, such as variable renewable energy and energy storage, and integration of these technologies into the electric grid. The Transportation Energy and Mobility Pathway Options (TEMPO) transportation-sector model enables analysis of household choices, with a focus on adoption, charging, and use of electric vehicles. The Scout buildings-sector model supports detailed consideration of the policies and markets that can accelerate the adoption of electrification and energy conservation measures in buildings. Such sector-specific models are instrumental in informing technology research, sectoral planning strategies, and sector-specific aspects of greenhouse gas mitigation strategies in the United States. The integrated multisector and sector-specific modeling approaches represented by GCAM and these sectoral models are complementary. The integrated multisector approach calculates energy pricing and resource allocation within the model, which is important for consistency when future conditions substantially diverge from current conditions in transformative scenarios. The sector-specific approach facilitates representation of granular details across spatial, temporal, technological, and market dimensions that enable exploration of particular interactions and trade-offs. This report presents the results of recent work to explore the differences and trade-offs between these approaches by comparing GCAM with the sector-specific ReEDS, TEMPO, and Scout models. The report compares both model structures and results, and it addresses their potential relevance and applications.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2024

A Scale‐Dependent Analysis of the Barotropic Vorticity Budget in a Global Ocean Simulation

Abstract The climatological mean barotropic vorticity budget is analyzed to investigate the relative importance of surface wind stress, topography, planetary vorticity advection, and nonlinear advection in dynamical balances in a global ocean simulation. In addition to a pronounced regional variability in vorticity balances, the relative magnitudes of vorticity budget terms strongly depend on the length‐scale of interest. To carry out a length‐scale dependent vorticity analysis in different ocean basins, vorticity budget terms are spatially coarse‐grained. At length‐scales greater than 1,000 km, the dynamics closely follow the Topographic‐Sverdrup balance in which bottom pressure torque, surface wind stress curl and planetary vorticity advection terms are in balance. In contrast, when including all length‐scales resolved by the model, bottom pressure torque and nonlinear advection terms dominate the vorticity budget (Topographic‐Nonlinear balance), which suggests a prominent role of oceanic eddies, which are of km in size, and the associated bottom pressure anomalies in local vorticity balances at length‐scales smaller than 1,000 km. Overall, there is a transition from the Topographic‐Nonlinear regime at scales smaller than 1,000 km to the Topographic‐Sverdrup regime at length‐scales greater than 1,000 km. These dynamical balances hold across all ocean basins; however, interpretations of the dominant vorticity balances depend on the level of spatial filtering or the effective model resolution. On the other hand, the contribution of bottom and lateral friction terms in the barotropic vorticity budget remains small and is significant only near sea‐land boundaries, where bottom stress and horizontal viscous friction generally peak.

Khatri, Hemant↗

DOE OSTI2024

A Test of Functional Balance Theory for Wetland Biomass Allocation in a Global Change Experiment

Abstract Forecasts of root growth and carbon sequestration under global change are compromised by uncertainty in how plants will allocate biomass between above and belowground pools. Here, we develop a simple model to assess whether functional balance theory can explain a complex biomass allocation response observed in a brackish marsh under experimental warming and elevated CO 2 . Our model shows how treatment‐driven changes in nitrogen supply and demand can explain divergent observations of root growth (i.e., maximum responses under intermediate warming and elevated CO 2 ). The model also reveals a surprising interaction between warming and eutrophication, where enhanced N loading to coastal marshes may reduce adverse impacts of warming on root growth. Our findings provide a mechanistic basis for incorporating biomass allocation into forecast models of marsh evolution. They also provide a general example of using ecological theory to decompose complex net responses observed in multi‐factor global change experiments into constituent processes.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Sulfur-Enriched Nanoporous Carbon: A Novel Approach to CO 2 Adsorption

Carbon dioxide (CO 2 ) intake plays a vital role in sustaining the environmental balance by influencing global carbon dynamics and climatic stability. This work addresses the production of sulfur-doped porous nanocarbons (SDCs) as prospective sorbents for CO 2 capture. SDCs were fabricated by utilizing coconut shell as a carbon precursor and potassium persulfate as both a chemical activating agent and a sulfur dopant. The incorporation of sulfur functionalities into carbon matrices creates structural variability and active sites, boosting CO 2 absorption capabilities. Sulfur's peculiar electrical structure allows greater intermolecular interactions with CO 2 , enhancing adsorption affinities. According to the experimental data, the CO 2 uptake was best measured as 3.37 mmol/g at 0(degrees)C and 1 bar and 2.56 mmol/g at 25 C-degrees and 1 bar. The results show that the higher porosity of SDC materials adds to a large amplification in the CO 2 uptake capability. The work underlines the delicate interaction between sulfur doping, morphological porosity, and surface reactivity in enhancing the effectiveness of CO 2 sequestration. SDC materials hold considerable promise in tackling the present ecological concerns and developing CO 2 collection techniques. The suggested single-step synthesis technique described here provides a sustainable and environmentally friendly method for synthesizing SDCs for carbon capture applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Computational Framework for Machine-Learning-Enabled 13 C Fluxomics

13 C metabolic flux analysis (MFA) has emerged as a powerful tool for synthetic biology. This optimization-based approach suffers long computation time and unstable solutions depending on the initial guess. Here, we develop a machine-learning-based framework for 13 C fluxomics. Specifically, training and test data sets are generated by metabolic network decomposition and flux sampling, in which flux ratios at metabolic nodes and simulated labeling patterns of metabolites are used as training targets and features, respectively. To improve prediction accuracy and simplify the model, automated processes are developed for flux ratio selection based on solvability and feature screening based on importance. We found that predictive performance can be significantly improved using both amino acids and central carbon metabolites in comparison with amino acids alone. Together with measured external fluxes, the predicted flux ratios determine the mass balance system, yielding global flux distributions. This approach is validated by flux estimation using both simulated and experimental data in comparison with canonical 13 C MFA. The approach represents a reliable fluxomics method readily applicable to high-throughput metabolic phenotyping, which highlights the advances of intelligent learning algorithms in synthetic biology, specifically in the Test and Learn stage of the Design-Build-Test-Learn cycle.

13C metabolic flux analysis↗

DOE OSTI2025

Three-Channel Sunphotometer Cloud Mode Value-Added Product Report

A primary source of uncertainty in Earth system model (ESM) predictions is the representation of cloud processes and associated cloud feedback. Several fundamental cloud properties critical to the understanding of aerosol-cloud interactions are poorly constrained by observations, with key deficiencies in our observations of cloud and precipitation droplet sizes and cloud optical depth. Observations of these cloud properties are often challenging to estimate from remote-sensing platforms and costly to obtain from in situ aircraft. Nevertheless, observations of boundary-layer clouds, and improved knowledge of stratocumulus cloud (Sc) processes, are especially important to ESM advancement. This is because these clouds have extensive coverage and exert controls on boundary-layer dynamics and the global radiative energy balance.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Balanced k -means clustering on an adiabatic quantum computer

Adiabatic quantum computers are a promising platform for efficiently solving challenging optimization problems. Therefore, many are interested in using these computers to train computationally expensive machine learning models. We present a quantum approach to solving the balanced k-means clustering training problem on the D-Wave 2000Q adiabatic quantum computer. In order to do this, we formulate the training problem as a quadratic unconstrained binary optimization (QUBO) problem. Unlike existing classical algorithms, our QUBO formulation targets the global solution to the balanced k-means model. We test our approach on a number of small problems and observe that despite the theoretical benefits of the QUBO formulation, the clustering solution obtained by a modern quantum computer is usually inferior to the solution obtained by the best classical clustering algorithms. Nevertheless, the solutions provided by the quantum computer do exhibit some promising characteristics. We also perform a scalability study to estimate the run time of our approach on large problems using future quantum hardware. Finally, as a final proof of concept, we used the quantum approach to cluster random subsets of the Iris benchmark data set.

97 MATHEMATICS AND COMPUTING↗