Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “ensemble methods”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 1,117 records · Page 62

Global Methane Budget 2000–2020

Abstract. Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. CH4 is the second most important human-influenced greenhouse gas in terms of climate forcing after carbon dioxide (CO2), and both emissions and atmospheric concentrations of CH4 have continued to increase since 2007 after a temporary pause. The relative importance of CH4 emissions compared to those of CO2 for temperature change is related to its shorter atmospheric lifetime, stronger radiative effect, and acceleration in atmospheric growth rate over the past decade, the causes of which are still debated. Two major challenges in quantifying the factors responsible for the observed atmospheric growth rate arise from diverse, geographically overlapping CH4 sources and from the uncertain magnitude and temporal change in the destruction of CH4 by short-lived and highly variable hydroxyl radicals (OH). To address these challenges, we have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to improve, synthesise, and update the global CH4 budget regularly and to stimulate new research on the methane cycle. Following Saunois et al. (2016, 2020), we present here the third version of the living review paper dedicated to the decadal CH4 budget, integrating results of top-down CH4 emission estimates (based on in situ and Greenhouse Gases Observing SATellite (GOSAT) atmospheric observations and an ensemble of atmospheric inverse-model results) and bottom-up estimates (based on process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven extrapolations). We present a budget for the most recent 2010–2019 calendar decade (the latest period for which full data sets are available), for the previous decade of 2000–2009 and for the year 2020. The revision of the bottom-up budget in this 2025 edition benefits from important progress in estimating inland freshwater emissions, with better counting of emissions from lakes and ponds, reservoirs, and streams and rivers. This budget also reduces double counting across freshwater and wetland emissions and, for the first time, includes an estimate of the potential double counting that may exist (average of 23 Tg CH4 yr−1). Bottom-up approaches show that the combined wetland and inland freshwater emissions average 248 [159–369] Tg CH4 yr−1 for the 2010–2019 decade. Natural fluxes are perturbed by human activities through climate, eutrophication, and land use. In this budget, we also estimate, for the first time, this anthropogenic component contributing to wetland and inland freshwater emissions. Newly available gridded products also allowed us to derive an almost complete latitudinal and regional budget based on bottom-up approaches. For the 2010–2019 decade, global CH4 emissions are estimated by atmospheric inversions (top-down) to be 575 Tg CH4 yr−1 (range 553–586, corresponding to the minimum and maximum estimates of the model ensemble). Of this amount, 369 Tg CH4 yr−1 or ∼ 65 % is attributed to direct anthropogenic sources in the fossil, agriculture, and waste and anthropogenic biomass burning (range 350–391 Tg CH4 yr−1 or 63 %–68 %). For the 2000–2009 period, the atmospheric inversions give a slightly lower total emission than for 2010–2019, by 32 Tg CH4 yr−1 (range 9–40). The 2020 emission rate is the highest of the period and reaches 608 Tg CH4 yr−1 (range 581–627), which is 12 % higher than the average emissions in the 2000s. Since 2012, global direct anthropogenic CH4 emission trends have been tracking scenarios that assume no or minimal climate mitigation policies proposed by the Intergovernmental Panel on Climate Change (shared socio-economic pathways SSP5 and SSP3). Bottom-up methods suggest 16 % (94 Tg CH4 yr−1) larger global emissions (669 Tg CH4 yr−1, range 512–849) than top-down inversion methods for the 2010–2019 period. The discrepancy between the bottom-up and the top-down budgets has been greatly reduced compared to the previous differences (167 and 156 Tg CH4 yr−1 in Saunois et al. (2016, 2020) respectively), and for the first time uncertainties in bottom-up and top-down budgets overlap. Although differences have been reduced between inversions and bottom-up, the most important source of uncertainty in the global CH4 budget is still attributable to natural emissions, especially those from wetlands and inland freshwaters. The tropospheric loss of methane, as the main contributor to methane lifetime, has been estimated at 563 [510–663] Tg CH4 yr−1 based on chemistry–climate models. These values are slightly larger than for 2000–2009 due to the impact of the rise in atmospheric methane and remaining large uncertainty (∼ 25 %). The total sink of CH4 is estimated at 633 [507–796] Tg CH4 yr−1 by the bottom-up approaches and at 554 [550–567] Tg CH4 yr−1 by top-down approaches. However, most of the top-down models use the same OH distribution, which introduces less uncertainty to the global budget than is likely justified. For 2010–2019, agriculture and waste contributed an estimated 228 [213–242] Tg CH4 yr−1 in the top-down budget and 211 [195–231] Tg CH4 yr−1 in the bottom-up budget. Fossil fuel emissions contributed 115 [100–124] Tg CH4 yr−1 in the top-down budget and 120 [117–125] Tg CH4 yr−1 in the bottom-up budget. Biomass and biofuel burning contributed 27 [26–27] Tg CH4 yr−1 in the top-down budget and 28 [21–39] Tg CH4 yr−1 in the bottom-up budget. We identify five major priorities for improving the CH4 budget: (i) producing a global, high-resolution map of water-saturated soils and inundated areas emitting CH4 based on a robust classification of different types of emitting ecosystems; (ii) further development of process-based models for inland-water emissions; (iii) intensification of CH4 observations at local (e.g. FLUXNET-CH4 measurements, urban-scale monitoring, satellite imagery with pointing capabilities) to regional scales (surface networks and global remote sensing measurements from satellites) to constrain both bottom-up models and atmospheric inversions; (iv) improvements of transport models and the representation of photochemical sinks in top-down inversions; and (v) integration of 3D variational inversion systems using isotopic and/or co-emitted species such as ethane as well as information in the bottom-up inventories on anthropogenic super-emitters detected by remote sensing (mainly oil and gas sector but also coal, agriculture, and landfills) to improve source partitioning. The data presented here can be downloaded from https://doi.org/10.18160/GKQ9-2RHT (Martinez et al., 2024).

54 ENVIRONMENTAL SCIENCES↗

Computationally efficient and error aware surrogate construction for numerical solutions of subsurface flow through porous media

Limiting the injection rate to restrict the pressure below a threshold at a critical location can be an important goal of simulations that model the subsurface pressure between injection and extraction wells. The pressure is approximated by the solution of Darcy’s partial differential equation for a given permeability field. The subsurface permeability is modeled as a random field since it is known only up to statistical properties. This induces uncertainty in the computed pressure. Solving the partial differential equation for an ensemble of random permeability simulations enables estimating a probability distribution for the pressure at the critical location. These simulations are computationally expensive, and practitioners often need rapid online guidance for real-time pressure management. An ensemble of numerical partial differential equation solutions is used to construct a Gaussian process regression model that can quickly predict the pressure at the critical location as a function of the extraction rate and permeability realization. The Gaussian process surrogate analyzes the ensemble of numerical pressure solutions at the critical location as noisy observations of the true pressure solution, enabling robust inference using the conditional Gaussian process distribution. Our first novel contribution is to identify a sampling methodology for the random environment and matching kernel technology for which fitting the Gaussian process regression model scales as O ( n log n ) instead of the typical O ( n 3 ) rate in the number of samples n used to fit the surrogate. The surrogate model allows almost instantaneous predictions for the pressure at the critical location as a function of the extraction rate and permeability realization. Our second contribution is a novel algorithm to calibrate the uncertainty in the surrogate model to the discrepancy between the true pressure solution of Darcy’s equation and the numerical solution. Finally, although our method is derived for building a surrogate for the solution of Darcy’s equation with a random permeability field, the framework broadly applies to solutions of other partial differential equations with random coefficients.

54 ENVIRONMENTAL SCIENCES↗

Nanoscale Spatial Distribution of Supported Nanoparticles Controls Activity and Stability in Powder Catalysts for CO Oxidation and Photocatalytic H 2 Evolution

Here we discuss, supported metal nanoparticles are essential components of high-performing catalysts, and their structures are intensely researched. In comparison, nanoparticle spatial distribution in powder catalysts is conventionally not quantified, and the influence of this collective property on catalyst performance remains poorly investigated. Here, we demonstrate a general colloidal self-assembly method to control uniformity of nanoparticle spatial distribution on common industrial powder supports. We quantify distributions on the nanoscale using image statistics and show that the type of nanospatial distribution determines not only the stability, but also the activity of heterogeneous catalysts. Widely investigated systems (Au–TiO 2 for CO oxidation thermocatalysis and Pd–TiO 2 for H 2 evolution photocatalysis) were used to showcase the universal importance of nanoparticle spatial organization. Spatially and temporally resolved microkinetic modeling revealed that nonuniformly distributed Au nanoparticles suffer from local depletion of surface oxygen, and therefore lower CO oxidation activity, as compared to uniformly distributed nanoparticles. Nanoparticle spatial distribution also determines the stability of Pd–TiO 2 photocatalysts, because nonuniformly distributed nanoparticles sinter while uniformly distributed nanoparticles do not. This work introduces new tools to evaluate and understand catalyst collective (ensemble) properties in powder catalysts, which thereby pave the way to more active and stable heterogeneous catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Group-kinetic theory of turbulence

The two phases are governed by two coupled systems of Navier-Stokes equations. The couplings are nonlinear. These equations describe the microdynamical state of turbulence, and are transformed into a master equation. By scaling, a kinetic hierarchy is generated in the form of groups, representing the spectral evolution, the diffusivity and the relaxation. The loss of memory in formulating the relaxation yields the closure. The network of sub-distributions that participates in the relaxation is simulated by a self-consistent porous medium, so that the average effect on the diffusivity is to make it approach equilibrium. The kinetic equation of turbulence is derived. The method of moments reverts it to the continuum. The equation of spectral evolution is obtained and the transport properties are calculated. In inertia turbulence, the Kolmogoroff law for weak coupling and the spectrum for the strong coupling are found. As the fluid analog, the nonlinear Schrodinger equation has a driving force in the form of emission of solitons by velocity fluctuations, and is used to describe the microdynamical state of turbulence. In order for the emission together with the modulation to participate in the transport processes, the non-homogeneous Schrodinger equation is transformed into a homogeneous master equation. By group-scaling, the master equation is decomposed into a system of transport equations, replacing the Bogoliubov system of equations of many-particle distributions. It is in the relaxation that the memory is lost when the ensemble of higher-order distributions is simulated by an effective porous medium. The closure is thus found. The kinetic equation is derived and transformed into the equation of spectral flow.

Tchen, C. M.↗

Improving Lightning NO(x) Parameterizations for Global Chemical Transport Models

Parameterization of lightning NO(x) in global chemical transport models requires a method to specify the temporal and geographic distribution of flash rates, an estimate of NO production per flash, and a method to specify the effective vertical distribution of NO production. Flash rate parameterizations using the upward convective cloud mass flux have been developed and tested for several GCM and assimilated meteorological data sets. This parameterization and others involving the cloud-top height and convective precipitation provide a generally acceptable climatological distribution of flashes after normalization with satellite data. However, considerable improvement in terms of geographic and temporal variability may be achieved in the future using cloud microphysics data available from next-generation GCMs. Cloud-resolving case-study simulations of convective transport and lightning NO production have yielded results which are directly applicable to the NO production per flash and the vertical NO distribution portions of the global model lightning parameterizations. In this work we have used cloud-resolving models (the Goddard Cumulus Ensemble Model (GCE) and MM5) to drive an off-line cloud-scale chemical transport model (CSCTM). The CSCTM, in conjunction with aircraft measurements of NO(x) in thunderstorms and ground-based lightning observations, has been used to constrain the amount of NO produced per flash. Observed lightning flash rates have been incorporated into the CSCTM, and several scenarios of NO production per intracloud (IC) and per cloud-to-ground (CG) flash have been tested in each of several case study storms. The resulting NO(x) mixing ratios are compared with aircraft measurements taken within the storm (typically the anvil region) to determine the most likely NO production scenario. The range of values of NO production per flash (or per meter of lightning channel length) that have been deduced from the model will be shown and compared with values of production in the literature that have been deduced from observed NO spikes and from anvil flux calculations. Results show that on a per flash basis, IC flashes are nearly as productive of NO as CG flashes. Estimates of mean NO production per flash vary by a factor of three from one simulated storm to another. Vertical profiles of lightning NOx mass at the end of the 3-D storm simulations have been summarized to yield suggested profiles for use in global models. These profiles show a larger percentage of the total lightning NO(x) mass in the free troposphere than those suggested by Pickering et al. (1998).

Pickering, Kenneth E.↗

Fundamental microscopic properties as predictors of large-scale quantities of interest: Validation through grain boundary energy trends

Correlations between fundamental microscopic properties computable from first principles, which we term canonical properties, and complex large-scale quantities of interest (QoIs) provide an avenue to predictive materials discovery. Here, we propose that such correlations can be efficiently discovered through simulations utilizing approximate interatomic potentials (IPs), which serve as an ensemble of “synthetic materials”. As a proof of principle we build a regression model relating canonical properties to the symmetric tilt grain boundary (GB) energy curves in face-centered cubic crystals, characterized by the scaling factor in the universal lattice matching model of Runnels et al. (2016), which we take to be our QoI. Our analysis recovers known correlations of GB energy to other properties and discovers new ones. We also demonstrate, using available density functional theory (DFT) GB energy data, that the regression model constructed from IP data is consistent with DFT results, confirming the assumption that the IPs and DFT belong to same statistical pool and thereby validating the approach. Regression models constructed in this fashion can be used to predict large-scale QoIs based on first-principles data and provide a general method for training IPs for QoIs beyond the scope of first-principles calculations.

36 MATERIALS SCIENCE↗

Quantum Emitter Formation Dynamics and Probing of Radiation-Induced Atomic Disorder in Silicon

Near-infrared color centers in silicon are emerging candidates for on-chip integrated quantum emitters, optical-access quantum memories, and sensing. We access ensemble G-color-center formation dynamics and radiation-induced atomic disorder in silicon for a series of megaelectronvolt proton-flux conditions. The photoluminescence results reveal that the G centers are formed more efficiently by pulsed-proton irradiation than by continuous-wave proton irradiation. The enhanced transient excitations and dynamic annealing within nanoseconds allows optimization of the ratio of G-center formation to nonradiative defect accumulation. The G centers preserve narrow line widths of about 0.1 nm when they are generated by moderate pulsed-proton fluences, while the line width broadens significantly as the pulsed-proton fluence increases. This implies vacancy or interstitial clustering by overlapping collision cascades. The tracking of G-center properties for a series of irradiation conditions enables sensitive probing of atomic disorder, serving as a complementary analytical method for sensing damage accumulation. Aided by ab initio electronic structure calculations, we provide insight into the atomic disorder induced inhomogeneous broadening by introducing vacancies, silicon interstitials, and oriented strain fields in the vicinity of a G center. A vacancy leads to a tensile strain and can result in either a red shift or a blue shift of the G-center emission, depending on its position relative to the G center. Meanwhile, Si interstitials lead to compressive strain, which results in a monotonic red shift. In conclusion, high-flux and tunable ion pulses enable the exploration of the fundamental dynamics of radiation-induced defects as well as methods for the optimization of G-center formation and qubit synthesis for quantum information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Celebrating 10 Years of the Sub-Seasonal to Seasonal Prediction Project and Looking to the Future

The conference clearly demonstrated the increasing interest and growth of the scientific community working on the development and application of sub-seasonal to seasonal prediction since the start of the World Weather Research Programme (WWRP)/World Climate Research Programme (WCRP) sub-seasonal to seasonal (S2S) prediction project in 2013. The conference, which was held at the University of Reading (United Kingdom), was organized into three main themes as briefly summarized below, with eleven invited talks, 74 oral contributed talks, and 101 posters. The conference also included a two-hour breakout session, wherein eight groups discussed the current state and prospect for S2S prediction, and an early career researcher event. A summary of these discussions and recommendations is presented below. The conference web page (https://research.reading.ac.uk/s2s-summit2023/) is archived at the University of Reading. Introductory comments by representatives of the World Meteorological Organization (WMO) WWRP and WCRP emphasized the importance of the weather–climate linkage, targeted by S2S forecasts (from 2 weeks to a season ahead), addressing the challenges of creating “end-to-end” forecasts that encompass the entire climate-services chain from the prediction science and forecast, to the development and issuing of forecast products tailored to informing user-decisions. They also emphasized the efficacy of multi-model ensemble efforts and databases to foster collaborations internationally and between operational centres and academia. Although the WWRP/WCRP S2S project comes to an end in 2023, S2S prediction will remain an important focus for WWRP and WCRP. In WWRP, a new project called SAGE (Sub-seasonal to seasonal predictions for Agriculture and Environment) will start in 2024. Another important legacy of the S2S project will be the maintenance of the S2S database (Vitart et al. 2017) and the establishment of a WMO Lead Center for sub-seasonal prediction multi-model ensemble (LC-SSPMME) which will provide real-time multi-model S2S climate information. In two keynote presentations, Prof. Brian Hoskins (University of Reading) and Dr. Gilbert Brunet (Australian Bureau of Meteorology) discussed the potential of S2S predictability and the ongoing journey for understanding and improving these predictions. This conference was a sequel to the International Conference on Sub-seasonal to Seasonal Prediction (Robertson et al., 2014) which took place in College Park (Maryland, USA) in February 2014 to celebrate the start of the WWRP/WCRP S2S project, and to WCRP and WWRP conferences in Boulder, USA, in 2018 (Merryfield et al., 2020). A significant development compared to the previous S2S conferences was the large number of presentations on research to operation (R2O) and S2S applications and on the use of artificial intelligence and machine learning (AI/ML) methods for S2S prediction. Some of these methods provide empirical S2S forecasts which are competitive with state-of-the-art dynamical models. Other presentations demonstrated that AI/ML can provide alternative calibration of dynamical model outputs to traditional methods. Several talks and posters highlighted the increasing use of AI/ML, including deep learning, in S2S forecast post-processing and using AI to identify higher flow-dependent skill. Finally, some presentations demonstrated the value of AI/ML methods for a better understanding of S2S sources of predictability and attribution of extreme events.

S. J. Woolnough↗

Understanding and Utilizing PBL Height Data from Multiple Observing Systems in the GEOS System

The accuracy of PBL height simulation is a key issue in many applications including forecasting near surface meteorology and air quality, however, it is a very challenging problem due to the lack of not only comprehensive, global Planetary Boundary Layer (PBL) observations but also a strategy and infrastructure to utilize PBL height data from a variety of sensors. Following the designation of PBL as an incubation class observable in the 2017 Decadal Survey, the PBL Incubation Study Team Report [14] made clear that “a future global PBL observing system requires modeling and data assimilation as essential components.” There is an urgent need for global modeling development in order to utilize Program of Record (POR) observations, assess their impacts, and identify gaps to be filled by future PBL missions. Our overall objective is to develop PBL data assimilation capabilities in the NASA Global Earth Observing System (GEOS), focusing on PBL height from multiple observing systems, to support the assessment and use of future PBL observations. The NASA GEOS system is composed of the GEOS global atmospheric general circulation model (AGCM) and the atmospheric data assimilation system (ADAS). The PBL parameterizations include the “Lock” K-profile scheme driven by surface and cloud-top buoyancy fluxes ([4]), and the “Louis” local scheme for stable conditions based on the Richardson number ([5]). Above the mixed layer defined by the Lock surface plume, shallow cumulus convection is represented by the mass flux scheme of [9]. Additional parameterizations are summarized in [1]. The ADAS employs the hybrid 4D Ensemble- Variational (EnVar) configuration ([15]), with the ensemble providing flow-dependent background error covariance information. The resultant analysis increments are fed back to the forecast model through the 4D incremental analysis update (IAU) approach ([11]). In this study, PBL height data are being or have been generated from radiosondes, GNSS RO, satellite (CATS, CALIPSO and ICESat-2) and ground-based (MPLNET) lidars, and wind profiler. Investigations have been conducted to specify quality marks for PBL height retrievals for the data assimilation purpose. These PBL height data have different strengths and weaknesses ([2], [3], [6], [7], [8], [10]), and the satellite PBL height data provide better global coverage and complement in-situ PBL height data. Radiosondes offer high accuracy and in situ measurement of temperature and humidity profiles, but with poor spatio-temporal sampling. The in-situ observing systems like MPLNET and wind profiler provide long history of PBL height records at each station. The GNSS RO based PBL height is retrieved based on the sharp gradients in refractivity profile that represent the fine vertical structure of temperature and moisture changes above the PBL. However, not all RO refractivity profiles reach the surface depending on location and regime, and RO refractivity retrievals can be negatively biased below 2km. The PBL height data from satellite lidars provide high resolution along track PBL height retrievals, but over land they are affected by previous day convective PBL aerosol and strongly associated with mixing layer and retrievals cannot be made below thick, attenuating clouds. A successful assimilation of PBL height data requires a thorough understanding of the observing method and the retrieval algorithm for each observing system in order to use the PBL height data from multiple observing systems properly. Due to the sensitivity of PBL height data to the observing method and choice of algorithm, it is important to use a model definition appropriate for each observation type to compute differences between PBL height data and model PBL height (OmFs). The GEOS model currently includes two PBL height definitions suitable for direct comparison with observed PBL height, and additional definitions are being added in this study. Evaluation of different model PBL height definitions is underway. Meanwhile, efforts have been made in the GEOS data assimilation system to develop PBL height data assimilation capability. PBL height data can be assimilated using two different approaches. The traditional approach is to construct an observation operator and its tangent linear and adjoint, which link control variables to PBL height data from each observing system. This observation operator can be very complicated, e.g., the lidar-based PBL height observation operator includes the backscatter lidar forward observation operator, the algorithm to derive PBL height from attenuated total backscatter, interpolation, and calculations handling the mismatch between observed and model scales. The other approach is to augment PBL height to the control variable vector, and it is adopted in this study. The latter approach was also used in previous studies, e.g., the assimilation of PBL height data from radiosonde and aircraft in the Real Time Mesoscale Analysis (RTMA) system for a dispersion modelling study ([13]); the PBL height assimilation study using lidar PBL height data at Greensburg, Kansas for a field campaign ([12]). The PBL height assimilation from multiple observing systems in this study allows us to take advantage of the diverse PBL height data that provide much better global coverage collectively under different meteorological conditions and with different temporal and spatial scales. As all the PBL heights are tightly coupled with the PBL thermodynamic variables, the strong correlations, which are provided by the 4D ensemble forecast, enable PBL height data from various sources to interact and combine coherently and provide additional information for PBL temperature and moisture fields. The results of comparisons among PBL height data from different sources and the evaluation of the model PBL height definitions with the PBL height data will be presented, and the PBL height data synergy strategies and preliminary results will also be discussed at the conference.

Y. Zhu↗

Nature of Zirconia on a Copper Inverse Catalyst Under CO 2 Hydrogenation Conditions

The growing concern over the escalating levels of anthropogenic CO 2 emissions necessitates effective strategies for its conversion to valuable chemicals and fuels. In this research, we embark on a comprehensive investigation of the nature of zirconia on a copper inverse catalyst under the conditions of CO 2 hydrogenation to methanol. We employ density functional theory calculations in combination with the Grand Canonical Basin Hopping method, enabling an exploration of the free energy surface including a variable amount of adsorbates within the relevant reaction conditions. Our focus centers on a model three-atom Zr cluster on a Cu(111) surface decorated with various OH, O, and formate ligands, noted Zr 3 O x (OH) y (HCOO) z /Cu(111), revealing major changes in the active site induced by various reaction parameters such as the gas pressure, temperature, conversion levels, and CO 2 /H 2 feed ratios. Further, through our analysis, we have unveiled insights into the dynamic behavior of the catalyst. Specifically, under reaction conditions, we observe a large number of composition and structures with similar free energy for the catalyst, with respect to changing the type, number, and binding sites of adsorbates, suggesting that the active site should be regarded as a statistical ensemble of diverse structures that interconvert.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluating Enhanced Reservoir Evaporation Losses From CMIP6‐Based Future Projections in the Contiguous United States

Abstract Enhanced reservoir evaporation has become an emerging concern regarding water loss, especially when compounded with the ever‐increasing water demand. In this study, we evaluated the evaporation rates and losses for 678 major reservoirs (representing nearly 90% of total storage capacity) in the Contiguous United States over historical baseline (1980–2019), near‐term (2020–2039), and mid‐term (2040–2059) future periods. The evaporation rate was estimated using the Lake Evaporation Model (LEM), an advanced lake evaporation model that addresses both heat storage and fetch effects, driven by multi‐ensemble downscaled Coupled Model Intercomparison Projects 6 (CMIP6) projections under the SSP585 emission scenario. The results project that the evaporation loss may increase by 2.5 × 10 7 m 3 /yr through the research period (1980–2059). Among all regions, the Rio Grande is projected to have the largest increasing rate in the near‐term and mid‐term future, with values of 7.11% of 10.25%, respectively. At the seasonal scale, the most significant increase in the evaporation rate is projected during the fall. The evaporation is projected to increase faster than the streamflow over many of the regions in the southwestern US during the summer/fall, suggesting that the shortage of water will be further exacerbated. The climate models contribute the most to the variance, as compared to the other components related to the projection of evaporation losses (e.g., hydrological model, downscaling method, and historical meteorological data set). These findings demonstrate the need to consider accelerated water loss through open water evaporation in long‐term water resources planning across various spatiotemporal scales.

54 ENVIRONMENTAL SCIENCES↗

Collaborative Supervised Learning for Sensor Networks

Collaboration methods for distributed machine-learning algorithms involve the specification of communication protocols for the learners, which can query other learners and/or broadcast their findings preemptively. Each learner incorporates information from its neighbors into its own training set, and they are thereby able to bootstrap each other to higher performance. Each learner resides at a different node in the sensor network and makes observations (collects data) independently of the other learners. After being seeded with an initial labeled training set, each learner proceeds to learn in an iterative fashion. New data is collected and classified. The learner can then either broadcast its most confident classifications for use by other learners, or can query neighbors for their classifications of its least confident items. As such, collaborative learning combines elements of both passive (broadcast) and active (query) learning. It also uses ideas from ensemble learning to combine the multiple responses to a given query into a single useful label. This approach has been evaluated against current non-collaborative alternatives, including training a single classifier and deploying it at all nodes with no further learning possible, and permitting learners to learn from their own most confident judgments, absent interaction with their neighbors. On several data sets, it has been consistently found that active collaboration is the best strategy for a distributed learner network. The main advantages include the ability for learning to take place autonomously by collaboration rather than by requiring intervention from an oracle (usually human), and also the ability to learn in a distributed environment, permitting decisions to be made in situ and to yield faster response time.

Wagstaff, Kiri L.↗

A model-free method for mass spectrometer response correction

A new method for correction of mass spectrometer output signals is described. Response-time distortion is reduced independently of any model of mass spectrometer behavior. The delay of the system is found first from the cross-correlation function of a step change and its response. A two-sided time-domain digital correction filter (deconvolution filter) is generated next from the same step response data using a regression procedure. Other data are corrected using the filter and delay. The mean squared error between a step response and a step is reduced considerably more after the use of a deconvolution filter than after the application of a second-order model correction. O2 consumption and CO2 production values calculated from data corrupted by a simulated dynamic process return to near the uncorrupted values after correction. Although a clean step response or the ensemble average of several responses contaminated with noise is needed for the generation of the filter, random noise of magnitude not above 0.5 percent added to the response to be corrected does not impair the correction severely.

Shykoff, Barbara E.↗

Screening Cu-Zeolites for Methane Activation Using Curriculum-Based Training

Machine learning (ML), when used synergistically with atomistic simulations, has recently emerged as a powerful tool for accelerated catalyst discovery. However, the application of these techniques has been limited by the lack of interpretable and transferable ML models. In this work, we propose a curriculum-based training (CBT) philosophy to systematically develop reactive machine learning potentials (rMLPs) for high-throughput screening of zeolite catalysts. Our CBT approach combines several different types of calculations to gradually teach the ML model about the relevant regions of the reactive potential energy surface. The resulting rMLPs are accurate, transferable, and interpretable. We further demonstrate the effectiveness of this approach by exhaustively screening thousands of [CuOCu] 2+ sites across hundreds of Cu-zeolites for the industrially relevant methane activation reaction. Specifically, this large-scale analysis of the entire International Zeolite Association (IZA) database identifies a set of previously unexplored zeolites (i.e., MEI, ATN, EWO, and CAS) that show the highest ensemble-averaged rates for [CuOCu] 2+ -catalyzed methane activation. We believe that this CBT philosophy can be generally applied to other zeolite-catalyzed reactions and, subsequently, to other types of heterogeneous catalysts. Thus, this represents an important step toward overcoming the long-standing barriers within the computational heterogeneous catalysis community.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Scalable learning of potentials to predict time-dependent Hartree–Fock dynamics

We propose a framework to learn the time-dependent Hartree–Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Although the entire TDHF Hamiltonian, including the inter-electronic potential, can be computed from first principles, we use this problem as a testbed to develop strategies that can be applied to learn a priori unknown terms that arise in other methods/approaches to quantum dynamics, e.g., emerging problems such as learning exchange–correlation potentials for time-dependent density functional theory. We develop, train, and test three models of the TDHF inter-electronic potential, each parameterized by a four-index tensor of size up to 60 × 60 × 60 × 60. Two of the models preserve Hermitian symmetry, while one model preserves an eight-fold permutation symmetry that implies Hermitian symmetry. Across seven different molecular systems, we find that accounting for the deeper eight-fold symmetry leads to the best-performing model across three metrics: training efficiency, test set predictive power, and direct comparison of true and learned inter-electronic potentials. All three models, when trained on ensembles of field-free trajectories, generate accurate electron dynamics predictions even in a field-on regime that lies outside the training set. To enable our models to scale to large molecular systems, we derive expressions for Jacobian-vector products that enable iterative, matrix-free training.

97 MATHEMATICS AND COMPUTING↗

Dynamic data-driven multiscale modeling for predicting the degradation of a 316L stainless steel nuclear cladding material

Here, we have developed a long short-term memory stacked ensemble (LSTM-SE) surrogate modeling approach that can provide rapid predictions of microstructural evolution and the resultant mechanical properties of American Iron and Steel Institute (AISI) 316L series stainless steel (316LSS) fuel cladding under conditions of varying temperature and radiation dose rate. To acquire training data, we developed and implemented a kinetic Monte Carlo (KMC) model to simulate precipitation kinetics of M 23 C 6 , γ', and G phases within SS316L cladding. Experimentally reported precipitation kinetics of SS316L in literature were linked to the kinetic parameters of the simulated precipitation in our KMC model. The model was then used to simulate microstructure evolution under synthetically generated treatments of varying temperature and radiation dose rate, for periods of up to 3000 hours. Changes in volume fraction, number density, and particle size of precipitates were recorded, and particle area fractions were correlated using statistical methods to develop the surrogate model. Simultaneously, the mechanical properties of the simulated microstructures were evaluated using microstructure-based finite element method (FEM) analysis to determine the elastic modulus, yield stress, ultimate tensile strength, and elongation to failure of the aged microstructures. Using this approach, our surrogate model can predict precipitation behavior within 0.25% volume fraction and mechanical properties within 6% relative error from the values predicted by the KMC and FEM models using 50 training simulations as input. The trained recurrent neural network-based model can return estimations of precipitation kinetics and mechanical properties ~1000 times faster than the physics-based codes. This work demonstrates, as a proof of concept, that reactor material service lifetimes under variable service conditions can be predicted for a statistics-based model from a practicably obtainable dataset.

36 MATERIALS SCIENCE↗

Dynamic Data-Driven Multiscale Modeling for Predicting Microstructure and Mechanical Properties of 316L Stainless Steel

We have developed a long short-term memory stacked ensemble (LSTM-SE) surrogate modeling approach that can provide rapid predictions of microstructural evolution and the resultant mechanical properties of American Iron and Steel Institute (AISI) 316L series stainless steel (316LSS) fuel cladding under conditions of varying temperature and radiation dose rate. To acquire training data, we developed and implemented a kinetic Monte Carlo (KMC) model to simulate precipitation kinetics of M 23 C 6 , γ', and G phases within SS316L cladding. Experimentally reported precipitation kinetics of SS316L in literature were linked to the kinetic parameters of the simulated precipitation in our KMC model. The model was then used to simulate microstructure evolution under synthetically generated treatments of varying temperature and radiation dose rate, for periods of up to 3000 hours. Changes in volume fraction, number density, and particle size of precipitates were recorded, and particle area fractions were correlated using statistical methods to develop the surrogate model. Simultaneously, the mechanical properties of the simulated microstructures were evaluated using microstructure-based finite element method (FEM) analysis to determine the elastic modulus, yield stress, ultimate tensile strength, and elongation to failure of the aged microstructures. Using this approach, our surrogate model can predict precipitation behavior within 0.25% volume fraction and mechanical properties within 6% relative error from the values predicted by the KMC and FEM models using 50 training simulations as input. The trained recurrent neural network-based model can return estimations of precipitation kinetics and mechanical properties ~1000 times faster than the physics-based codes. This work demonstrates, as a proof of concept, that reactor material service lifetimes under variable service conditions can be predicted for a statistics-based model from a practicably obtainable dataset.

36 MATERIALS SCIENCE↗