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DOE OSTI2023

Topology-enhanced mechanical stability of swelling nanoporous electrodes

Abstract Materials like silicon and germanium offer a 10-fold improvement in charge capacity over conventional graphite anodes in lithium-ion batteries but experience a roughly threefold volume increase during lithiation, which challenges ensuring battery integrity. Nanoporous silicon, created by liquid-metal-dealloying, is a potentially attractive anode design to mitigate this challenge, exhibiting both higher capacity and extended cycle lifetimes. However, how nanoporous structures accommodate the large volume change is unknown. Here, we address this question by using phase-field modeling to produce nanoporous particles and to investigate their elastoplastic swelling behavior and fracture. Our simulations show that enhanced mechanical stability results from the network topology consisting of ligaments connected by bulbous, sphere-like nodes. The ligaments forcefully resist elongation while the nodes, behaving like isolated spherical particles, experience large stresses driving fracture. However, being smaller compared to a sphere of the same volume as the entire nanoporous particle, the nodes are more protected against fracture.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Dark radiation constraints on portal interactions with hidden sectors

Here, we update dark radiation constraints on millicharged particle (MCP) and gauged baryon-number-minus-lepton-number (B-L) extensions of the Standard Model (SM). In these models, a massive SM gauge singlet mediator couples the SM plasma to additional SM-singlet light degrees of freedom. In the early Universe, these new light particles are populated via the interaction of the SM with the MCP, or the new B-L gauge boson, and act as dark radiation. The presence of dark radiation in the early Universe is tightly constrained by current and upcoming cosmic microwave background (CMB) measurements. We update bounds on MCPs from current measurements of N eff and show that future CMB experiments will be able to rule out or discover the extended MCP model invoked to explain the EDGES anomaly. Our analysis of the gauged B-L model goes beyond previous studies by including quantum-statistical and out-of-equilibrium effects. Further, we account for the finite lifetime of the B-L gauge boson, which boosts the subsequent right-handed neutrino energy density. We also develop a number of approximations and techniques for simplifying and solving the relevant Boltzmann equations. We use our approximations to develop a lower bound on the radiation density in a generic hidden sector with a light relic that is insensitive to the details of the hidden sector, provided the mediator interacts more strongly with the hidden sector than with the SM.

cosmological neutrinos↗

DOE OSTI2023

Strong Evidence for N 9 and the Limits of Existence of Atomic Nuclei

The boundaries of the Chart of Nuclides contain exotic isotopes that possess extreme proton-to-neutron asymmetries. Here we report on strong evidence of 9 N, one of the most exotic proton-rich isotopes where more than one half of its constitute nucleons are unbound. With seven protons and two neutrons, this extremely proton-rich system would represent the first-known example of a ground-state five-proton emitter. Here, the invariant-mass spectrum of its decay products can be fit with two peaks whose energies are consistent with the theoretical predictions of an open-quantum-system approach, however we cannot rule out the possibility that only a single resonance-like peak is present in the spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

From Cell to System: Accelerated hpc Simulations of BESS Aging under Frequency Regulation and Arbitrage use cases

Lithium-ion battery energy storage systems (BESS) packs have emerged as a leading solution for grid-scale energy storage, enhancing resiliency and balancing load fluctuations. Yet, experimental characterization of large-format LIB packs-particularly to assess performance and degradation over hundreds of cycles - demands substantial hardware investment and multi-year testing campaigns. In this work, we couple a hierarchical, physics-based modeling framework agnostic to electrode chemistries with high-performance computing to accelerate systems level evaluation by upto two orders of magnitude. Building on the open-source liionpack platform, we implement cell, module, and pack-scale electrochemical models enriched with mechanistic aging mechanisms and deploy them on an HPC cluster to simulate 150−200kWh systems over 500 - 1,000 cycles with in days. We subject these virtual B ESS to both constant-current cycling and realistic grid service profiles spanning frequency regulation, ramp-rate support, and energy arbitrage-and quantify the resulting degradation patterns. Our results reveal that localized cell aging can induce substantial nonuniformity at module and pack levels, with service-specific cycling protocols driving distinct aging modes. This rapid, multiscale modeling approach provides a powerful design-space exploration tool for optimizing electrical architecture, control strategies, and operational schedules to prolong pack lifetime and lower total cost of ownership.

Ayalasomayajula, Surya [ORNL] (ORCID:0009000860788↗

DOE OSTI2022

PyPVRPM: Photovoltaic Reliability and Performance Model in Python

The ability to perform accurate techno-economic analysis of solar photovoltaic (PV) systems is essential for bankability and investment purposes. Most energy yield models assume an almost flawless operation (i.e., no failures); however, realistically, components fail and get repaired stochastically. This package, PyPVRPM, is a Python translation and improvement of the Language Kit (LK) based PhotoVoltaic Reliability Performance Model (PVRPM), which was first developed at Sandia National Laboratories in Goldsim software (Granata et al., 2011) (Miller et al., 2012). PyPVRPM allows the user to define a PV system at a specific location and incorporate failure, repair, and detection rates and distributions to calculate energy yield and other financial metrics such as the levelized cost of energy and net present value (Klise, Lavrova, et al., 2017). Our package is a simulation tool that uses NREL’s Python interface for System Advisor Model (SAM) (National Renewable Energy Laboratory, 2020b) (National Renewable Energy Laboratory, 2020a) to evaluate the performance of a PV plant throughout its lifetime by considering component reliability metrics. Besides the numerous benefits from migrating to Python (e.g., speed, libraries, batch analyses), it also expands on the failure and repair processes from the LK version by including the ability to vary monitoring strategies. These failures, repairs, and monitoring processes are based on user-defined distributions and values, enabling a more accurate and realistic representation of cost and availability throughout a PV system’s lifetime.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Carrier Dynamics of Polar, Semipolar, and Nonpolar InGaN/GaN LEDs Measured by Small-Signal Electroluminescence

The carrier dynamics in InGaN/GaN light-emitting diodes (LEDs) are directly tied to their efficiency and maximum modulation speed, which are important metrics for solid-state lighting, displays, and optical communication. In this work, we measure the carrier dynamics of a variety of InGaN/GaN LEDs using small-signal electroluminescence methods [1]. A rate equation approach and associated small-signal circuit are used to model carrier injection, recombination in the active region, recombination in the cladding regions, and carrier escape. The model is fit to the measured optical frequency response (S21) and input impedance (S11) of the LEDs to extract the various carrier lifetimes, the carrier density, and the radiative and non-radiative recombination rates. We specifically study planar nonpolar and semipolar LEDs, which show record-high modulation speeds for III-nitride LEDs and present the modulation characteristics of core-shell nanowire-based LEDs. The planar nonpolar m-plane ($101\bar{0}$) micro-LEDs achieve a record-high -3dB modulation bandwidth for a III-nitride LED of 1.5 GHz [2]. The -3dB response of an electrically injected nanowire-based micro-LED with nonpolar facets is also reported, showing a -3dB bandwidth of 1.2 GHz [3]. The high speed is attributed to the shorter carrier lifetime associated with the nonpolar orientation. We also study the carrier dynamics in semipolar ($20\bar{2}\bar{1}$) LEDs for various temperatures [4]. Finally, we present carrier dynamics measurements on commercial-grade c-plane epitaxy for various active region designs, including a wavelength series and a growth quality series. The wavelength series offers insight into the contributions of the quantum confined Stark effect (QCSE) and InGaN material quality on the green gap [5]. The growth quality series investigates the role of non-radiative centers on the LED performance. Extraction of the carrier dynamics using small-signal electroluminescence offers insight into the factors limiting the efficiency and high-speed performance of III-nitride emitters and can be leveraged to ultimately improve the devices.

LEDs, InGaN, electroluminescence, bandwidth, modul↗

DOE OSTI2024

Computational design of high entropy alloy coating for hydrogen turbine applications

This project aims to develop novel high entropy alloy (HEA)-based coatings to protect critical components in hydrogen-fueled turbine power system. The HEA-coatings will demonstrate superior performance in hydrogen combustion environment to commercial NiCoCrAlY coating in current natural gas turbine system. The HEA coating facilitates the formation of a protective scale of alpha-alumina to slow down the inward diffusion of oxidizing species and the outward diffusion of metal elements, and possesses ultrahigh corrosion and spallation resistance to prolong the service lifetime of critical components in hydrogen turbine power system. Aimed to accelerate the discovery of novel HEA coating compositions, high throughput computational modeling including CALPHAD and density functional theory and machine learning are performed to predict phase stability, oxygen permeability, oxidation rate constant, coefficient of thermal expansion, and mechanical properties. Based on the modeling and machine learning prediction, experimental validation is performed. Preliminary results will be presented and approaches to minimize oxidation will be discussed.

alloy design↗

DOE OSTI2024

A digital twin solution for floating offshore wind turbines validated using a full-scale prototype

Abstract. In this work, we implement, verify, and validate a physics-based digital twin solution applied to a floating offshore wind turbine. The digital twin is validated using measurement data from the full-scale TetraSpar prototype. We focus on the estimation of the aerodynamic loads, wind speed, and section loads along the tower, with the aim of estimating the fatigue lifetime of the tower. Our digital twin solution integrates (1) a Kalman filter to estimate the structural states based on a linear model of the structure and measurements from the turbine, (2) an aerodynamic estimator, and (3) a physics-based virtual sensing procedure to obtain the loads along the tower. The digital twin relies on a set of measurements that are expected to be available on any existing wind turbine (power, pitch, rotor speed, and tower acceleration) and motion sensors that are likely to be standard measurements for a floating platform (inclinometers and GPS sensors). We explore two different pathways to obtain physics-based models: a suite of dedicated Python tools implemented as part of this work and the OpenFAST linearization feature. In our final version of the digital twin, we use components from both approaches. We perform different numerical experiments to verify the individual models of the digital twin. In this simulation realm, we obtain estimated damage equivalent loads of the tower fore–aft bending moment with an accuracy of approximately 5 % to 10 %. When comparing the digital twin estimations with the measurements from the TetraSpar prototype, the errors increased to 10 %–15 % on average. Overall, the accuracy of the results is promising and demonstrates the possibility of using digital twin solutions to estimate fatigue loads on floating offshore wind turbines. A natural continuation of this work would be to implement the monitoring and diagnostics aspect of the digital twin to inform operation and maintenance decisions. The digital twin solution is provided with examples as part of an open-source repository.

17 WIND ENERGY↗

DOE OSTI2023

Continuum Damage Mechanics Modeling of High-Temperature Flaw Propagation: Application to Creep Crack Growth In 316H Standardized Specimens and Nuclear Reactor Components

Predicting creep crack growth (CCG) of flaws found during operation in high-temperature alloy components is essential for assessing the remaining lifetime of those components. While defect assessment procedures are available for this purpose in design codes, these are limited in their range of applicability. This study assesses the application of a local damage-based finite-element methodology as a more general technique for the prediction of CCG at high temperatures on a variety of structural configurations. Numerical results for stainless steel 316H, which are validated against experimental data, show the promise of this approach. This integration of continuum damage mechanics (CDM) based methodologies, together with adequate inelastic models, into assessment procedures can therefore inform the characterization of CCG under complex operating conditions, while avoiding excessive conservatism. This article shows that such modeling frameworks can be calibrated to experimental data and used to demonstrate that the degree of tri-axiality ahead of a growing creep crack affects its rate of growth. The framework is also successfully employed in characterizing CCG in a realistic reactor pressure vessel geometry under an arbitrary loading condition. These results are particularly relevant to the nuclear power industry for defect assessment and inspections as part of codified practices of structural components with flaws in high-temperature reactors.

42 ENGINEERING↗

DOE OSTI2026

Collapse of Nuclear Collectivity along the 𝑁 = 𝑍 Line

The lifetime of the 𝐽 𝜋 = 2 + state in the self-conjugate 88 Ru nucleus has been determined in an experiment performed using rare-isotope beams provided by the new Facility for Rare Isotope Beams. This is the heaviest 𝑁 = 𝑍 nucleus for which such a measurement has been achieved. 88 Ru was populated by both one-neutron knockout and charge-exchange reactions, and the lifetime of 14.3$^{+2.5}_{−3.4}$ ps was determined using the triple-foil plunger technique. The extracted electromagnetic transition strength shows that the quadrupole collectivity has dropped significantly compared with the highly deformed 𝑁 = 𝑍 region around 𝐴 ∼ 80. These results are compared with state-of-the-art large-scale shell-model and discrete nonorthogonal shell-model calculations. The theoretical calculations indicate a moderate triaxial deformation and suggest that low-lying states in this nucleus are no longer dominated by strong many-particle many-hole excitations, unlike the lighter, highly deformed 𝑁 = 𝑍 nuclei nearby.

59 ≤ A ≤ 89↗

DOE OSTI2023

Application of NEAMS Multiphysics Framework for Species Tracking in Molten Salt Reactors

This report from Idaho National Laboratory (INL) summarizes the key modeling and simulation activities conducted under the Department of Energy (DOE) Molten Salt Reactor (MSR) Campaign during the Fiscal Year 2023 (FY23). The focus of the work was to leverage state-of-the-art modeling capabilities from the DOE Nuclear Energy Advanced Modeling and Simulation (NEAMS) codes to enable novel multiphysics and multiscale modeling and simulation of MSRs. Through collaboration with NEAMS code developers, advanced multiphysics analysis capabilities for MSR systems were demonstrated by coupling depletion, thermal-hydraulics, and thermochemistry into an innovative framework for chemical species transport in MSRs. As a result, the framework can track nuclides throughout their lifetimes in the core, from production (depletion) to advection throughout the salt volume (thermal-hydraulics) and off-gassing or precipitation outside of the salt (thermochemistry). This work supports the near-term deployment of MSRs by integrating the synergistic efforts between the DOE’s MSR Campaign and NEAMS program. The resulting framework will help better connect system design modelers with experimentalists to better understand and predict complex physical behaviors in MSRs. Researchers and MSR developers alike can now leverage these new modeling and simulation capabilities to perform novel analyses with applications including: • MSR dynamics during normal operational transients and accident scenarios • Off-gas system design and performance for fuel cycle and depletion analysis • Corrosion and active chemistry control for reactor component health and lifetime determination • Source term, decay heat and activity determination in accident scenarios • Special nuclear material accountancy and chemical forensic analysis for safeguards • Digital twin development of experiments and experimental reactor demonstrations • Measurement requirements for instrumentation and control design • Uncertainty and sensitivity analysis of missing data to inform future experimental data collection.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2021

Flipped SU(5) GUT phenomenology: proton decay and $\mathbf {g_\mu - 2}$

We consider proton decay and $\mathbf {g_\mu - 2}$ in flipped SU(5) GUT models. We first study scenarios in which the soft supersymmetry-breaking parameters are constrained to be universal at some high scale M in above the standard GUT scale where the QCD and electroweak SU(2) couplings unify. In this case the proton lifetime is typically > rsim10 36 years, too long to be detected in the foreseeable future, and the supersymmetric contribution to $\mathbf {g_\mu - 2}$ is too small to contribute significantly to resolving the discrepancy between the experimental measurement and data-driven calculations within the Standard Model. However, we identify a region of the constrained flipped SU(5) parameter space with large couplings between the 10- and 5-dimensional GUT Higgs representations where p → e + π 0 decay may be detectable in the Hyper-Kamiokande experiment now under construction, though the contribution to $\mathbf {g_\mu - 2}$ is still small. A substantial contribution to $\mathbf {g_\mu - 2}$ is possible, however, if the universality constraints on the soft supersymmetry-breaking masses are relaxed. We find a ‘quadrifecta’ region where observable proton decay co-exists with a (partial) supersymmetric resolution of the $\mathbf {g_\mu - 2}$ discrepancy and acceptable values of m h and the relic LSP density.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Quantifying the Impact of Excluding the Submersion Exposure Route for Existing Superfund Radionuclide Screening Level Calculator Soil and Tap Water Models

The U.S. Environmental Protection Agency (EPA) provides initial data screening guidelines for radionuclide-contaminated Superfund sites using preliminary remediation goals (PRGs) and dose compliance concentrations (DCCs). PRGs and DCCs are target concentration values based on acceptable excess lifetime cancer risk and annual dose limits, respectively. They are calculated for various environmental media that may be encountered by residential and worker land uses. PRGs and DCCs typically consist of multiple exposure routes. One of these routes is submersion, which is exposure to a gaseous or particulate radionuclide that is suspended in air. Currently, submersion is only included in air calculations. This study focused on determining whether factoring submersion into total PRG/DCC calculations for soil and tap water created a significant difference in the target concentrations. New equations for individual submersion PRGs/DCCs for each land use of interest for soil and tap water were developed. A wind-driven particulate emission factor and Andelman’s constant were used to model the amount of soil and vapor in the air from soil and household use of tap water, respectively. The submersion PRG/DCC was then included in the total PRG/DCC for each radionuclide, followed by a percent difference comparison of the old and new totals to quantify the impact of the change. For total soil PRGs/DCCs, with and without submersion, the difference was less than 1 percent; however, many of the tap water radionuclides analyzed – including multiple radon and polonium isotopes – showed as high as a 200 percent difference.This technical memorandum (TM) presents recommendations for updates to current EPA guidelines for initial data screens of radionuclide contaminated tap water.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Model to predict annual energy production loss based on blade erosion class

Leading edge erosion (LEE) of wind turbine blades has been identified as a major factor in decreased wind turbine blade lifetimes and energy output over time. Accordingly, the International Energy Agency Wind Technology Collaboration Programme (IEA Wind TCP) has created the Task 46 to undertake cooperative research in the key topic of blade erosion. Participants in the task are given in Table 1.

17 WIND ENERGY↗

DOE OSTI2022

Predicting Solar Cell Performance from Terahertz and Microwave Spectroscopy

Abstract Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current‐voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter‐laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br) 3 halide perovskite thin‐film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance‐free JV‐curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra‐grain charge transport is characterized by terahertz sum mobilities of ≈32 cm 2 V −1 s −1 . Drift‐diffusion simulations indicate that these intra‐grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best‐realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.

14 SOLAR ENERGY↗

DOE OSTI2021

Proton decays in 16 Ne and 18 Mg and isospin-symmetry breaking in carbon isotopes and isotones

We report that proton-rich nuclei possess unique properties in the nuclear chart. Due to the presence of both continuum coupling and Coulomb interaction, phenomena such as halos, Thomas-Ehrman shift, and proton emissions can occur. Relevant experimental data are difficult to obtain, so that theoretical calculations are needed to understand nuclei at drip lines and to guide experimentalists. In particular, the 16 Ne and 18 Mg isotopes are supposed to be one-proton and/or two-proton emitting nuclei, but associated experimental data are either incomplete or even unavailable. Consequently, we performed Gamow shell model calculations of carbon isotones bearing A = 15 - 18 . Isospin-symmetry breaking occurring in carbon isotones and isotopes is also discussed. It is hereby shown that the mixed effects of continuum coupling and Coulomb interaction at drip lines generate complex patterns in isospin multiplets. Added to that, it is possible to determine the one-proton and two-proton widths of 16 Ne and 18 Mg . Obtained decay patterns are in agreement with those obtained in previous experimental and theoretical works. Moreover, to our knowledge, this is the first theoretical calculation of binding energy and partial decay widths of 18 Mg in a configuration interaction picture.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Reductive Dynamic and Static Excited State Quenching of a Homoleptic Ruthenium Complex Bearing Aldehyde Groups

A new homoleptic Ru polypyridyl complex bearing two aldehyde groups on each bipyridine ligand, [Ru(dab) 3 ](PF 6 ) 2 , where dab is 4,4′-dicarbaldehyde-2,2′-bipyridine, was synthesized, characterized, and utilized for iodide photo-oxidation studies. In acetonitrile (CH 3 CN) solution, the complex displayed an intense metal-to-ligand charge transfer (MLCT) absorbance maximum at 475 nm (ε = 22,000 M –1 cm –1 ) and an infrared (IR) band at 1712 cm –1 assigned to the pendent aldehyde groups. Visible light excitation in air-saturated solution resulted in room temperature photoluminescence (PL) with a maximum at 675 nm, a quantum yield, ϕ PL = 0.048, and an excited state lifetime, τ ο = 440 ns, from which radiative and nonradiative relaxation rate constants were extracted, k r = 9.1 × 10 4 s –1 and knr = 1.8 × 10 6 s –1 . Pulsed visible light excitation yielded transient UV–vis and IR absorption spectra consistent with an MLCT excited state; relaxation occurred with the maintenance of two isosbestic points in the visible region, and a lifetime that agreed with that measured by time-resolved PL. Cyclic voltammetry studies in a CH 3 CN solution with 0.1 M TBAPF 6 electrolyte revealed a quasi-reversible oxidation, E°(Ru III/II ) = +1.25 V vs. Fc +/0 , and three sequential one-electron reductions at −1.10, −1.25, and −1.54 V vs. Fc +/0 . Here, an excited state reduction potential of E°(Ru *2+/+ ) = +0.89 V vs. Fc +/0 was estimated with the Rehm–Weller expression. Titration of tetrabutylammonium iodide, TBAI, into a CD 3 CN solution of [Ru(dab) 3 ](PF 6 ) 2 resulted in significant shifts in the aldehyde H atom and 3,3′-biypridyl resonances that were analyzed with a 1:1 equilibrium model, from which K eq = 460 M –1 was extracted, increasing to 5800 M –1 when the solvent was changed to acetone-d 6 . Iodide titrations resulted in a significant quenching of the [Ru(dab) 3 ] *2+ lifetime and quantum yield in both CH 3 CN and acetone solvents. In CH 3 CN, the quenching was mainly dynamic and well described by the Stern–Volmer model, from which a quenching rate constant, k q , of 4.5 × 10 10 M –1 s –1 and an equilibrium constant, K eq , of 8.3 × 10 3 M –1 were obtained. In acetone, the static quenching pathway by iodide was greatly enhanced, with a K eq of 1.2 × 10 4 M –1 and a higher k q of 9.2 × 10 10 M –1 s –1 .

Aldehydes↗

DOE OSTI2024

Solid breeder material crystal structure evolution due to Li burn up–Loss of crystal stability

Solid breeder materials for fusion power plants are subjected to extreme conditions of radiation damage, high temperature and designed component burn-up. Here, the loss of lattice stability of Li 2 TiO 3 due to Li burn-up was investigated using first principles-based approaches to aid evaluation of upper limit of component lifetime. The lattice stability is analyzed using calculated phonon dispersion in the Li 2 TiO 3 supercell, while Li burn-up is modeled by the introduction of Li-vacancies. It has been determined that the studied ceramic can be structurally stable up to ~40% of Li atoms burn-up. At 50% burn-up, the negative frequency branch in the phonon dispersion spectrum appears indicating the loss of lattice dynamical stability. Moreover, the structure obtained by introduction of unstable frozen phonons with minima energy amplitude also results in a phonon dispersion with negative branches in the structure obtained. Therefore, the system completely loses stability when approximately half of Li atoms are consumed.

36 MATERIALS SCIENCE↗