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DOE OSTI2020

Electron transfer in nonpolar media

The Marcus theory of electron transfer views fluctuating orientations of permanent dipoles as the nuclear mode bringing the donor and acceptor into the tunneling resonance. Electronic polarization of the solvent is excluded as the fast mode adiabatically following the electronic density. This view, valid for solids, does not apply to molecular liquids where molecular translations (density fluctuations) modulate the induction interaction of the donor-acceptor complex with the solvent. This mechanism of promoting radiation-less electronic transitions is considered here in the framework of the perturbation liquid-state theory. The reorganization energy of electron transfer in nonpolar solvents is nonzero and reaches the values of 0.1–0.3 eV for typical molecular sizes and solvents used in applications. The reorganization energy scales quadratically with the molecular polarizability of the solvent and decays as the inverse fifth power with the size of the donor and acceptor. The combination of the entropic character of the density fluctuations, driven by re-packing of molecular cores, with the short range of induction solute–solvent interactions leads to the violation of the fluctuation–dissipation theorem for the variance of the donor-acceptor energy gap. An explicit, approximately hyperbolic, dependence of the reorganization energy on temperature is predicted. It leads to a non-Arrhenius kinetic law for the rate constant of electron transfer in nonpolar liquid solvents.

14 SOLAR ENERGY↗

DOE OSTI2020

Reply to Robinson and Michaud, arXiv:2002.08893

We respond to Robinson and Michaud's (RM) comment (arXiv:2002.08893) on our recent preprint arXiv:2002.06937, in which we discuss recent excesses in low-threshold dark matter searches, and offer a potential unifying dark matter interpretation. We thank RM for their feedback, which highlights the critical need for future measurements to directly calibrate plasmon charge yields for low $\sim$ 10 eV energy depositions. RM objected to our assertion that plasmons generated at energy scales below 100~eV may have a large branching fraction into phonons. As we argue below, the points raised by RM do not invalidate our primary conclusions, as they pertain to a much different energy scale than we discuss in our paper.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

A Circular Economy for Lithium-Ion Batteries Used in Mobile and Stationary Energy Storage: Drivers, Barriers, Enablers, and U.S. Policy Considerations

As large-format battery energy storage (BES) capacity increases in the United States, so will the volume of spent lithium-ion batteries (LiBs) (Bade 2019). Estimates based on a 10-year lifetime assumption found that the volume of LiBs that have reached the end of their utility for electric vehicle (EV) applications could total two million units (four million metric tons) annually by 2040 in the United States (Richa et al. 2014; Ai and Borucki 2018). Although there is currently no publicly available decommissioning or end-of-life (EoL) projection for stationary BES systems, the U.S. energy storage market is expected to grow from an annual deployment of 523 megawatts in 2013 to 7.3 gigawatts in 2025 (Wood MacKenzie and ESA 2020; Wesoff 2020). Despite potential secondary market opportunities and the potential benefits associated with the reuse/recovery of LiB material, anecdotal evidence suggests that in the United States most decommissioned LiBs from EVs are landfilled or otherwise disposed of (Steward et al. 2019; Salim et al. 2019; CPUC 2019; DTSC 2019d; NREL 2019b; Jacoby 2019; DOE 2019). The reuse of large-format LiBs is not at commercial scale and to date consists of only a handful of U.S.-led pilot projects. Similarly, less than 5% of LiBs from EVs are sent to recycling facilities in the United States (Steward et al. 2019; Jacoby 2019; America Made 2019; Patel 2017). As awareness of current practices grows, and the demand for critical LiB materials increases, U.S. industry stakeholders, regulators, and policymakers are starting to (1) consider solutions to drive and enable environmentally sustainable materials management decisions and behaviors and (2) identify barriers to a circular economy for LiBs (Figure 1). Circular economy principles (Figure 1) attempt to transition from a “take-make-consume-dispose” linear economic system to a circular system that allows for the long life, high performance, and the reuse/recovery of products and materials (Ellen MacArthur Foundation 2016). We begin this report by summarizing drivers, barriers, and enablers to a circular economy for LiBs used in mobile and stationary BES systems in the United States. We then report on our analysis of federal and state regulatory considerations that may impact the reuse/recovery and disposal of LiBs, and potential civil and criminal liabilities associated with noncompliance. We conclude by highlighting state policies and initiatives in the United States that expressly address reuse/recovery and disposal of large-format LiBs. Our results are based on legal and literature-based research and interviews with mobile and stationary BES industry stakeholders, regulators, and policymakers. While this report addresses stationary BES, as well as mobile BES, much of the information and experience with LiB decommissioning and EoL material management is derived from the increasing management of spent EV LiBs in the United States.

25 ENERGY STORAGE↗

DOE OSTI2023

A Robust Parallel Distributed State Estimation for Large Scale Distribution Systems

The growing need and interest in real-time monitoring of large distribution networks motivated by the rapid population of renewable sources, EVs and etc. demand a computationally efficient state estimation framework. Furthermore, this paper presents an improved computational framework for implementing a robust state estimator using a multi-core processor. The main contribution of the paper is the proposed computational framework along with two partitioning strategies which enable fast and robust state estimation for large scale radial and/or meshed distribution systems. Formulation of the proposed method and its implementation are described in detail. Performance of the estimator is tested by simulations first using a small 84-bus radial distribution system. Then the method’s scalability is demonstrated by simulations on two very large scale distribution networks one configured radially and the other meshed each containing over 12,500 buses.

42 ENGINEERING↗

DOE OSTI2023

Dynamic Monkey Bar Mechanism of Superionic Li‐ion Transport in LiTaCl 6

Abstract The LiTaCl 6 solid electrolyte has the lowest activation energy of ionic conduction at ambient conditions (0.165 eV), with a record high ionic conductivity for a ternary compound (11 mS cm −1 ). However, the mechanism has been unclear. We train machine‐learning force fields (MLFF) on ab initio molecular dynamics (AIMD) data on‐the‐fly and perform MLFF MD simulations of AIMD quality up to the nanosecond scale at the experimental temperatures, which allows us to predict accurate activation energy for Li‐ion diffusion (at 0.164 eV). Detailed analyses of trajectories and vibrational density of states show that the large‐amplitude vibrations of Cl − ions in TaCl 6 − enable the fast Li‐ion transport by allowing dynamic breaking and reforming of Li−Cl bonds across the space in between the TaCl 6 − octahedra. We term this process the dynamic‐monkey‐bar mechanism of superionic Li + transport which could aid the development of new solid electrolytes for all‐solid‐state lithium batteries.

Lei, Ming↗

DOE OSTI2024

Finite Bubble Statistics Constrain Late Cosmological Phase Transitions

We consider first order cosmological phase transitions (PTs) happening at late times below standard model temperatures T PT ≲ GeV. The inherently stochastic nature of bubble nucleation and the finite number of bubbles associated with a late-time PT lead to superhorizon fluctuations in the PT completion time. We compute how such fluctuations eventually source curvature fluctuations with universal properties, independent of the microphysics of the PT dynamics. Using cosmic microwave background (CMB) and large scale structure measurements, we constrain the energy released in a dark-sector PT. For 0.1 eV ≲ T PT ≲ keV this constraint is stronger than both the current bound from additional neutrino species Δ⁢N eff , and in some cases, even CMB-S4 projections. Future measurements of CMB spectral distortions and pulsar timing arrays will also provide competitive sensitivity for keV ≲ T PT ≲ GeV.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Collective optical Thomson scattering in pulsed-power driven high energy density physics experiments (invited)

Optical collective Thomson scattering is used to diagnose magnetized high energy density physics experiments at the Magpie pulsed-power generator at Imperial College London. The system uses an amplified pulse from the 2nd harmonic of a Nd:YAG laser (3 J, 8 ns, 532 nm) to probe a wide diversity of hightemperature plasma objects; with densities in the range of 10 17 -10 19 cm -3 and temperatures between 10 eV and a few keV. The scattered light is collected from 100 μm-scale volumes within the plasmas, which are imaged onto optical fiber arrays. Multiple collection systems observe these volumes from different directions, providing simultaneous probing with different scattering K-vectors (and different associated α-parameters, typically in the range 0.5 – 3) allowing independent measurements of separate velocity components of the bulk plasma flow. The fiber arrays are coupled to an imaging spectrometer with a gated ICCD. The spectrometer is configured to view the ion-acoustic waves (IAWs) of the collective Thomson scattered spectrum. Fits to the spectra with the theoretical spectral density function S(K,ω) yield measurements of the local plasma temperatures and velocities. Fitting is constrained by independent measurements of the electron density from laser interferometry, and the corresponding spectra for different scattering vectors. Furthermore, this TS diagnostic has been successfully implemented on a wide range of experiments, revealing temperature and flow velocity transitions across magnetized shocks, inside rotating plasma jets and imploding wire arrays, as well as providing direct measurements of drift velocities inside a magnetic reconnection current sheet.

47 OTHER INSTRUMENTATION↗

NASA NTRSDate not supplied

Advanced Manufacturing of the SLS Block 1B Payload Adapter: Engineering Development Unit

The Payload Adapter (PLA) for the Space Launch System Block 1B configuration (SLS B1B) is a structural frustum that interfaces with the Exploration Upper Stage (EUS) and the Universal Stage Adapter (USA) or the cargo fairing at the aft end and interfaces with the primary or co-manifested payload at the forward end. The primary structure is composed of a single piece aluminum forward ring, a segmented aluminum aft ring, eight carbon composite sandwich panels, and composite bonded longitudinal joints. The PLA is designed and fabricated in-house at MSFC. Development and flight article builds are joint efforts between the Materials & Processes Laboratory (EM), the Spacecraft & Vehicle Systems Department (EV), the Space Systems Department (ES), and the Test Laboratory (ET). The large-scale manufacturing efforts associated with this task include the fabrication of pathfinder panels; the fabrication and assembly of a full-scale Manufacturing Demonstration Article (MDA); the fabrication, assembly, and test of an Engineering Demonstration Unit (EDU); the fabrication, assembly, and test of a qualification Article; and the fabrication, assembly, and proof test of subsequent flight articles. The PLA team recently completed assembly of the EDU. The final assembly included the instillation of the co-manifested secondary payload, NEST, and the instillation and tensioning of the Payload Separation System (PSS). This poster will detail the assembly process which includes: (1) composite panel to ring assembly, (2) adhesive bonding for the longitudinal joints, and (3) instillation of the NEST and PSS. The PLA EDU is prepared to undergo modal and static load testing.

Monique Wallace↗

NASA NTRS2001

The KLEM High-Energy Cosmic Ray Collector for the Nucleon Satellite Mission

The basic objective of the KLEM (Kinematic Lightweight Energy Meter) Project is to directly measure the elemental energy spectra of very high-energy (10(exp 11) - 10(exp 16) eV) cosmic rays by determining the angular distribution of secondaries produced in a target layer. A small-scale version of a KLEM device has been designed for inclusion in the NUCLEON Russian satellite mission. Despite its 3 relatively small size of 36 x 36 x 30 cubic cm, this instrument has an aperture of about 0.12 square m sr and can thus make an important contribution to data concerning the elemental energy spectra of cosmic rays up to 10(exp 15) eV. Details of the experiment and the astrophysical significance of the mission will be presented.

Bashindzhagyan, G.↗

DOE OSTI2024

Technical Impacts of Light-Duty and Heavy-Duty Transportation Electrification on a Coordinated Transmission and Distribution System

In this study, we propose a strategy to model the required spatiotemporal charging demand from light-duty (LD) and medium- and heavy-duty (MHD) electric vehicles (EVs) using actual transportation data by mapping the demand for the required EV charging to a realistic and coordinated distribution and transmission electric grid at the predicted times of the day to study their impact on the power system in a variety of load, weather, and EV penetration scenarios. This work is the first study that includes the actual weather data and transportation data with realistic and coordinated distribution and transmission grid data in a large industry-scale level study. The main goal of this study is to identify possible issues and required upgrades in the electric grid, caused by an increase in EV integration. The transmission case study is a large grid with 6717 buses over a Texas footprint, and the distribution grid is over Houston, a city in Texas, covering over three million customers. The resulting overloads and voltage violations experienced in the system are discussed, and required planning upgrades to avoid these issues are suggested.

AC optimal power flow (AC-OPF)↗

DOE OSTI2023

Dynamic Monkey Bar Mechanism of Superionic Li–ion Transport in LiTaCl 6

Here, the LiTaCl 6 solid electrolyte has the lowest activation energy of ionic conduction at ambient conditions (0.165 eV), with a record high ionic conductivity for a ternary compound (11 mS cm –1 ). However, the mechanism has been unclear. We train machine-learning force fields (MLFF) on ab initio molecular dynamics (AIMD) data on-the-fly and perform MLFF MD simulations of AIMD quality up to the nanosecond scale at the experimental temperatures, which allows us to predict accurate activation energy for Li-ion diffusion (at 0.164 eV). Detailed analyses of trajectories and vibrational density of states show that the large-amplitude vibrations of Cl – ions in TaCl 6 – enable the fast Li-ion transport by allowing dynamic breaking and reforming of Li–Cl bonds across the space in between the TaCl 6 – octahedra. We term this process the dynamic-monkey-bar mechanism of superionic Li + transport which could aid the development of new solid electrolytes for all-solid-state lithium batteries.

25 ENERGY STORAGE↗

DOE OSTI2021

The Impact of Behind-the-Meter Heterogeneous Distributed Energy Resources on Distribution Grids

The increasing integration of distributed energy resources (DERs) on the electric grid brings new challenges and opportunities for utility grid operations. With the rapid deployment of DERs, there is emerging interest in integrating these controllable devices with utility operations at all levels for monitoring and management. To understand the challenges with increasing behind-the-meter (BTM) DERs and to identify the needs in deploying advanced controls, a comprehensive grid impact study is indispensable. This paper presents the analysis which help visualize the DER impact on the grid, identify the challenges and provides an insight into the new distribution management and control needs to enable reliable and resilient grid operations.

behind-the-meter↗

DOE OSTI2026

Accurate energies for ππ* excited states via exchange scaling: the XS-CASSCF method

The state-averaged complete-active space self-consistent field method (SA-CASSCF) is a widely employed electronic structure method used for studying photochemistry and dynamics owing to its ability to provide a reliable description even of complicated cases while still retaining computational efficiency. However, SA-CASSCF suffers from one Achilles heel, related to the description of ionic ππ* excited states, whose energy is often overestimated by 1–2 eV. In light of this challenge, we present the XS-CASSCF method, a new approach based on the idea of exchange scaling (XS) that screens the involved energy terms to improve the excitation energies of singlet ionic ππ* states. First, we illustrate the power of the XS-CASSCF method using hexatriene and para-quinodimethane as examples, showing that it corrects the targeted ionic states while leaving the other states largely unaffected, giving root-mean-square errors (RMSE) below 0.2 eV for the four lowest states in both cases. Subsequently, XS-CASSCF vertical excitation energies are tested against theoretical best estimates for a set of 11 molecules and 56 excited states. XS-CASSCF performs exceptionally well for the ππ* states of hydrocarbons, reducing the RMSE over 21 excitation energies from 0.96 to 0.27 eV. In the challenging subset of molecules with heteroatoms and a larger number of ππ* and nπ* states, we find that improvements can also be obtained, albeit not as pronounced. We conclude with an outlook into more realistic molecular materials focusing on their singlet–triplet (S 1 /T 1 ) gaps, finding that significant improvements can be obtained along the whole range of S 1 /T 1 gaps studied, going from 0.1 eV to more than 1.5 eV. Owing to notable improvements across significant classes of molecules combined with its conceptual simplicity, we believe that XS-CASSCF is a promising addition to the electronic structure toolbox, serving both as a standalone electronic structure method and as a starting point for further correlated treatment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

On the Speed-up of Wave-like Dark Matter Searches with Entangled Qubits

Qubit-based sensing platforms offer promising new directions for wave-like dark matter searches. Recent proposals demonstrate that entangled qubits can achieve quadratic scaling of the signal in the number of qubits. In this work we expand on these proposals to analyze the bandwidth and scan rate performance of entangled qubit protocols across different error regimes. We find that the phase-based readout of entangled protocols preserves the search bandwidth independent of qubit number, in contrast to power-based detection schemes, thereby achieving a genuine scan-rate advantage. We derive coherence time and error rate requirements for qubit systems to realize this advantage. Applying our analysis to dark photon searches, we find that entangled states of approximately 100 qubits can become competitive with benchmark photon-counting cavity experiments for masses $\gtrsim 30{-}40~μ{\rm eV}$, provided sufficiently low error rates are achieved. The advantage increases at higher masses where cavity volume scaling becomes less favorable.

Bodas, Arushi [Fermilab; Chicago U.] (ORCID:000000↗

DOE OSTI2022

A backing detector for order-keV neutrons

In this work, we have designed and tested a large-area (0.15 m 2 ) neutron detector based on neutron capture on 6Li. The neutron detector design has been optimized for the purpose of tagging the scattering angle of keV-scale neutrons. These neutron detectors would be employed to calibrate the low-energy (<100 eV) nuclear recoil in detectors for dark matter and coherent elastic neutrino nucleus scattering (CE$\textit{v}$NS). We describe the design, construction, and characterization of a prototype. The prototype is designed to have a tagging efficiency of ~25% at the relevant $\mathcal{O}$(keV) neutron energies, and with a mean capture time of ~ 17 μs. The prototype was characterized using a 252 Cf neutron source and agreement with the simulation was observed within a few percent level.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Time-dependent density-functional theory study on nonlocal electron stopping for inertial confinement fusion

Understanding laser–target coupling is of the utmost importance for achieving high performance in laser-direct-drive (LDD) inertial confinement fusion (ICF) experiments. Thus, accurate modeling of electron transport and deposition through ICF-relevant materials and conditions is necessary to quantify the total thermal conduction and ablation. The stopping range is a key transport quantity used in thermal conduction models; in this work, we review the overall role that the electron mean free path (MFP) plays in thermal conduction and hydrodynamic simulations. The currently used modified Lee–More model employs various physics approximations. We discuss a recent model that uses time-dependent density functional theory (TD-DFT) to eliminate these approximations in both the calculation of the electron stopping power and corresponding MFP in conduction zone polystyrene (CH) plasma. In general, the TD-DFT calculations showed a larger MFP (lower stopping power) than the standard modified Lee–More model. Using the TD-DFT results, an analytical model for the electron deposition range, λTD−DFT(ρ,T,K), was devised for CH plasmas between ρ=[0.05−1.05] g/cm3, kBT=[100−1000] eV. We implemented this model into LILAC, for simulations of a National Ignition Facility-scale LDD implosion and compared key physics quantities to ones obtained by simulations using the standard model. The implications of the obtained results and the path moving forward to calculate this same quantity in conduction-zone deuterium–tritium plasmas are further discussed, to hopefully close the understanding gap for laser target coupling in LDD-ICF simulations.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Hardware Implementation and Market Impacts of Grid-Supportive Functions in End-Use Loads

Grid-supportive loads (GSLs) are power electronics-based end-use loads that can provide frequency response and other grid services by autonomously adjusting their output power using local grid measurements. This report provides details on GSL hardware design options and their associated costs and benefits for multiple devices, including EV chargers, refrigerators, and heat pumps. We consider mechanisms to incentivize adoption of GSLs at scale and estimate the quantity of frequency response that can be procured with GSLs.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2025

Universal lower bound on the axion decay constant from free streaming effects

We show that enhancement of the axion relic abundance compared to the standard misalignment contribution generically leads to the production of nonzero momentum axion modes, resulting in warm dark matter behavior and enhanced isocurvature perturbations. It leads to universal constraints on the axion parameter space that are independent of detailed model assumptions and cosmological history. For models enhancing relic abundance with gradient axion modes, observations of the Lyman-$α$ forest impose a lower bound on the axion decay constant, $f_a \gtrsim 10^{15} {\rm GeV}\,(10^{-18}{\rm eV}/m_a)$, from the free-streaming effect. For models relying on the delay of coherent axion oscillations, we obtain a slightly weaker bound, $f_a \gtrsim 10^{14} {\rm GeV}\,(10^{-18}{\rm eV}/m_a)$. We make relatively conservative choices to establish these universal bounds but also provide scaling parameters that can be calibrated for stronger constraints in concrete models and updated as observations improve.

Harigaya, Keisuke [Chicago U., EFI; Tokyo U., IPMU↗