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DOE OSTI2023

First-Principles-Based Machine Learning Models for Phase Behavior and Transport Properties of CO 2

In this work, we construct distinct first-principles-based machine-learning models of CO 2 , reproducing the potential energy surface of the PBE-D3, BLYP-D3, SCAN and SCAN-rvv10 approximations of density functional theory. Here we employ the Deep Potential methodology to develop the models and consequently achieve a significant computational efficiency over ab initio molecular dynamics (AIMD) that allows for larger system sizes and time scales to be explored. Although our models are trained only with liquid phase configurations, they are able to simulate a stable interfacial system and predict vapor-liquid equilibrium properties, in good agreement with results from the literature. Because of the computational efficiency of the models, we are also able to obtain transport properties, such as viscosity and diffusion coefficients. We find that the SCAN-based model presents a temperature shift in the position of the critical point, while the SCAN-rvv10-based model shows improvement but still exhibits a temperature shift that remains approximately constant for all properties investigated in this work. We find that the BLYP-D3-based model generally performs better for liquid phase and vapor-liquid equilibrium properties, but the PBE-D3-based model is better suited for predicting transport properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

CHARGED POINT DEFECTS AND DEFECT COMPLEXES IN PHOSPHORENE AND STRUCTURAL PREDICTION OF TAU-11, A DENSITY FUNCTIONAL THEORY APPROACH

With the advent of powerful computers, first principle calculations have become a robust and reliable tool to complement experiments in the study of materials. First principle calculations such as density functional theory can be used to guide experiments to save time and effort when it comes to new and advanced materials discovery. Study of charge defects in materials and crystal structure prediction are such areas in which density functional theory calculations facilitate the prediction of defect formation energy, charge transition levels and elemental site occupations. Experimentally, studying charge defects requires inferring results from various techniques. Likewise, determining site occupancies for similar elements using experimental techniques is challenging and sometimes impossible. In this work, we study the charged intrinsic and extrinsic defects and defect complexes in phosphorene and determine the site occupancies of Al, Fe and Si in the τ11 phase using density functional theory. In the defect work, we calculate the defect formation energy, charge transition level, binding energies and Stokes shift for vacancy, dopant substitution and dopant-vacancy defect complexes in phosphorene. We found that vacancy defect in phosphorene becomes negatively charged in n-type doping and may passivate the dopants and reduce carrier concentration and mobility. For non-metal dopants in phosphorene, we predict that O, S and Si prefer to form dopant-vacancy complexes removing the vacancy defect states from the band gap. Mn dopant-vacancy defect complex exhibits possibility of switching between two magnetic spin states. Lastly, using density functional theory, we complement the results from neutron powder diffraction to determine the site occupancies of Al and Si in τ11 phase which was used to determine the alloying element to develop a high temperature and low density alloy.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Smaller than Expected Bright-spot Offsets in Spitzer Phase Curves of the Hot Jupiter Qatar-1b

We present Spitzer full-orbit thermal phase curves of the hot Jupiter Qatar-1b, a planet with the same equilibrium temperature—and intermediate surface gravity and orbital period—as the well-studied planets HD 209458b and WASP-43b. We measure secondary eclipse depths of 0.21 ± 0.02% at 3.6 μm and 0.30 ± 0.02% at 4.5 μm, corresponding to dayside brightness temperatures of 1542{sub −31}{sup +32} K and 1557{sub −36}{sup +35} K, respectively, consistent with a vertically isothermal dayside. The respective nightside brightness temperatures are 1117{sub −71}{sup +76} and 1167{sub −74}{sup +69} K, in line with a trend that hot Jupiters all have similar nightside temperatures. We infer a Bond albedo of 0.12{sub −0.16}{sup +0.14} and a moderate day–night heat recirculation efficiency, similar to HD 209458b. General circulation models for HD 209458b and WASP-43b predict that their bright spots should be shifted east of the substellar point by tens of degrees, and these predictions were previously confirmed with Spitzer full-orbit phase curve observations. The phase curves of Qatar-1b are likewise expected to exhibit eastward offsets. Instead, the observed phase curves are consistent with no offset: 11° ± 7° at 3.6 μm and −4° ± 7° at 4.5 μm. The discrepancy in circulation patterns between these three otherwise similar planets points to the importance of secondary parameters like rotation rate and surface gravity, and the presence or absence of clouds, in determining atmospheric conditions on hot Jupiters.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Spin-strain interactions under hydrostatic pressure in α-RuCl 3

We investigate the effects of hydrostatic pressure on 𝛼−RuCl 3 , a prototypical material for the Kitaev spin model on a honeycomb lattice with a possible spin-liquid ground state. Using ultrasound measurements at pressures up to 1.16 GPa, we reveal significant modifications of the acoustic properties and the 𝐻−𝑇 phase diagram of this material. Hydrostatic pressure suppresses the three-dimensional magnetic order and induces a dimerization transition at higher pressures. At low pressures, the sound attenuation exhibits a linear temperature dependence, while above 0.28 GPa, it becomes nearly temperature independent, suggesting a shift in the phonon scattering regime dominated by Majorana fermions. These findings provide new insights into spin-strain interactions in Kitaev magnets and deliver a detailed characterization of the 𝐻−𝑇 phase diagram of 𝛼−RuCl 3 under hydrostatic pressure.

Focused ion beam↗

DOE OSTI2023

Quantification of Energy Savings and Demand Reduction for a Heat Pump Integrated with Thermal Energy Storage (Final Report)

To mitigate the variation in demand on the electric grid, thermal energy storage (TES) is an alternative to electric batteries or installing new peaking power plants. Stakeholders and policy makers across the United States have expressed interests in promoting TES, as demonstrated by the US Department of Energy’s Grid-Interactive Efficient Buildings program and the efforts of various state legislatures. However, the cost value provided by TES are unclear. If reliable cost benefits were determined, stakeholders would have a clearer picture of the financial returns that can be gained from their investment in TES. The study in this report is conducted by ORNL with collaboration with Emerson the Helix Innovation Center. In the first part of this report, EnergyPlus was used to perform whole-building simulations for two residential buildings in Indianapolis and Atlanta. The HVAC system in both buildings were equipped with phase change material TES. The TES tank was charged in off-peak hours and discharged in peak hours to perform load shifting. First, the economic value implied by existing time-of-use (TOU) rates offered by utility companies was analyzed via whole-building simulation. Second, existing demand reduction (DR) incentives sourced from 3 different electrical grid administrators (i.e., California, Texas, and New England region) were surveyed to determine their implied value. The study suggests that the traditional value analysis that focuses on ROI for the building owner significantly undervalues TES technology making economic viability difficult. A more comprehensive value analysis that includes peak demand management and deferred capital for peaking power plants shows that TES should be economically viable but here the value is greater for the utility and requires large market penetration and aggregation to fully realize the benefits. Therefore, to facilitate commercialization, new business models are needed that include a broader range of stakeholders and distribute the value of TES proportionally. In the 2 nd part of this project, the benefits of a novel phase change material (PCM) integrated heat pump configuration were evaluated via detailed component based simulation. A one-dimensional PCM heat exchanger model which discretizes the PCM tank and refrigerant tubes into small control volumes is developed. Each control volume can have different PCM temperatures, PCM properties, and heat transfer coefficients. The PCM tank is charged by a wrapped tank condenser and discharged by an internal refrigerant coil. The PCM heat exchanger model is integrated into DOE/ORNL Heat Pump Design Model for heat pump system simulation. To demonstrate the performance of the PCM integrated heat pump, a case study in Chicago was performed. A Time-of-Use utility structure-based control strategy is implemented to schedule the PCM tank charging and discharging mode switching. Compared with a conventional electric heat pump, the PCM integrated heat pump shows superior performance on load shifting and utility cost reduction. As a result, the proposed system demonstrates 24.6% utility saving for cooling application and 25.8% utility saving for heating application.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2020

Experimental Analysis of Salt Hydrate Latent Heat Thermal Energy Storage System With Porous Aluminum Fabric and Salt Hydrate as Phase Change Material With Enhanced Stability and Supercooling

Phase change materials (PCMs), especially salt hydrates possess high volumetric energy storage capacity in their transition temperature range. These materials are used in applications where it is necessary to store thermal energy due to temporary load shift between demand and availability. Thus, possible applications are HVAC, recovery of waste heat, and defense thermal management. Despite salt hydrates potential, the practical feasibility of latent heat storage with salt hydrates is limited due to low power rating, supercooling, phase segregation, and long-term stability. Its low power rating and long-term stability limits its application in most applications. This work experimentally validates the stability and thermal performance of a compact heat exchanger charged with salt hydrate during melting and freezing. The compact heat exchanger was designed with fins on both the heat transfer fluid (HTF) and salt hydrate PCM side. The thermal performance of the latent heat thermal energy storage system (LHTESS) was evaluated for various operating conditions. The results show that LHTESS could achieve an average heat transfer coefficient of 124 and 87 W/(m2 K) during melting and solidification, respectively. The stability of the system in suppressing supercooling was validated over 800 cycles with nucleating agent and active homogenous nucleation techniques. The supercooling was reduced to 3 °C with zinc hydroxyl nitrate as nucleating agent and less than 1 °C with the active homogenous nucleation technique. The LHTESS showed less than 6% degradation in energy storage capacity over 800 cycles.

42 ENGINEERING↗

DOE OSTI2020

Evaluation of the Quasi‐Biennial Oscillation in global climate models for the SPARC QBO‐initiative

Abstract Quasi‐biennial oscillations (QBOs) in thirteen atmospheric general circulation models forced with both observed and annually repeating sea surface temperatures (SSTs) are evaluated. In most models the QBO period is close to, but shorter than, the observed period of 28 months. Amplitudes are within ±20 % of the observed QBO amplitude at 10 hPa, but typically about half of that observed at lower altitudes (50 and 70 hPa). For almost all models, the oscillation's amplitude profile shows an overall upward shift compared to reanalysis and its meridional extent is too narrow. Asymmetry in the duration of eastward and westward phases is reasonably well captured, though not all models replicate the observed slowing of the descending westward shear. Westward phases are generally too weak, and most models have an eastward time mean wind bias throughout the depth of the QBO. The intercycle period variability is realistic and in some models is enhanced in the experiment with observed SSTs compared to the experiment with repeated annual cycle SSTs. Mean periods are also sensitive to this difference between SSTs, but only when parametrized non‐orographic gravity wave (NOGW) sources are coupled to tropospheric parameters and not prescribed with a fixed value. Overall, however, modelled QBOs are very similar whether or not the prescribed SSTs vary interannually. A portrait of the overall ensemble performance is provided by a normalized grading of QBO metrics. To simulate a QBO, all but one model used parametrized NOGWs, which provided the majority of the total wave forcing at altitudes above 70 hPa in most models. Hence the representation of NOGWs either explicitly or through parametrization is still a major uncertainty underlying QBO simulation in these present‐day experiments.

Bushell, A. C.↗

DOE OSTI2023

Dynamics of oil–water interface at the beginning of the ultrasonic emulsification process

A lot of effort has been dedicated in recent years towards understanding the basics of cavitation induced emulsification, mainly in the form of single cavitation bubbles. Regarding bulk acoustic emulsification, a lot less research has been done. In our here presented work we utilize advanced high-speed observation techniques in visible light and X-Rays to build upon that knowledge and advance the understanding of bulk emulsion preparation. During research we discovered that emulsion formation has an acute impact on the behavior of the interface and more importantly on its position relative to the horn, hence their interdependence must be carefully studied. We did this by observing bulk emulsification with 2 cameras simultaneously and corroborating these measurements with observation under X-Rays. Since the ultrasonic horns location also influences interface behavior, we shifted its initial position to different locations nearer to and further away from the oil–water interface in both phases. We found that a few millimeters distance between the horn and interface is not enough for fine emulsion formation, but that they must be completely adjacent to each other, with the horn being located inside the oil–water interface. We also observed some previously undiscovered phenomena, such as the splitting of the interface to preserve continuous emulsion formation, climbing of the interface up the horn and circular interface protrusions towards the horn forming vertical emulsion streams. Interestingly, no visible W/O emulsion was ever formed during our experiments, only O/W regardless of initial horn position.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Reactive Separations of CO/CO 2 mixtures over Ru–Co Single Atom Alloys

Reactive separations of CO/CO 2 mixtures are a promising pathway to lower the energy requirement of CO 2 hydrogenation to chemicals and fuels, with applications in the U.S. Navy’s seawater-to-fuel process. With the CO/CO 2 feedstock, a challenge is activating CO to produce heavier hydrocarbons while preventing CO 2 methanation, requiring low-temperature Fischer-Tropsch synthesis (FTS) catalysts. In this work, we demonstrate that a Ru–Co single atom alloy (SAA) catalyst produces C 5+ hydrocarbons at a rate of 11.7 μmol/s/g-cobalt (hexane basis) in a 50/50 CO/CO 2 stream with ≤1% CO 2 conversion. The reaction operates at a relatively low temperature (200 °C) and high gas hourly space velocity (GHSV: 84,000 mL/g/h) that is compatible with the upstream reverse water-gas shift reaction. Detailed experiments, catalyst characterizations, and density functional theory (DFT) calculations have been conducted to understand the active phase, the role of the Ru dopant, and catalyst restructuring that occurs at elevated temperatures (>200 °C). Ru dopants are found to promote the reduction of Co species, enabling catalytic activity for CO hydrogenation without pre-reduction, but may not enhance the FTS activity or desired C 5+ hydrocarbon selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Femtosecond exciton dynamics in WSe 2 optical waveguides

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe 2 , prompted by femtosecond light pulses. Using time-resolved scanning near-field optical microscopy we visualize the electric field profiles of waveguide modes in real space and time and extract the temporal evolution of the optical constants following femtosecond photoexcitation. By monitoring the phase velocity of the waveguide modes, we detect incoherent A-exciton bleaching along with a coherent optical Stark shift in WSe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Detection efficiency measurement and operational tests of the X-Arapuca for the first module of DUNE far detector

The Deep Underground Neutrino Experiment (DUNE) is a dual-site experiment for long-baseline neutrino oscillation studies, able to resolve the neutrino mass hierarchy and measure δ$_{CP}$. DUNE will also have sensitivity to supernova neutrinos and to processes beyond the Standard Model, such as nucleon decay searches. The Far Detector (FD) will consist of four liquid argon TPC (17.5 kt total mass) with systems for the detection of charge and scintillation light produced by an ionization event. The charge detection system permits both calorimetry and position determination. In addition, the photon-detection system (PDS) enhances the detector capabilities for all DUNE physics drivers. The PDS of the first FD module consists of light collector modules placed in the inactive space between the innermost wire planes of the TPC anode. The light collectors, the so-called X-ARAPUCAS, are functionally a light trap that captures wavelength-shifted photons inside boxes with highly reflective internal surfaces where they are guided to Silicon Photo-multipliers (SiPM) by wavelength-shifting (WLS) bars. Functionality and operational tests of the X-ARAPUCAS to be installed in ProtoDUNE-SP phase II (FD DUNE prototype at the scale 1:20), as well as the measurement of their absolute detection efficiency is reported in this publication.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

Direct observation of ion micromotion in a linear Paul trap

In this paper, the first direct observation of micromotion for multiple ions in a laser-cooled trapped ion crystal is discussed along with a novel measurement technique for micromotion amplitude. Micromotion is directly observed using a time-resolving, single-photon sensitive camera that provides both fluorescence and position data for each ion on the nanosecond time scale. Micromotion amplitude and phase for each ion in the crystal is measured which allows this method to be sensitive to tilts and shifts of the ion chain from the null of the radiofrequency quadrupole potential in the linear trap. Spatial resolution makes this micromotion detection technique suitable for complex ion configurations, including two-dimensional geometries. It does not require any additional equipment or laser beams, and the modulation of the cooling lasers or trap voltages is not necessary for detection, as it is in other methods.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Atomic-Scale Imaging of Polarization Switching in an (Anti-)Ferroelectric Memory Material: Zirconia (ZrO2)

Direct, atomic-scale visualization of polarization switching in a functional, polycrystalline, binary oxide via in-situ high-resolution transmission electron microscopy (HRTEM) biasing is reported for the first time. Antiferroelectric (AFE) ZrO2 was used as the model system, which is important for commercial DRAMs and as emerging NVMs (through work-function engineering). We observed (1) clear shifting and coalescing of domains within a single grain, and (2) dramatic changes of the atomic arrangements and crystalline phases—both at voltages above the critical voltage measured for AFE switching. Similar synergistic in-situ structural-electrical characterization can pave the way to understand and engineer microscopic mechanisms for retention, fatigue, variability, sub-coercive switching and analog states in ferroelectric and AFE-based memory devices.

Lombardo, Sarah↗

DOE OSTI2024

Space charge dominated momentum spread and compensation strategies in the post-linac section of Proton Improvement Plan-II at Fermilab

The upcoming Proton Improvement Plan-II (PIP-II), designated for enhancements to the Fermilab accelerator complex, features a new 800 MeV superconducting linac and a Beam Transfer Line (BTL) to transport the beam to the existing Booster synchrotron. To mitigate the space charge tune shift associated with a high intensity accumulated beam, the low emittance linac beam is used to paint the ring phase space both transversely and longitudinally. To prevent losses caused by particles injected outside the rf separatrix while painting longitudinal phase space, the momentum spread of the incoming beam should not exceed 2.1 x 10^-4. Detailed simulations showed that due to space charge, the rms momentum spread increases to 4 x 10^-4 while it is transported in the BTL --about twice the allowable limit. In this paper, we outline a mitigation strategy involving a debuncher cavity. We discuss location, operating frequency, and gap voltage under both nominal and perturbed beam conditions, specifically accounting for momentum jitter. The impact of cavity misalignments is also assessed. The paper concludes by recommending an optimized configuration.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Recharge Demand Mitigation for Latent Heat Thermal Energy Storage at Off-peak Hours

The utilization of integrated heat pump thermal energy storage (HP-TES) systems for space conditioning applications can reduce electrical power demand and achieve utility savings resulting from peak shaving and load shifting. However, issues arise when the energy required to recharge the TES exceeds the shifted energy demand, especially in extreme climates where high-temperature lifts between the outdoor air conditions and phase-change materials (PCMs) during recharging may occur. In this work, a single room-temperature (22°C) PCM-TES is integrated into a single-speed heat pump system using a secondary hydronic loop where the TES is recharged using the outdoor unit during off-peak hours. Three recharge strategies were investigated as potential pathways to reduce recharging power demand: (i) considering different heat source/sink temperatures, (ii) using a variable-speed compressor, and (iii) using a variable-speed pump. Simulations were conducted using Modelica for HP-TES recharging at different heat source/sink temperatures from -30 – 20℃ in heating mode and 0 – 30℃ in cooling mode. Results show that the most effective recharge demand reduction strategy is an HP-TES system using a single-speed compressor with a variable-speed pump for the hydronic loop run at preferable heat source/sink temperatures when the temperature lifts were reduced. Utilizing a variable-speed compressor for the HP-TES system reduced recharge time in extreme cases at the cost of additional compressor power input. The findings motivate potential control strategies that minimize recharge energy and maximize peak energy savings, hence reducing overall operating costs and annual energy consumption for HP-TES systems for space conditioning applications.

25 ENERGY STORAGE↗

DOE OSTI2023

Evolution of the Internal Climate Modes under Future Warming

Abstract Climate modes play an important role in weather and climate variability over multiple spatial and temporal scales. This research assesses Earth system model (ESM) projections of the spatiotemporal characteristics of key internal climate modes (NAM, SAM, PNA, ENSO, PDO, and AMO) under high (SSP585) and low (SSP126) radiative forcing scenarios and contextualizes those projections using historical fidelity. Time series analyses are used to assess trends and mode phase characteristics are summarized for the historical period and for the end of the twenty-first century. Spatial patterns are compared to infer morphological changes. Shifts in the power spectra are used to examine changes in variability at subannual, interannual, and interdecadal scales. Changes in time-lagged correlations are used to capture the evolution of first-order interactions. While differences in historical skill are predominantly ESM dependent, changing mode characteristics in a warmer climate also exhibit variability between individual ensemble realizations. NAM, SAM, and ENSO tend to evolve toward increased prevalence of the positive phase up to 2100 across the multimodel ensemble while the PNA and PDO exhibit little trend but increasing phase intensity. AMO characteristics are shown to depend on the method used to remove the external signal. ESMs that show higher historical fidelity tend to show more modest changes in those modes under global nonstationarity. Changes in mode interactions are found to be highly ESM dependent but exhibit broadly similar behavior to historical relationships. These findings have implications for our understanding of internal variability and make clear that the choice of ESM, and even the ESM realization, matters for applications of climate projections. Significance Statement Internal modes of variability are important to understand due to their impact on local, regional, and global weather and climate patterns. Future climate changes will not only be affected by the variability arising from these modes, but the modes will themselves change in response to the changing climate. Spatial and temporal aspects of the modes are assessed from projections of future climate and related to how well they are captured in the historical climate. This yields some measure of confidence in the changes exhibited by the models. In most cases, when historically skillful models exhibit changes that are different from those produced by less skillful models, they tend to produce more modest changes. These results, as well as the variability between model outcomes, mean decisions on which ESM to use for projections of the future climate matter significantly.

Meteorology & Atmospheric Sciences↗

DOE OSTI2025

Krylov complexity in mixed phase space

We investigate the Krylov complexity of thermofield double states in systems with mixed phase space, uncovering a direct correlation with the Brody distribution, which interpolates between Poisson and Wigner statistics. Our analysis spans two-dimensional random matrix models featuring (I) GOE-Poisson and (II) GUE-Poisson transitions and extends to higher-dimensional cases, including a stringy matrix model (GOE-Poisson) and the mass-deformed SYK model (GUE-Poisson). Krylov complexity consistently emerges as a reliable marker of quantum chaos, displaying a characteristic peak in the chaotic regime that gradually diminishes as the Brody parameter approaches zero, signaling a shift toward integrability. These results establish Krylov complexity as a powerful diagnostic of quantum chaos and highlight its interplay with eigenvalue statistics in mixed phase systems.

chaos & nonlinear dynamics↗

DOE OSTI2020

A conservative phase-space moving-grid strategy for a 1D-2V Vlasov–Fokker–Planck Solver

In this work, we develop a conservative configuration- and velocity-space (i.e., phase-space) moving-grid strategy for the Vlasov–Fokker–Planck (VFP) equation in a planar geometry. The velocity-space grid is normalized and shifted in terms of the thermal speed and the bulk-fluid velocity, respectively. The configuration-space grid is moved according to a mesh-motion-partial-differential equation (MMPDE), which equidistributes a monitor function that is inversely proportional to the gradient-length scales of the macroscopic plasma quantities. The resulting inertial terms in the transformed VFP equations are discretized to ensure the discrete conservation of mass, momentum, and energy. To satisfy the discrete conservation theorems in the presence of phase-space mesh motion, we employ the method of discrete nonlinear constraints – explored in previous studies – but the underlying symmetries are determined in a much more efficient manner than before. The conservative grid-adaptivity strategy provides an efficient scheme that resolves important physical structures in the phase-space while controlling the computational complexity at all times. We demonstrate the favorable features of the proposed algorithm through a set of test cases of increasing complexity. The problems test independent components of the algorithms, as well as the integrated capability on settings relevant to inertial confinement fusion.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗