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DOE OSTI2018

Quantum Efficiency of Charge Transfer Competing against Nonexponential Processes: The Case of Electron Transfer from CdS Nanorods to Hydrogenase

Photoexcited charge transfer from semiconductor nanocrystals to charge acceptors is a key step for photon energy conversion in semiconductor nanocrystal-based light-harvesting systems. Charge transfer competes against relaxation processes within the nanocrystals, and this competition determines the quantum efficiency of charge transfer. The quantum efficiency is a critical design element in photochemistry, but in nanocrystal-acceptor systems its extraction from experimental data is complicated by sample heterogeneity and intrinsically nonexponential excited-state decay pathways. In this manuscript, we systematically explore these complexities using TA spectroscopy over a broad range of timescales to probe electron transfer from CdS nanorods to the redox enzyme hydrogenase. To analyze the experimental data, we build a model that quantifies the quantum efficiency of charge transfer in the presence of competing, potentially nonexponential, relaxation processes. Our approach can be applied to calculate the efficiency of charge or energy transfer in any donor-acceptor system that exhibits nonexponential donor decay and any ensemble distribution in the number of acceptors, provided that donor relaxation and charge transfer can be described as independent, parallel decay pathways. We apply this analysis to our experimental system and unveil the connections between particle morphology and quantum efficiency. Our model predicts a finite quantum efficiency even when the mean recombination time diverges, as it does in CdS nanostructures with spatially separated electron-hole pairs that recombine with power-law dynamics. We contrast our approach to the widely used expressions for the quantum efficiency based on average lifetimes, which for our system overestimate the quantum efficiency. Furthermore, the approach developed here is straightforward to implement and should be applicable to a wide range of systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

Dynamic Processes of CO 2 Storage in the Field: 1. Multiscale and Multipath Channeling of CO 2 Flow in the Hierarchical Fluvial Reservoir at Cranfield, Mississippi

A consistent picture of dynamic channeling, invasion, spreading, and breakthrough (CISB) of supercritical CO 2 in the hierarchical fluvial reservoir at Cranfield, Mississippi is presented after 10 years of integration and analysis of complementary field monitoring and characterization data. The dynamic CISB with small-scale CO 2 -flow channels in the F1-F2-F3 cross section (F1, F2, and F3 are one injection and two monitoring wells) was imaged by daily electrical resistance tomography (ERT) and time-lapse crosswell seismic surveys. One, three, and four CO 2 flow channels logged at F1, F2, and F3, respectively, were dynamically connected with strong temporal variations in CO 2 saturation during 221 days of drainage with injection rate doubling twice and 81 days of imbibition. Three intermediate-scale CO 2 flow channels (with highest CO 2 saturation) normal to the cross section were ERT-imaged during late-time drainage. A large-scale, sinuous fluvial CO 2 flow channel was imaged by repeat surface seismic survey at the end of the imbibition. The fluvial sandstone channel sinuously bypasses the F1-F2-F3 cross section in a point bar, but the channel is connected to the cross section through an intermediate-scale sandstone channel, forming a complicated flow channel network. The multiscale flow channel network (in the fluvial channel-point bar system) revealed from the observed CISB enables us to consistently interpret the hydrological monitoring data of three tracer tests, each conducted during an injection rate step, and preinjection hydraulic-thermal-tracer tests. Finally, this interpretation of the CISB and flow channel network can guide future modeling and data inversion to best understand the effects of natural heterogeneity on CO 2 storage efficiency and residual trapping.

58 GEOSCIENCES↗

DOE OSTI2021

Spin-glass dynamics in the presence of a magnetic field: exploration of microscopic properties

The synergy between experiment, theory, and simulations enables a microscopic analysis of spin-glass dynamics in a magnetic field in the vicinity of and below the spin-glass transition temperature T g . The spin-glass correlation length, ξ(t, t w ; T), is analysed both in experiments and in simulations in terms of the waiting time t w after the spin glass has been cooled down to a stabilised measuring temperature T < T g and of the time t after the magnetic field is changed. This correlation length is extracted experimentally for a CuMn 6 at. % single crystal, as well as for simulations on the Janus II special-purpose supercomputer, the latter with time and length scales comparable to experiment. The non-linear magnetic susceptibility is reported from experiment and simulations, using ξ(t, t w ; T) as the scaling variable. Previous experiments are reanalysed, and disagreements about the nature of the Zeeman energy are resolved. The growth of the spin-glass magnetisation in zero-field magnetisation experiments, M ZFC (t, t w ; T), is measured from simulations, verifying the scaling relationships in the dynamical or non-equilibrium regime. Lastly, our preliminary search for the de Almeida–Thouless line in D = 3 is discussed.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Agentic artificial intelligence for multistage physics experiments at a large-scale user facility particle accelerator

We present a language-model-driven agentic artificial intelligence (AI) system to autonomously execute multistage physics experiments on a production synchrotron light source. Implemented at the Advanced Light Source particle accelerator, the system translates natural language user prompts into structured execution plans that combine archive data retrieval, control-system channel resolution, automated script generation, controlled machine interaction, and analysis. In a representative machine physics task, we show that preparation time was reduced by 2 orders of magnitude relative to manual scripting even for a system expert, while operator-standard safety constraints were strictly upheld. Core architectural features, plan-first orchestration, bounded tool access, and dynamic capability selection, enable transparent, auditable execution with fully reproducible artifacts. These results establish a blueprint for the safe integration of agentic AI into accelerator experiments and demanding machine physics studies, as well as routine operations, with direct portability across accelerators worldwide and, more broadly, to other large-scale scientific infrastructures.

Accelerator/storage ring control systems↗

DOE OSTI2015

Relativistic Coulomb excitation within the time dependent superfluid local density approximation

Within the framework of the unrestricted time-dependent density functional theory, we present for the first time an analysis of the relativistic Coulomb excitation of the heavy deformed open shell nucleus 238 U. The approach is based on the superfluid local density approximation formulated on a spatial lattice that can take into account coupling to the continuum, enabling self-consistent studies of superfluid dynamics of any nuclear shape. We compute the energy deposited in the target nucleus as a function of the impact parameter, finding it to be significantly larger than the estimate using the Goldhaber-Teller model. The isovector giant dipole resonance, the dipole pygmy resonance, and giant quadrupole modes are excited during the process. As a result, the one-body dissipation of collective dipole modes is shown to lead a damping width Γ↓≈0.4 MeV and the number of preequilibrium neutrons emitted has been quantified.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Antibody dynamics to SARS‐CoV‐2 in asymptomatic COVID‐19 infections

Abstract Background The missing asymptomatic COVID‐19 infections have been overlooked because of the imperfect sensitivity of the nucleic acid testing (NAT). Globally understanding the humoral immunity in asymptomatic carriers will provide scientific knowledge for developing serological tests, improving early identification, and implementing more rational control strategies against the pandemic. Measure Utilizing both NAT and commercial kits for serum IgM and IgG antibodies, we extensively screened 11 766 epidemiologically suspected individuals on enrollment and 63 asymptomatic individuals were detected and recruited. Sixty‐three healthy individuals and 51 mild patients without any preexisting conditions were set as controls. Serum IgM and IgG profiles were further probed using a SARS‐CoV‐2 proteome microarray, and neutralizing antibody was detected by a pseudotyped virus neutralization assay system. The dynamics of antibodies were analyzed with exposure time or symptoms onset. Results A combination test of NAT and serological testing for IgM antibody discovered 55.5% of the total of 63 asymptomatic infections, which significantly raises the detection sensitivity when compared with the NAT alone (19%). Serum proteome microarray analysis demonstrated that asymptomatics mainly produced IgM and IgG antibodies against S1 and N proteins out of 20 proteins of SARS‐CoV‐2. Different from strong and persistent N‐specific antibodies, S1‐specific IgM responses, which evolved in asymptomatic individuals as early as the seventh day after exposure, peaked on days from 17 days to 25 days, and then disappeared in two months, might be used as an early diagnostic biomarker. 11.8% (6/51) mild patients and 38.1% (24/63) asymptomatic individuals did not produce neutralizing antibody. In particular, neutralizing antibody in asymptomatics gradually vanished in two months. Conclusion Our findings might have important implications for the definition of asymptomatic COVID‐19 infections, diagnosis, serological survey, public health, and immunization strategies.

Lei, Qing↗

DOE OSTI2015

Noise analysis for near field 3-D FM-CW radar imaging systems

Near field radar imaging systems are used for several applications including concealed weapon detection in airports and other high-security venues. Despite the near-field operation, phase noise and thermal noise can limit the performance in several ways including reduction in system sensitivity and reduction of image dynamic range. In this paper, the effects of thermal noise, phase noise, and processing gain are analyzed in the context of a near field 3-D FM-CW imaging radar as might be used for concealed weapon detection. In addition to traditional frequency domain analysis, a time-domain simulation is employed to graphically demonstrate the effect of these noise sources on a fast-chirping FM-CW system.

microwave imaging↗

DOE OSTI2019

Two temperature regimes of triplet transfer in the dissociation of the correlated triplet pair after singlet fission

The ability to undergo spin-allowed exciton multiplication makes singlet fission materials promising for photovoltaic applications. Here, we examine the separation of correlated triplet pairs, 1 (T…T), in polycrystalline pentacene films via temperature-dependent transient absorption spectroscopy. Single wavelength analysis reveals a profound delay in 1 (T…T) dynamics. Moreover, the dynamics of 1 (T…T) exhibit temperature dependence, whereas other features show no discernable temperature dependence. Previous literatures have suggested that correlated triplet separation is mediated by a thermally activated hopping process. Surprisingly, we found that the time constants governing triplet pair separation display two distinct temperature-dependent regimes of triplet transport. The high temperature regime follows a thermally activated hopping mechanism. The experimentally derived reorganization energy and electronic coupling is verified by density matrix renormalization group quantum chemical calculations. In addition, we evaluated the low temperature regime and show that the trend can be modelled by a Miller–Abrahams-type model that incorporates the effects of energetic disorder. We conclude that the correlated triplet pair separation is mediated by thermally activated hopping or a disorder driven Miller–Abrahams-type mechanism at high and low temperature, respectively. We observe that crossover between two regimes occurs ~226 K. We find the time constant for triplet–triplet energy transfer to be 1.8 ps at ambient temperature and 21 ps at 77 K.

Chemistry↗

DOE OSTI2023

Modes and Mechanisms of Pacific Decadal-Scale Variability

The modes of Pacific decadal-scale variability (PDV), traditionally defined as statistical patterns of variance, reflect to first order the ocean's integration (i.e., reddening) of atmospheric forcing that arises from both a shift and a change in strength of the climatological (time-mean) atmospheric circulation. While these patterns concisely describe PDV, they do not distinguish among the key dynamical processes driving the evolution of PDV anomalies, including atmospheric and ocean teleconnections and coupled feedbacks with similar spatial structures that operate on different timescales. In this review, we synthesize past analysis using an empirical dynamical model constructed from monthly ocean surface anomalies drawn from several reanalysis products, showing that the PDV modes of variance result from two fundamental low-frequency dynamical eigenmodes: the North Pacific–central Pacific (NP-CP) and Kuroshio–Oyashio Extension (KOE) modes. Both eigenmodes highlight how two-way tropical–extratropical teleconnection dynamics are the primary mechanisms energizing and synchronizing the basin-scale footprint of PDV. While the NP-CP mode captures interannual- to decadal-scale variability, the KOE mode is linked to the basin-scale expression of PDV on decadal to multidecadal timescales, including contributions from the South Pacific.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Cloud Radiative Feedbacks and El Niño–Southern Oscillation

Cloud radiative feedbacks are disabled via “cloud-locking” in the Community Earth System Model, version 1.2 (CESM1.2), to result in a shift in El Niño–Southern Oscillation (ENSO) periodicity from 2–7 years to decadal time scales. We hypothesize that cloud radiative feedbacks may impact the periodicity in three ways: by 1) modulating heat flux locally into the equatorial Pacific subsurface through negative shortwave cloud feedback on sea surface temperature anomalies (SSTA), 2) damping the persistence of subtropical southeast Pacific SSTA such that the South Pacific meridional mode impacts the duration of ENSO events, or 3) controlling the meridional width of off-equatorial westerly winds, which impacts the periodicity of ENSO by initiating longer Rossby waves. The result of cloud-locking in CESM1.2 contrasts that of another study, which found that cloud-locking in a different global climate model led to decreased ENSO magnitude across all time scales due to a lack of positive longwave feedback on the anomalous Walker circulation. CESM1.2 contains this positive longwave feedback on the anomalous Walker circulation, but either its influence on the surface is decoupled from ocean dynamics or the feedback is only active on interannual time scales. The roles of cloud radiative feedbacks in ENSO in other global climate models are additionally considered. In particular, it is shown that one cannot predict the role of cloud radiative feedbacks in ENSO through a multimodel diagnostic analysis. Instead, they must be directly altered.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Photo-Switching of Protein Dynamical Collectivity

We examine changes in the picosecond structural dynamics with irreversible photobleaching of red fluorescent proteins (RFP) mCherry, mOrange2 and TagRFP-T. Measurements of the protein dynamical transition using terahertz time-domain spectroscopy show in all cases an increase in the turn-on temperature in the bleached state. The result is surprising given that there is little change in the protein surface, and thus, the solvent dynamics held responsible for the transition should not change. A spectral analysis of the measurements guided by quasiharmonic calculations of the protein absorbance reveals that indeed the solvent dynamical turn-on temperature is independent of the thermal stability/photostate however the protein dynamical turn-on temperature shifts to higher temperatures. This is the first demonstration of switching the protein dynamical turn-on temperature with protein functional state. The observed shift in protein dynamical turn-on temperature relative to the solvent indicates an increase in the required mobile waters necessary for the protein picosecond motions, that is, these motions are more collective. Melting-point measurements reveal that the photobleached state is more thermally stable, and structural analysis of related RFP’s shows that there is an increase in internal water channels as well as a more uniform atomic root mean squared displacement. These observations are consistent with previous suggestions that water channels form with extended light excitation providing O2 access to the chromophore and subsequent fluorescence loss. We report that these same channels increase internal coupling enhancing thermal stability and collectivity of the picosecond protein motions. The terahertz spectroscopic characterization of the protein and solvent dynamical onsets can be applied generally to measure changes in collectivity of protein motions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Revisiting the Architecture of the KOI-89 System

While high stellar obliquities observed in exoplanetary systems may be attributed to processes that tilt the planetary orbits, it is also possible that they reflect misalignments between protoplanetary disks and stellar spins. This latter hypothesis predicts the presence of coplanar multiplanetary systems misaligned with their central stars. Here we reevaluate the evidence of such an architecture that has been claimed for the KOI-89 system. An early-type star, KOI-89 has one validated transiting planet, KOI-89.01/Kepler-462b (period 84.7 days, radius 3.0 R {sub ⊕}), and one transiting planet candidate, KOI-89.02 (period 207.6 days, radius 4.0 R {sub ⊕}), where the latter exhibits transit timing variations (TTVs). A previous modeling of the stellar gravity-darkening effect in the transit light curves inferred a high stellar obliquity of ≈70°. We perform photodynamical modeling of the Kepler transit light curves and use the resulting constraints on the orbital configuration and transit times to update the gravity-darkened transit model. As a result, we find no firm evidence for the gravity-darkening effect in the transit shapes and conclude that stellar obliquity is not constrained by the data. Given the evidence for low orbital eccentricities from the dynamical analysis, the system architecture can thus be consistent with many other multitransiting systems with flat, near-circular orbits aligned with the stellar spin. We find that the TTVs imparted on its neighbor imply that KOI-89.01 has a mass ≳20 M {sub ⊕}. This would render it one of the densest known sub-Neptunes, mostly composed of a solid core. Lower masses are possible if the TTVs are instead due to an unseen third planet.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Model-Agnostic Algorithm for Real-Time Attack Identification in Power Grid using Koopman Modes

Malicious activities on measurements from sensors like Phasor Measurement Units (PMUs) can mislead the control center operator into taking wrong control actions resulting in disruption of operation, financial losses, and equipment damage. In particular, false data attacks initiated during power systems transients caused due to abrupt changes in load and generation can fool the conventional model-based detection methods relying on thresholds comparison to trigger an anomaly. In this paper, we propose a Koopman mode decomposition (KMD) based algorithm to detect and identify false data attacks in real-time. The Koopman modes (KMs) are capable of capturing the nonlinear modes of oscillation in the transient dynamics of the power networks and reveal the spatial embedding of both natural and anomalous modes of oscillations in the sensor measurements. The Koopman-based spatio-temporal nonlinear modal analysis is used to filter out the false data injected by an attacker. The performance of the algorithm is illustrated on the IEEE 68-bus test system using synthetic attack scenarios generated on GridSTAGE, a recently developed multivariate spatio-temporal data generation framework for simulation of adversarial scenarios in cyber-physical power systems.

Nandanoori, Sai Pushpak↗

DOE OSTI2020

Dynamic domain kinematic modelling for predicting interflow over leaky impeding layers

Traditional Boussinesq or kinematic simulations of interflow (i.e., lateral subsurface flow) assume no leakage through the impeding layer and require a no-flow boundary condition at the ridge top. However, recent analyses of many interflow-producing landscapes indicate that leaky impeding layers are common, that most interflow percolates well before reaching the toe slope, and therefore, the downslope contributing length is shorter than the hillslope length. In watersheds characterised by perched interflow over a low conductivity layer through permeable topsoil, interflow with percolation may be modelled with a kinematic wave model using a mobile upslope boundary condition defining the hillslope portion contributing interflow to valleys. Here, we developed and applied a dynamic interflow model to simulate interflow using a downslope travel distance concept such that only the active contributing length is modelled at any time. The model defines a variable active area based on the depth of the perched layer, the topographic slope and the ratio of the hydraulic conductivity of topsoil to that of the impeding layer. It incorporates a two-layer soil moisture accounting water balance analysis, a pedo-transfer function, and percolation and evaporation routines to predict interflow rates in continuous and event-based scenarios. We tested the modelling concept on two sets of data (2-year dataset of rainfall observations for the continuous simulation and a multi-day irrigation experiment for the event simulation) from a 121-m-long open interflow collection trench on an experimental hillslope at the Savannah River Site, South Carolina. The continuous model simulation partially represented the observed interflow hydrograph and perched water depth in the experimental hillslope with correlation coefficients of 0.85 and 0.35, respectively. Model performance improved significantly at event-scale analysis. The modelling approach realistically represents interflow dynamics in hillslopes with leaky impeding layers and can be integrated into catchment-scale hydrology models for more detailed hillslope process modelling.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Investigation of the Use of Dynamic Probabilistic Risk Assessment Methodologies for Identifying Digital I&C System Common Cause Failures

Digital Instrumentation and Control (I&C) systems have a key role in nuclear power plants in the upgrade of aging analog systems. Digital systems improve plant safety and reliability through features such as increased hardware reliability and stability and improved failure detection capability. There is no consensus on which of the current probabilistic risk assessment methods are most suitable for use in the reliability analysis of digital I&C systems. While the traditional event-tree/fault-tree (ET/FT) approach is still used for their reliability modeling, there are concerns regarding this approach in properly accounting for dynamic interactions among system components since potentially significant dependencies among failure events may not be identified and/or their likelihood may not be properly quantified. Dynamic methodologies are expected to provide a much more accurate representation of probabilistic evolution of the I&C systems in time due to their capability to more properly account for complex interactions than the static approach. The applicability of dynamic PRA methodologies for digital I&C system is investigated using the criteria presented in the NUREG/CR-6901, and the comparisons made in NUREG/CR-6901 are updated in light of the latest studies. The Dynamic Event Tree (DET) approach has been identified as one of the top dynamic methods when evaluated against the requirements for the reliability modeling of digital I&C systems. The DET method is a strong candidate for integration into existing PRA studies, as it bears many similarities to the traditional ET approach. In this study, the DET approach has been applied to the Plant Protection System of the APR1400 design, and the results are compared to results from its available traditional ET/FT analysis. Possible approaches to evaluate and quantify the effects of common cause failures on system safety using dynamic methods are also examined.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2017

Destruction dynamics of a heterogeneous body (diorite) under friction

Triboluminescence bursts are observed in two heterogeneous (diorite) specimens under friction against each other. Triboluminescence appears upon the relaxation of excited free ≡Si–O{sup –} radicals and Fe{sup 3+} ions and the capture of electrons with acceptor traps formed upon the destruction of the plagioclase crystal lattice. The analysis of the time dependence of these bursts shows that the friction surfaces accumulate clusters, in which the concentration of free ≡Si–O{sup –} radicals and electron traps is at least an order of magnitude higher than in their surrounding. The time interval between the appearance of two sequential clusters variates from 0.1 to 1 μs. The linear sizes of clusters are ~0.5 μm.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Multi-scale, Multi-disciplinary, and Multi-agent Explainable AI with Koopman-Undergirded Learning, Prediction, and Analysis (M3EA KULPA) (Project Closeout Report)

The goal of this project was to develop and use domain-aware machine learning formulations, based on the Koopman Operator (KO), for modelling multi-scale, multi-disciplinary (e.g., multi-physics), and/or multi-agent systems. The project developed these formulations for the following cases: • Systems with dynamics at two separate time scales, • Systems with a bi-level hierarchical control structure, • Systems with bi-level hierarchical control and dynamics at two separate time scales (the lower level controls operating at the faster time scale), and • Systems with n separate but interacting agents/disciplines (with/without control, respectively); the controls for each agent could include bi-level hierarchical control and dynamics at two separate time scales as described above. The project then defined a set of dynamical systems consisting of different nonlinear oscillators that could be used to test these different formulations and then subsequently learned the KO models for those systems. With the KO models, we were able to do the following: • Quantify system stability, including both long-term and transient behavior, • Quantify the effects of feedbacks between the different time scales and agents/disciplines in terms of those feedbacks’ effects on system stability, • Replace a standard Proportional-Integral (PI) control in the hierarchical control structure with a KO-based Linear-Quadratic Regular (LQR), a form of optimal control, • Calculate optimal supervisory control policies a) with and without time scale separated dynamics at the lower level control levels and b) with both PI and KO-based LQR lower level control policies, and • Calculate dynamic Nash equilibria for multi-agent systems where each agent makes its own control decisions.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2026

Rewarding Grid-Friendly Behavior: Estimating the Potential Bill Reduction and Load Shifting Benefits of Dynamic Prices

Shifting electric load from times of peak demand can be a key strategy to slow price growth as reducing peak demand avoids the cost of upgrading generation, transmission and distribution infrastructure. Utilities are releasing time-varying prices, such as time of use rates or dynamic prices, to incentivize grid-friendly load shifting. New dynamic price programs provide insight into the true cost of operating electricity grids and the potential economic benefits of load shifting. Program developers and device manufacturers need to understand the economic opportunities in terms of 1) the variation in prices across hours, days, and seasons; 2) the change in utility bills for customers who don’t shift load; and 3) the potential load shifted and economic value of different technologies if manufacturers or aggregators deploy price-responsive controls. This paper estimates possible impacts of dynamic price adoption and load shifting controls if customers paid the dynamic rate from one pilot program. Statistical analysis of historical prices identified annual and seasonal metrics as well as representative price curves for each circuit in the pilot. Simulations for residential technologies with price-responsive controls including unitary heat pump water heaters, central multifamily heat pump water heaters, heating & cooling + storage systems, and pool pumps estimated the potential impacts of highly dynamic prices both with and without load shifting controls. Results showed the potential to reduce electricity costs on representative days by 42-94% and reduce consumption during times of high electricity prices by 63-100% compared to baseline operation for those flex-friendly devices.

Grant, Peter↗