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DOE OSTI2021

An Ab Initio Multiple Cloning Method for Non-Adiabatic Excited-State Molecular Dynamics in NWChem

The recently developed ab-initio multiple cloning (AIMC) approach based on the multicongurational Ehrenfest (MCE) method provides a powerful and accurate way of describing the excited-state dynamics of molecular systems. The AIMC method is a controlled approximation to non-adiabatic dynamics with a particular strength in the proper description of decoherence effects due to branching of vibrational wavepackets at a level crossing. In this work, we report a new implementation of the AIMC algorithm in the open source NWChem computational chemistry program. The framework combines linear-response time-dependent density functional theory with Ehrenfest mean-eld theory to determine the equations of motion for classical trajectories. The multi-dimensional wave function is decomposed into a superposition of Gaussian coherent states guided by Ehrenfest trajectories (i.e., MCE approach), which can clone with fully quantum mechanical amplitudes and phases. By using an efficient time-derivative based non-adiabatic coupling approach within the AIMC method, all observable are calculated on-the-y in the non-adiabatic molecular dynamics process. As a representative example, we apply our implementation to study the ultrafast photoinduced electronic and vibrational energy transfer in a pyridine molecule. The effects of the cloning procedure on electronic and vibrational coherence, relaxation and unidirectional energy transfer are discussed. This new AIMC implementation provides a high-level non-adiabatic molecular dynamics framework for simulating photoexcited dynamics in complex molecular systems and experimentally relevant ultrafast spectroscopic probes, such as nonlinear coherent optical and X-ray signals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Group-velocity-dispersion engineering of tantala integrated photonics

Designing integrated photonics, especially to leverage Kerr-nonlinear optics, requires accurate and precise knowledge of the refractive index across the visible to infrared spectral ranges. Tantala ( T a 2 O 5 ) is an emerging material platform for integrated photonics and nanophotonics that offers broadband ultralow loss, moderately high nonlinearity, and advantages for scalable and heterogeneous integration. We present refractive index measurements on a thin film of tantala, and we explore the efficacy of this data for group-velocity-dispersion (GVD) engineering with waveguide and ring-resonator devices. In particular, the observed spectral extent of supercontinuum generation in fabricated waveguides and the wavelength dependence of free spectral range (FSR) in optical resonators provide a sensitive test of our integrated photonics design process. Our work opens up new design possibilities with tantala, including with octave-spanning soliton microcombs.

Black, Jennifer A.↗

DOE OSTI2020

Impact of Drying on Meso- and Nanoscale Structures of Citrus Fiber: A Study by SFG, ATR-IR, XRD, and DLS

Citrus fibers are a sidestream of the pectin extraction process from citrus peel. This sidestream can be converted into a functional ingredient through a shear-induced homogenization process. One technical challenge with this material is that dehydration and subsequent rehydration result in reduction of viscosity compared to the original product. In this study, various drying methods were compared with never-dried fibers to investigate the structural changes underlying the viscosity loss. Infrared and X-ray diffraction analyses confirmed no changes in chemical composition and crystalline structure of citrus fibers. Here, the dynamic light scattering and sum frequency generation analyses of citrus fiber suspension showed that the rehydration process could not fully disperse aggregated fibers, which appears to be the main cause for the viscosity loss.

09 BIOMASS FUELS↗

DOE OSTI2025

Applying deep learning methods to develop new models of molecular charge transfer, nonadiabatic dynamics, and nonlinear spectroscopy in the condensed phase

Photon- and field-induced charge transfer has central importance in the generation and storage of electricity, the novel properties of materials, photo-induced catalysis, and electro-optic activity (e.g., photovoltaic cells, fuel cells, and organic chromophores for use in optical fibers and light-emission diodes). These non-equilibrium electronic and chemical transformations are probed by ultrafast, nonlinear spectroscopies. Accurate simulations play a crucial role in our ability to understand, optimize, and control these transformations. This project applies modern deep learning and machine learning (ML) methods to dramatically improve models of electronic dynamics, electronic-nuclear dynamics, and spectroscopic measurements for improved simulations of chemistry in complex environments, far from equilibrium phenomena, and processes in extreme environments, such as materials exposed to strong or resonant fields. This project develops accurate neural net models that go beyond predictive capability to also provide new insight into the fundamental physics underlying electron and nuclear dynamics. To achieve its objectives, this project explores and develops customized versions of high-capacity deep learning algorithms/models. These techniques are developed with an emphasis on fundamental chemical insight, not just predictive accuracy, to assist the development of the next generation of quantum simulation methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Optically induced umklapp shift currents in striped cuprates

Motivated by recent experiments that observed low-frequency second-order optical responses in doped striped superconductors, here we investigate the nonlinear electrodynamics of systems exhibiting a charge density wave (CDW) order parameter. Due to the Bragg scattering off the CDW order, an incoming spatially homogeneous electric field in addition to zero momentum current generates umklapp currents that are modulated in space at momenta of the reciprocal CDW lattice. In particular, here we predict and microscopically evaluate the umklapp shift current, a finite momentum analog of the regular shift current which represents the second-order optical process that downconverts homogeneous AC electric field into low-frequency, zero momentum current. Specifically, we evaluate real-time response functions within mean-field theory via the Keldysh technique and use the Peierls substitution to compute observables at finite momenta in lattice models. We find that systems with certain lattice symmetries (such as inversion symmetry), where the regular shift current is disallowed, may give rise to the umklapp one. We apply our framework to investigate lattice symmetries in layered materials with helical-like stripes and show that both types of shift currents provide insight into the nature of intertwined phases of matter. Finally, we discuss the relation of our findings to recent experiments in striped superconductors. Published by the American Physical Society 2024

Materials Science↗

DOE OSTI2024

Guided Mode Evolution and Ionization Injection in Meter-Scale Multi-GeV Laser Wakefield Accelerators

Here, we show that multi-GeV laser wakefield electron accelerators in meter-scale, low density hydrodynamic plasma waveguides operate in a new nonlinear propagation regime dominated by sustained beating of lowest order modes of the ponderomotively modified channel; this occurs whether or not the injected pulse is linearly matched to the guide. For a continuously doped gas jet, this emergent mode beating effect leads to axially modulated enhancement of ionization injection and a multi-GeV energy spectrum of multiple quasimonoenergetic peaks; the same process in a locally doped jet produces single multi-GeV peaks with <10% energy spread. A three-stage model of drive laser pulse evolution and ionization injection characterizes the beating effect and explains our experimental results.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

Determination of the nonlinear thermo-optic coefficient of silicon nitride and oxide using an effective index method

There is little literature characterizing the temperature-dependent thermo-optic coefficient (TOC) for low pressure chemical vapor deposition (LPCVD) silicon nitride or plasma enhanced chemical vapor deposition (PECVD) silicon dioxide at temperatures above 300 K. In this study, we characterize these material TOC’s from approximately 300-460 K, yielding values of (2.51 ± 0.08) · 10 −5 K −1 for silicon nitride and (5.67 ± 0.53) · 10 −6 K −1 for silicon oxide at room temperature (300 K). We use a simplified experimental setup and apply an analytical technique to account for thermal expansion during the extraction process. We also show that the waveguide geometry and method used to determine the resonant wavelength have a substantial impact on the precision of our results, a fact which can be used to improve the precision of numerous ring resonator index sensing experiments.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Soliton formation and topology manipulation of coupled spins via ultrafast re-magnetization

The major goal of the project was to explore the properties of magnetic order driven far out of equilibrium by optical excitations. These include fundamental questions related to the interplay of magnetic, structural and electronic degrees of freedom in materials that are optically excited. These problems break down in short term quenching of the magnetization as a results of the energy of the optical pulse studying how the energy of the optical pulse and the angular momentum of the magnetization flow between the different degrees of freedom. This is followed by the longer time re-emergence of the magnetism as the system cools. Within this goal we explored the formation of solitons, both with and without non-trivial topology, via rapid re-magnetization processes after optical-driven ultrafast demagnetization. Guided by theory, we predict that turbulence and modulational instabilities will drive the formation of solitons, including dispersive shock waves, magnon droplets, and skyrmions. In the case of topological defect formation, i.e. skyrmion generation, related processes have long been predicted based on general principles of symmetry-breaking phase transitions; the density of topological defects in a long-range-ordered phase can be controlled by varying the quench rate through the second-order phase transition, i.e. the Kibble-Zurek (KZ) mechanism. We, more broadly, had the goal to study a range of other emergent magnetic behaviors after optical excitation. While great attention has been given to ultrafast demagnetization, less is known of the subsequent spin dynamics and coupling to the lattice. What is increasingly appreciated is that ultrafast demagnetization leads to spin currents that can carry angular momentum from the rapidly demagnetized sample. These spin currents appear in many ways but fundamentally controls demagnetization, drives interactions between regions of the material, and control the spin resulting structure. They can be probed many ways including THz emission which, in turn, gives insight into the demagnetization processes. Simultaneously if there is magneto-elastic coupling ultrafast demagnetization can drive structural excitations that are not expected from thermal energy added to the lattice. We explored a range of complex phenomena that arise from photo-excitation of magnetic systems with the coupling of electronic, magnetic and structural degrees of freedom. We have made a number of fundamental discoveries that are reflected in our publications list with additional work still being prepared for publication. Highlights of this work include (i) ultra-efficient, nonlinear THz surface acoustics (ii) spin-current-mediated rapid magnon localization and coalescence, (iii) spin-wave soliton formation in ferromagnetic FePt nanoparticles, (iv) dynamic phonon coupling in elemental antiferromagnetic Cr, (v) THz emission from Co/Pt bilayers and FeRh/Pt bilayers, (vi) theoretical investigation of spin hydrodynamics, solitons and shock waves, and (vii) ultrafast perturbation of magnetic domains by optical pumping.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Enhancing the Range and Reliability of the Spacer Layer Imaging Method

The spacer layer imaging method (SLIM) is widely used to measure the thickness of additive and lubricant films, in lubricant development and evaluation, and for fundamental research into elastohydrodynamic lubrication and tribofilm formation mechanisms. The film thickness measurement, as implemented on several popular tribometers, provides powerful, non-destructive in-situ mapping of film topography with nanometre-scale height sensitivity. However, the results can be highly sensitive to experimental procedure, machine condition, and image analysis, in some cases reporting unphysical film thickness trends. The prevailing image analysis techniques make it challenging to interrogate these errors, often hiding their multivariate nonlinear behaviour from the user by spatial averaging. Herein, several common ‘silent errors’ in the SLIM measurement, including colour matching to incorrect fringe orders, and colour drift due to the optical properties of the system or film itself, are discussed, with examples. A robust suite of novel a priori and a posteriori methods to address these issues, and to improve the accuracy and reliability of the measurement, are also presented, including a novel, computationally inexpensive circle-finding algorithm for automated image processing. In combination, these methods allow reliable mapping of films up to at least 800 nm in thickness, representing a significant milestone for the utility of SLIM applied to elastohydrodynamic contact.

EHL film geometry↗

DOE OSTI2025

Femtojoule optical nonlinearity for deep learning with incoherent illumination

Optical neural networks (ONNs) are a promising computational alternative for deep learning due to their inherent massive parallelism for linear operations. However, the development of energy-efficient and highly parallel optical nonlinearities, a critical component in ONNs, remains an outstanding challenge. Here, we introduce a nonlinear optical microdevice array (NOMA) compatible with incoherent illumination by integrating the liquid crystal cell with silicon photodiodes at the single-pixel level. We fabricate NOMA with more than half a million pixels, each functioning as an optical analog of the rectified linear unit at ultralow switching energy down to 100 femtojoules per pixel. With NOMA, we demonstrate an optical multilayer neural network. Our work holds promise for large-scale and low-power deep ONNs, computer vision, and real-time optical image processing.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Remote quantification of Cm(III) and HNO 3 by fluorescence spectroscopy and chemometrics

A unique approach to remotely quantify Cm(III) (0–100 µg mL −1 ) in HNO 3 (1–12 M) using steady-state laser fluorescence spectroscopy and multivariate regression models was developed. Photoluminescence is amenable to remote measurements using fiber-optic cables and is sensitive to numerous lanthanide and actinide species. In-line measurements can provide feedback to support complex processing in harsh environments (e.g., hot cells) to help guide and optimize radiochemical separations. In this work, Cm(III) spectra were acquired remotely in a glove box as a function of HNO 3 concentration to better understand spectral characteristics and evaluate the utility of multivariate regression models in this system. Furthermore, the Cm(III) fluorescence peak shape, width, position, and intensity changed significantly as a function of HNO 3 concentration, likely because of the displacement of emission quenching inner-sphere water molecules and complexation with nitrate ions. Despite significant covariance and nonlinearity in the data, a D-optimal design strategy successfully minimized training set sample size and was used to build effective partial least squares regression models for Cm(III) and HNO 3 concentrations without a priori knowledge of solution conditions. Chemometrics for modeling complex fluorescence spectra are promising and may find widespread applicability for online analysis in numerous chemical systems found in the nuclear field.

Actinide↗

DOE OSTI2024

Enhanced beam-beam modeling to include longitudinal variation during weak-strong simulation

Beam-beam interactions pose substantial challenges in the design and operation of circular colliders, significantly affecting their performance. In particular, the weak-strong simulation approach is pivotal for investigating single-particle dynamics during the collider design phase. This paper evaluates the limitations of existing models in weak-strong simulations, noting that while they accurately account for energy changes due to slingshot effects, they fail to incorporate longitudinal coordinate changes ( z variation). To address this gap, we introduce two novel transformations that enhance Hirata’s original framework by including both z variation and slingshot effect-induced energy changes. Through rigorous mathematical analysis and extensive weak-strong simulation studies, we validate the efficacy of these enhancements in achieving a more precise simulation of beam-beam interactions. Our results reveal that although z variation constitutes a higher-order effect and does not substantially affect the emittance growth rate within the specific design parameters of the Electron-Ion Collider, the refined model offers improved accuracy, particularly in scenarios involving the interaction between beam-beam effects and other random diffusion processes, as well as in simulations incorporating realistic lattice models. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Real-Time GPU-Accelerated OFDR With an Integrated Auxiliary Interferometer

A GPU-accelerated optical frequency domain reflectometry (OFDR) system with an improved integrated auxiliary interferometer is proposed. Unlike conventional approaches that require separate auxiliary interferometers and multiple detection channels, the proposed OFDR system embeds this functionality directly into the signal via an intentional beat component. This enables self-calibration of laser nonlinearity while maintaining a cost-effective hardware configuration. Building on this simplified configuration, the system leverages GPU acceleration with an NVIDIA RTX 4070 Ti to achieve real-time performance, delivering high-throughput signal processing for continuous OFDR interrogation. The signal processing pipeline comprises signal capture, resampling for nonlinearity compensation, and frequency shift computation, all optimized for parallel execution. Hardware benchmarking demonstrates substantial acceleration over CPU implementations, achieving up to a 45× speedup for resampling and frequency shift computations and enabling processing latencies below 30 ms. Thermal response validation is conducted under two complementary scenarios: localized heating using a water bath and cryogenic-temperature conditions using liquid nitrogen. Under localized heating, the system achieves an accuracy of 0.249 °C with a thermal sensitivity of 5.971 GHz/°C, while cryogenic-temperature validation demonstrates a frequency shift response with a sensitivity of 2.383 GHz/°C and an accuracy of 2.04 °C. The high acceleration of the proposed GPU-accelerated OFDR system and its accuracy are achieved by exploiting CUDA-based stride indexing, enabling efficient parallel segmentation and processing of large datasets without additional memory copies. The benchmarking results confirm the robustness, accuracy, and deployability of the proposed OFDR system across a wide temperature range, establishing it as a practical platform for real-time distributed fiber sensing in structurally dynamic environments.

Harb, Salah [Lawrence Berkeley National Laboratory↗

DOE OSTI2025

Shock-induced bubble jets: a dual perspective of bubble collapse and interfacial instability theory

Interactions between shock waves and gas bubbles in a liquid can lead to bubble collapse and high-speed liquid jet formation, relevant to biomedical applications such as shock wave lithotripsy and targeted drug delivery. This study reveals a complex interplay between acceleration-induced instabilities that drive jet formation and radial accelerations causing overall bubble collapse under shock wave pressure. Using high-speed synchrotron X-ray phase contrast imaging, the dynamics of micrometre-sized air bubbles interacting with laser-induced underwater shock waves are visualised. These images offer full optical access to phase discontinuities along the X-ray path, including jet formation, its propagation inside the bubble, and penetration through the distal side. Jet formation from laser-induced shock waves is suggested to be an acceleration-driven process. A model predicting jet speed based on the perturbation growth rate of a single-mode Richtmyer–Meshkov instability shows good agreement with experimental data, despite uncertainties in the jet-driving mechanisms. The jet initially follows a linear growth phase, transitioning into a nonlinear regime as it evolves. To capture this transition, a heuristic model bridging the linear and nonlinear growth phases is introduced, also approximating jet shape as a single-mode instability, again matching experimental observations. Upon piercing the distal bubble surface, jets can entrain gas and form a toroidal secondary bubble. Linear scaling laws are identified for the pinch-off time and volume of the ejected bubble relative to the jet’s Weber number, characterising the balance of inertia and surface tension. At low speeds, jets destabilise due to capillary effects, resulting in ligament pinch-off.

Drops and Bubbles: Bubble dynamics↗

DOE OSTI2023

Ultrafast nonequilibrium dynamics and high-harmonic generation in two-dimensional quantum spin Hall materials

For this work, we develop the theoretical framework of nonequilibrium ultrafast photonics in monolayer quantum spin Hall insulators supporting a multitude of topological states. In these materials, ubiquitous strong light-matter interactions in the femtosecond scale lead to nonadiabatic quantum dynamics, resulting in topology-dependent nonlinear optoelectronic transport phenomena. We investigate the mechanism driving topological Dirac fermions interacting with strong ultrashort light pulses and uncover various experimentally accessible physical quantities that encode fingerprints of the quantum material's topological electronic state from the high-harmonic generated spectrum. Our work sets the theoretical cornerstones to realize the full potential of time-resolved harmonic spectroscopy for understanding nonequilibrium processes in quantum topological systems and identifying topological invariants in two-dimensional quantum spin Hall solid state systems.

2-dimensional systems↗

DOE OSTI2023

Quantum interferometry and pathway selectivity in the nonlinear response of photosynthetic excitons

We propose a time–frequency resolved spectroscopic technique which employs nonlinear interferometers to study exciton–exciton scattering in molecular aggregates. A higher degree of control over the contributing Liouville pathways is obtained as compared to classical light. We show how the nonlinear response can be isolated from the orders-of-magnitude stronger linear background by either phase matching or polarization filtering. Both arise due to averaging the signal over a large number of noninteracting, randomly oriented molecules. We apply our technique to the Frenkel exciton model which excludes charge separation for the photosystem II reaction center. We show how the sum of the entangled photon frequencies can be used to select two-exciton resonances, while their delay times reveal the single-exciton levels involved in the optical process.

Science & Technology - Other Topics↗

DOE OSTI2026

Bound Exciton Complexes in Near-Infrared Emitting Quantum Shells

Near-infrared (NIR) light sources based on colloidal semiconductor nanocrystals (NCs) represent a scalable, low-cost alternative to epitaxial semiconductor platforms. However, their performance remains hindered by rapid Auger recombination, a problem that is particularly pronounced in narrow-bandgap materials. Here, we report on CdS/HgS/CdS and CdS/HgCdSe/ ZnS quantum shells (QSs), a class of spherical quantum wells specifically engineered for a suppression of nonradiative Auger processes. Fabricated QSs exhibit tunable NIR emission with photoluminescence quantum yields reaching ∼60% below 1000 nm and up to 30% near 1300 nm. Optical gain and stimulated emission were observed in CdS/HgS/CdS QSs. In contrast, CdS/HgCdSe/ZnS QSs displayed a photoinduced absorption in lieu of optical gain despite demonstrating a comparatively stronger Auger suppression. Transient absorption spectroscopy revealed that this phenomenon arises from the formation of bound multiexciton complexes that induce long-lived sub-bandgap multiexciton states. The observation of such bound excitonic clusters at room temperature offers a pathway toward nonlinear NIR photonic phenomena, including biexciton−exciton cascade emission, optical modulation, and singleexciton gain.

Auger recombination↗

DOE OSTI2020

Machine-Learning Enabled Evaluation of Probability of Piping Degradation In Secondary Systems of Nuclear Power Plants

The transition to condition-based, risk-informed automated maintenance will contribute to a significant reduction of operations and maintenance costs that account for the majority of nuclear power generation costs. Furthermore, of the operations and maintenance costs in U.S. plants, approximately 80% are labor costs. To address the issue of rising operating costs and economic viability, technologies used to perform online monitoring of piping and other secondary system structural components in commercial nuclear power plants (NPPs) are under evaluation. These online monitoring systems have the potential to identify when a more detailed inspection is needed using real time measurements, rather than at a pre-determined inspection interval thus reducing the maintenance cost. This paper describes distributed high-temperature stable fiber sensors fabricated in optical fibers through a roll-to-roll laser direct writing process using femtosecond lasers. Using phase-sensitive optical time domain reflectometry, distributed acoustic and vibration sensors can be developed and deployed to critical components and systems in NPPs to perform active measurements with spatial resolution down to 0.5-meter throughout the piping systems. Complex acoustic and vibration signatures harnessed by distributed sensors are registered and analyzed by artificial intelligence algorithms for degradation detection and flaw identification. Piping elbows with machined-in flaws were instrumented with fiber sensors. High-spatial-resolution data were used to develop and validate machine learning algorithms, including both linear and nonlinear regression, and classification. Additionally, classification and sensor analysis were also performed for data analysis. The paper concludes with recommendations and future work on applications of machine learning enabled high-resolution fiber sensors for piping degradation monitoring in current or future NPPs.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗