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At least 127 records · Page 7

Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations

Nano-size confinement induces many intriguing non-Fourier heat conduction phenomena, such as nonlinear temperature gradients, temperature jumps near the contacts, and size-dependent thermal conductivity. Over the past decades, these effects have been studied and interpreted by nonequilibrium molecular dynamics (NEMD) and phonon Boltzmann transport equation (BTE) simulations separately, but no theory that unifies these two methods has ever been established. In this work, we unify these methods using a quantitative mode-level comparison and demonstrate that they are equivalent for various thermostats. We show that different thermostats result in different non-Fourier thermal transport characteristics due to the different mode-level phonon excitations inside the thermostats, which explains the different size-dependent thermal conductivities calculated using different reservoirs, even though they give the same bulk thermal conductivity. Specifically, the Langevin thermostat behaves like a thermalizing boundary in phonon BTE and provides mode-level thermal-equilibrium phonon outlets, while the Nose-Hoover chain thermostat and velocity rescaling method behave like biased reservoirs, which provide a spatially uniform heat generation and mode-level nonequilibrium phonon outlets. These findings explain why different experimental measurement methods can yield different size-dependent thermal conductivity. They also indicate that the thermal conductivity of materials can be tuned for various applications by specifically designing thermostats. Finally, the unification of NEMD and phonon BTE will largely facilitate the study of thermal transport in complex systems in the future by, e.g., replacing computationally unaffordable first-principles NEMD simulations with computationally less expensive spectral BTE simulations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Opportunities for gas-phase science at short-wavelength free-electron lasers with undulator-based polarization control

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range of photon energies. Their revolutionary and innovative developments have opened new fields of science regarding nonlinear light-matter interaction, the investigation of ultrafast processes from specific observer sites, and approaches to imaging matter with atomic resolution. A core aspect of FEL science is the study of isolated and prototypical systems in the gas phase with the possibility of addressing well-defined electronic transitions or particular atomic sites in molecules. Notably for polarization-controlled short-wavelength FELs, the gas phase offers new avenues for investigations of nonlinear and ultrafast phenomena in spin-orientated systems, for decoding the function of the chiral building blocks of life as well as steering reactions and particle emission dynamics in otherwise inaccessible ways. This roadmap comprises descriptions of technological capabilities of facilities worldwide, innovative diagnostics and instrumentation, as well as recent scientific highlights, novel methodology, and mathematical modeling. The experimental and theoretical landscape of using polarization controllable FELs for dichroic light-matter interaction in the gas phase will be discussed and comprehensively outlined to stimulate and strengthen global collaborative efforts of all disciplines. Published by the American Physical Society 2025

Ilchen, Markus↗

Potential quantum advantage for simulation of fluid dynamics

Numerical simulation of turbulent fluid dynamics needs to either parametrize turbulence—which introduces large uncertainties—or explicitly resolve the smallest scales—which is prohibitively expensive. Here, we provide evidence through analytic bounds and numerical studies that a potential quantum speedup can be achieved to simulate fluid dynamics using quantum computing. Specifically, we provide a lattice Boltzmann formulation of fluid dynamics for which we give evidence that low-order Carleman linearization is much more accurate than previously believed for these systems. This is achieved via a combination of reformulating the Navier-Stokes nonlinearity (u·$\triangledown$u) to lattice-Boltzmann nonlinearity (u 2 ) and accurately linearizing the dynamical equations, which effectively trades nonlinearity for additional degrees of freedom that add negligible expense in the quantum solver. Based on this, we apply a quantum algorithm for simulating the Carleman-linearized lattice Boltzmann equation and provide evidence that its cost scales logarithmically with system size compared with polynomial scaling in the best known classical algorithms. In this paper, we suggest that a quantum advantage may exist for simulating fluid dynamics, paving the way for simulating nonlinear multiscale transport phenomena in a wide range of disciplines using quantum computing.

42 ENGINEERING↗

LOKI

LOKI is a simulation code that models weakly-coupled plasma evolution using Eulerian kinetic models in four phase space dimensions. The code is useful to understand basic plasma nonlinear plasma physics phenomena - in particular, wave-particle and wave-wave resonances that occur in laser plasma interactions. LOKI can simulate fundamental physical process in low-density plasmas on a scale of hundreds of light wavelengths. It does so by solving the relativistic Vlasov and Valsov-Fokker-Planck differential transport equations describing the collision less and low-collisionality evolution of charged particles in electromagnetic fields in two configuration space and two velocity space dimensions. Two principle electromagnetic models are provided: electrostatic (Poisson's Equation) and electromagnetic (Maxwell's equations).

DIMITS, ANDRIS↗

Bayesian optimization of Fisher Information in nonlinear multiresonant quantum photonics gyroscopes

Abstract We propose an on-chip gyroscope based on nonlinear multiresonant optics in a thin film χ (2) resonator that combines high sensitivity, compact form factor, and low power consumption simultaneously. We theoretically analyze a novel holistic metric – Fisher Information capacity of a multiresonant nonlinear photonic cavity – to fully characterize the sensitivity of our gyroscope under fundamental quantum noise conditions. Leveraging Bayesian optimization techniques, we directly maximize the nonlinear multiresonant Fisher Information. Our holistic optimization approach orchestrates a harmonious convergence of multiple physical phenomena – including noise squeezing, nonlinear wave mixing, nonlinear critical coupling, and noninertial signals – all encapsulated within a single sensor-resonator, thereby significantly augmenting sensitivity. We show that ∼ 470 × $\sim 470{\times}$ improvement is possible over the shot-noise limited linear gyroscope with the same footprint, intrinsic quality factors, and power budget.

42 ENGINEERING↗

A reactive electrochemomechanical theory for growth and remodeling of polyelectrolyte hydrogels and application to dynamic polymerization of $\text{DNA}$ hydrogels

Here this study develops a framework for growth and remodeling of active polyelectrolyte hydrogels that accounts for effects of compositional changes on the mechanical response. By developing a reactive electrochemomechanical theory, thermodynamical constraints upon reactive and remodeling processes are elucidated within a general framework that allows any number of chemical reactions to evolve the response of the gel and transfer mass and charge between constituents. Fully coupled, nonlinear constitutive relations are adopted for molar fluxes, allowing exploration of effects including cross-diffusion, electrophoresis, and electro-osmosis. A robust finite element implementation is developed in the open source FEBio software (febio.org) by exploiting an equivalence between electrochemomechanics and mixture theory. The implementation is verified against analytical solutions for free swelling, and a proper reduction to a prior chemomechanical theory is demonstrated for neutral gels swollen only by a solvent with no solutes. The theory and implementation are then applied to model the tunable large swelling achieved through dynamic polymerization of DNA crosslinkers seen in our recently developed experimental hydrogel system (Cangialosi et al., 2017). A novel constitutive model for reaction-driven evolution of the locking stretch λ L in a non-Gaussian mechanical free energy was developed, where the increasing concentration of DNA crosslinkers makes further swelling energetically favorable. With a single free parameter, excellent agreement was found between measured and predicted equilibrium swelling ratios. This study demonstrated the ability to extend the electrochemomechanical framework to include chemical reactions and composition-aware constitutive models, and showed that development of reactive models allows simulation of complex dynamic polymerization phenomena not treated before. The theoretical frame here can be further expanded in scope to incorporate additional non-ideal and nonlinear phenomena.

42 ENGINEERING↗

Topological valley Hall polariton condensation

A photonic topological insulator features robust directional propagation and immunity to defect perturbations of the edge/surface state. Exciton-polaritons, that is, the hybrid quasiparticles of excitons and photons in semiconductor microcavities, have been proposed as a tunable nonlinear platform for emulating topological phenomena. However, mainly due to excitonic material limitations, experimental observations so far have not been able to enter the nonlinear condensation regime or only show localized condensation in one dimension. Here, in this study, we show a topological propagating edge state with polariton condensation at room temperature and without any external magnetic field. We overcome material limitations by using excitonic CsPbCl 3 halide perovskites with a valley Hall lattice design. The polariton lattice features a large bandgap of 18.8 meV and exhibits strong nonlinear polariton condensation with clear long-range spatial coherence across the critical pumping density. The geometric parameters and material composition of our nonlinear many-body photonic system platform can in principle be tailored to study topological phenomena of other interquasiparticle interactions. Polariton condensation of topological propagating edge states is demonstrated with halide perovskite microcavities.

42 ENGINEERING↗

Tunable Laser-Plasma Amplifier (Final Report)

Exploration at the laser intensity frontier has always offered new avenues for physics and reaching beyond this frontier is a grand challenge. Present-day petawatt-class lasers provide focused intensities on target of 10 22 W/cm 2 , corresponding to electric fields of 200 TV/m, while laser-plasma amplification opens a route for focused intensities well above 10 23 W/cm 2 . Intensities in this range provide the ability to test quantum electrodynamics in the unexplored low-energy, strong-field regime where signatures for new physics may arise. The behavior of matter under such extraordinary conditions is a rich and fascinating subject, not only in its own right in fundamental plasma physics, but for the many potential applications that promise to enrich the natural sciences in the future, including compact electron-beam, ion-beam particle accelerators, and ultra-bright X-ray sources. Although laser systems are now under construction internationally to access intensities of 10 23 W/cm 2 , the current technologies used appear to be fundamentally limited to these intensities. The realization of intensities beyond 10 23 W/cm 2 using parametric amplification in plasmas promises a breakthrough in high-energy density physics. Parametric amplification using Raman scattering in a plasma could provide the enabling technology for the generation of ultra-high-power laser pulses, but a more complete understanding of the nonlinear optics of plasmas is required. There is a significant gap in well-diagnosed laser-plasma instability studies of nonlinear plasma-wave phenomena, which are critical to understand for future laser-plasma devices. To achieve an efficient laser-plasma amplifier, plasma waves must be driven to large amplitude where significant energy can be rapidly transferred from the pump to the seed over the pulse duration of the seed. Simulations suggest that this nonlinear pump depletion regime can be achieved in the “pi-pulse” amplification regime. While simulations show this optimal regime with efficient amplification, it has remained elusive in experiments and there is a growing consensus within the community that thermal effects and pump beam limitations prevent laser-plasma amplifiers from progressing through the linear regime into the nonlinear pump depletion regime. Previous experiments have been significantly limited by the laser power available at the necessary wavelengths for the seed laser; therefore, the amplification is required to start in the linear regime where it is sensitive to many deleterious effects. The enabling technology (currently unique to plasma-wave amplification in the world) at the University of Rochester is the ability to provide a seed pulse with sufficient power (4 mJ/100 fs seed) to immediately drive nonlinear plasma waves into the pi-pulse regime and to tune its wavelength to optimize the efficiency of energy transfer. This in combination with the state-of-the-art OMEGA heater beams providing multiple kilojoules in a nanosecond to sufficiently heat the plasma make this system distinct from previous studies. These heater beams will provide, for the first time in Raman amplification studies, a homogeneous electron temperature high enough to prevent pump beam propagation issues that have plagued previous experiments. These systems will provide a platform for driving electron-plasma waves into the nonlinear regime where pump depletion and pulse shortening are predicted to lead to high amplification efficiencies (>30%). The Team has made significant progress through prior support from DOE Fusion Energy Sciences [DOE Office of Science Award Number DE-SC0016253 (2016-2022)]. This includes twenty-two peer-reviewed manuscripts, one patent, ten contributed talks presented at international conferences, and research that was highlighted as invited talks at fifteen international conferences. The broader impacts of this research are evident in the support of early career scientists, two Ph.D. theses, four current graduate students, a Masters Project, two undergraduate researchers, and an underrepresented minority student hired through the California Alliance for Minority Participation who now works as a Research Engineer in the group. This research met all of the funded research objectives and the highlights from primary Raman amplification thrust of this work are discussed below and form the foundation for the proposed research.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Coupling magnons to an opto-electronic parametric oscillator

Hybrid magnonic systems have emerged as versatile modular components for quantum signal transduction and sensing applications owing to their capability of connecting distinct quantum platforms. To date, the majority of the magnonic systems have been explored in a local, near-field scheme, due to the close proximity required for realizing a strong coupling between magnons and other excitations. This constraint greatly limits the applicability of magnons in developing remotely coupled, distributed quantum network systems. On the contrary, opto-electronic architectures hosting self-sustained oscillations have been a unique platform for long-haul signal transmission and processing. Here, we integrated an opto-electronic oscillator with a magnonic oscillator consisting of a microwave waveguide and a Y 3 Fe 5 O 12 (YIG) sphere, and demonstrated strong and coherent coupling between YIG’s magnon modes and the opto-electronic oscillator’s characteristic photon modes—revealing the hallmark anti-crossing gap in the measured spectrum. In particular, the photon mode is produced on-demand via a nonlinear, parametric process as stipulated by an external seed pump. Both the internal cavity phase and the external pump phase can be precisely tuned to stabilize either degenerate or nondegenerate auto-oscillations. Our result lays out a new, hybrid platform for investigating the long-distance coupling and nonlinearity in coherent magnonic phenomena, which may be found useful in constructing the future “distributed hybrid magnonic systems.”

36 MATERIALS SCIENCE↗

Harmonic generation predominantly from a single spin channel in a half metal

Harmonic generation in atoms and molecules has reshaped our understanding of ultrafast phenomena beyond the traditional nonlinear optics and has launched attosecond physics. Harmonics from solids represent a new frontier, where both majority and minority spin channels contribute to harmonics. This is true even in a ferromagnet whose electronic states are equally available to optical excitation. In this work, we demonstrate that harmonics can be generated {mostly} from a single spin channel in half metallic chromium dioxide. An energy gap in the minority channel greatly reduces the harmonic generation, so harmonics predominantly emit from the majority channel, with a small contribution from the minority channel. However, this is only possible when the incident photon energy is well below the energy gap in the minority channel, so all the transitions in the minority channel are virtual. The onset of the photon energy is determined by the transition energy between the dipole-allowed transition between the O-$2p$ and Cr-$3d$ states. Harmonics mainly from a single spin channel can be detected, regardless of laser field strength, as far as the photon energy is below the minority band energy gap. This prediction should be tested experimentally

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Femtosecond-Terawatt Hard X-Ray Pulse Generation with Chirped Pulse Amplification on a Free Electron Laser

Advances of high intensity lasers have opened up the field of strong field physics and led to a broad range of technological applications. Recent x ray laser sources and optics development makes it possible to obtain extremely high intensity and brightness at x ray wavelengths. In this paper, we present a system design that implements chirped pulse amplification for hard x ray free electron lasers. Numerical modeling with realistic experimental parameters show that near-transform-limit single-femtosecond hard x ray laser pulses with peak power exceeding 1 TW and brightness exceeding 4×10 35 s -1 mm -2 mrad -2 0.1\%bandwdith -1 can be consistently generated. In conclusion, realization of such beam qualities is essential for establishing systematic and quantitative understanding of strong field x-ray physics and nonlinear x ray optics phenomena.

47 OTHER INSTRUMENTATION↗

Stable tuning of photorefractive microcavities using an auxiliary laser

Cavity nonlinear optics enables intriguing physical phenomena to occur at micro- or nano-scales with modest input powers. While this enhances capabilities in applications such as comb generation, frequency conversion, and quantum optics, undesired nonlinear effects including photorefraction and thermal bistability are exacerbated. In this Letter, we propose and demonstrate a highly effective method of achieving cavity stabilization using an auxiliary laser for controlling photorefraction in a z-cut periodically poled lithium niobate (LN) microcavity system. Our numerical study accurately models the photorefractive effect under high input powers, guiding future analyses and development of LN microcavity systems.

42 ENGINEERING↗

The data-driven future of high-energy-density physics

High-energy-density physics is the field of physics concerned with studying matter at extremely high temperatures and densities. Such conditions produce highly nonlinear plasmas, in which several phenomena that can normally be treated independently of one another become strongly coupled. The study of these plasmas is important for our understanding of astrophysics, nuclear fusion and fundamental physics—however, the nonlinearities and strong couplings present in these extreme physical systems makes them very difficult to understand theoretically or to optimize experimentally. Here we argue that machine learning models and data-driven methods are in the process of reshaping our exploration of these extreme systems that have hitherto proved far too nonlinear for human researchers. Furthermore, from a fundamental perspective, our understanding can be improved by the way in which machine learning models can rapidly discover complex interactions in large datasets. From a practical point of view, the newest generation of extreme physics facilities can perform experiments multiple times a second (as opposed to approximately daily), thus moving away from human-based control towards automatic control based on real-time interpretation of diagnostic data and updates of the physics model. To make the most of these emerging opportunities, we suggest proposals for the community in terms of research design, training, best practice and support for synthetic diagnostics and data analysis.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The Complexity of Nonlinear Flow and non-Fickian Transport in Fractures Driven by Three-Dimensional Recirculation Zones

Subsurface fluid flow and solute transport are typically described by first-order or linear rate laws. However, deviations from the first-order rate laws (or anomalous behavior) are typical and lead to nonlinear flow and non-Fickian transport phenomena. The shared underlying mechanisms for these “anomalous” flow and transport phenomena, which are actually typical of fractures, are seldom analyzed. We investigated the co-occurrence of nonlinear flow and non-Fickian transport through numerical simulation experiments of pore-scale flow and solute transport processes through three-dimensional natural fractures. In these fractures, 3-D recirculation zones (RZs) developed and grew with increasing flow rates. Flow nonlinearity resulted from the RZ development and growth, which shrank the main flow channel. Moreover, the same RZs also captured solutes from the main flow channel and released them back later. This retardation resulted in non-Fickian transport. Thus, nonlinear flow and non-Fickian transport are intertwined via their shared dependence on RZs.

58 GEOSCIENCES↗

Quantum kinetics of anomalous and nonlinear Hall effects in topological semimetals

Highlights: • Linear and photogalvanic anomalous Hall responses are systematically derived. • Extrinsic mechanisms of AHE include Gaussian, diffractive, hybrid skew scattering. • Diagrammatic calculations are matched to semiclassical picture of AHE. • The Pancharatnam phase of multifold fermions determines the skew scattering amplitude. • Photon-induced interband scattering are accompanied by coordinate shifts. We present a systematic microscopic derivation of the semiclassical Boltzmann equation for band structures with the finite Berry curvature based on Keldysh technique of nonequilibrium systems. In the analysis, an AC electrical driving field is kept up to quadratic order, and both cases of small and large frequencies corresponding to intra- and interband transitions are considered. In particular, this formulation is suitable for the study of nonlinear Hall effect and photogalvanic phenomena. The role of impurity scattering is carefully addressed. Specifically, in addition to previously studied side-jump and skew-scattering processes, quantum interference diffractive contributions are now explicitly incorporated within the developed framework. This theory is applied to multifold fermions in topological semimetals, for which the generic formula for the skew scattering rate from the Pancharatnam phase is obtained along with the corresponding anomalous Hall conductivity.

36 MATERIALS SCIENCE↗

Development of a conduction-based model for analyzing frozen startup of alkali-metal heat pipes

One key area of interest in heat pipe modeling/simulation is to analyze the startup behavior of the liquid-metal heat pipes (LMHPs) from a frozen state. This so-called ‘frozen startup’ process involves a complex set of nonlinear mass and heat transport phenomena, including phase transitions from solid to liquid and vapor, multiphase interactions, microporous wick flow, and compressible vapor dynamics. The complexity of these processes makes it challenging to simulate LMHP’s frozen startup using conventional numerical methods or commercial computational fluid dynamics (CFD) software. This paper presents a simplified conduction-based modeling approach that can provide practical insights into the entire LMHP frozen startup process, while alleviating the challenges of modeling its complex physics. The theoretical foundation and physical assumptions of the proposed model are based solely on heat-conduction equation, allowing for a more tractable simulation without sacrificing essential physical accuracy. The proposed model was implemented in a commercial CFD software, and its prediction was compared with the experimental data obtained from sodium heat-pipe startup experiments. The comparison highlights the proposed model's ability to capture the transient thermal behavior of LMHP during frozen startup. This study not only validates the conduction-based frozen startup modeling method but also shows its potential as a practical and efficient tool for understanding the startup performance of the LMHP systems.

Microreactor↗

Time-resolved atomic-resolution Brownian tomography of single nanocrystals reveals size-dependent dynamics

Atomic-resolution structure identification of nanocrystals by graphene liquid cell electron microscopy (GLC-EM) has revealed that small, solubilized platinum nanocrystals consist of an ordered crystalline core surrounded by mobile surface atoms, which dissociate during oxidative etching, resulting in distinct temporal structural states. Requirements imposed by the 3D reconstruction algorithm limit the number of structural states that can be resolved. We introduce a regularized 3D reconstruction algorithm that exploits the redundancy inherent in the experimental data, allowing us to improve the time resolution. Our developments provide a comprehensive molecular picture at unprecedented spatial and temporal resolution of the nonlinear, linear, and fluctuating dynamic phenomena that single nanocrystals undergo during the GLC-EM experiment. We determined atomic structures of 66 temporal structural states, extracted from 15 time trajectories of individual nanocrystals. Large (478 to 698 atoms) and small (<300 atoms) nanocrystals show etching that preserves a stable core, whereas mid-sized (351 to 571 atoms) nanocrystals present dynamics that change the coordination of the core.

Meana-Pañeda, Rubén↗

Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1- x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities

Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second-order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain-tunable photonics. Though very different phenomena at distinct frequencies, both second-order optical nonlinearity and piezoelectricity are third-rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm –2 was reported in Zn 1-x Mg x O films. Here, ferroelectric Zn 1-x Mg x O is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi-phase-matched optical harmonic generation as well as domain-engineered piezoelectric devices.

36 MATERIALS SCIENCE↗