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285 records · Page 16

Coherent band-edge oscillations and dynamic longitudinal-optical phonon mode splitting as evidence for polarons in perovskites

The coherence of collective modes, such as phonons and polarons, and their modulation of electronic states is long sought in complex systems, which is a crosscutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polarons, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal-optical (LO) phonons, has been intensely studied yet is still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect tolerance, long charge lifetimes, and diffusion lengths. In this work we use the intense single-cycle THz pulse with peak electric field up to E THz = 1000 kV/cm to drive coherent polaronic band-edge oscillations at room temperature in CH 3 NH 3 PbI 3 (MAPbI 3 ). We reveal the oscillatory behavior is dominated by a specific quantized lattice vibration mode at $ω$ LO ~ 4 THz, which is both dipole and momentum forbidden. THz-driven coherent polaron dynamics exhibits distinguishing features: room temperature coherent oscillations at ω LO longer than 1 ps in both single crystals and thin films, mode-selective modulation of different band-edge states assisted by electron-phonon interaction, and dynamic mode splitting at low temperature due to entropy and anharmonicity of organic cations. Our results demonstrate intense THz-driven coherent band-edge modulation is a powerful probe of electron-lattice coupling phenomena and polaronic quantum control in perovskites.

36 MATERIALS SCIENCE↗

Experiments to validate Thermodynamics and Transport models of Strongly Coupled Dusty Plasma Matter (Final Technical Report for DE-SC0023416)

The goal of this two-year grant is to provide access to the PI to dusty plasma experimental facilities at the DOE-funded Collaborative Research Facility Magnetized Plasma Research Laboratory, Auburn University to become a user of that facility, to obtain experimental data to support another ongoing grant DE-SC0021146 (an Early Career Award to the PI that is focused on modeling of dusty plasma thermodynamics and transport processes), to generate experimental data for funding proposals, and to provide exposure to University of Memphis students to advanced experimental techniques. The following technical accomplishments were made: 1. Development of a novel Bidirectional Electrode Control Arms Assembly (BECAA) for producing perfect 2D grain layers for complex plasma experimentation. BECAA uses movable electrode arms to tilt or move the electrode in a RF discharge from outside the chamber, allowing for the manipulation of grain clouds without needing to change the plasma parameters or gas pressure. This work addresses a longstanding gap in the literature for a method to produce clusters of selectable number of grains and that are perfectly two dimensional as opposed to being only quasi-2D. 2. Experimental investigation of the structural properties of finite-N clusters with N=2 to 50. Individual particle behavior in clusters could vary from grain to grain and this study measured systematically produced clusters for two different grain sizes. Analysis (funded by another grant DE-SC0021146) is currently underway to quantify the differences between grains that are found on the surface vs. the interior of clusters, the shell structure, and the decay of correlations in position, velocity, and kinetic energy. 3. An experimental method to measure the structural entropy of clusters was developed by observing the self-induced structural transitions between various possible arrangements. In a series of heating and cooling cycles, the number of times each possible arrangement was attained was experimentally observed and used to compute the probability of existence of that arrangement, and subsequently the configurational entropy of the cluster. Analysis (funded by another grant DE-SC0021146) is currently underway to produce the entropy of clusters as a function of the number of grains and use the same to compute thermodynamic state variables for 2D complex plasma/grain clusters. 4. A preliminary experimental study of multibody collisions between N grains (N=2 – 10) was conducted. The clusters were produced using the BECAA technique and velocities were imparted to the grains using manipulation laser pulses. Analysis (funded by another grant DE-SC0021146) is currently underway to develop a theoretical framework to describe multibody collisions analogous to classical two-body interactions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultrafast time-resolved 2D imaging of laser-driven fast electron transport in solid density matter using an x-ray free electron laser

High-power, short-pulse laser-driven fast electrons can rapidly heat and ionize a high-density target before it hydrodynamically expands. The transport of such electrons within a solid target has been studied using two-dimensional (2D) imaging of electron-induced Kα radiation. However, it is currently limited to no or picosecond scale temporal resolutions. Here, we demonstrate femtosecond time-resolved 2D imaging of fast electron transport in a solid copper foil using the SACLA x-ray free electron laser (XFEL). An unfocused collimated x-ray beam produced transmission images with sub-micron and ~10 fs resolutions. The XFEL beam, tuned to its photon energy slightly above the Cu K-edge, enabled 2D imaging of transmission changes induced by electron isochoric heating. Time-resolved measurements obtained by varying the time delay between the x-ray probe and the optical laser show that the signature of the electron-heated region expands at ~25% of the speed of light in a picosecond duration. Time-integrated Cu Kα images support the electron energy and propagation distance observed with the transmission imaging. The x-ray near-edge transmission imaging with a tunable XFEL beam could be broadly applicable for imaging isochorically heated targets by laser-driven relativistic electrons, energetic protons, or an intense x-ray beam.

47 OTHER INSTRUMENTATION↗

Purcell enhancement of directional edge photocurrent in a van der Waals self-cavity

Cavities provide a means to manipulate the optical and electronic responses of quantum materials by selectively enhancing light-matter interaction at specific frequencies and momenta. While cavities typically involve external structures, exfoliated flakes of van der Waals (vdW) materials can form intrinsic self-cavities due to their small finite dimensions, confining electromagnetic fields into plasmonic cavity modes, characterized by standing-wave current distributions. While cavity-enhanced phenomena are well-studied at optical frequencies, the impact of self-cavities on nonlinear electronic responses—such as directional photocurrent—remains largely unexplored, particularly in the terahertz regime, critical for emerging ultrafast optoelectronic technologies. Here, we report a self-cavity-induced Purcell enhancement of directional photocurrents in the vdW semimetal WTe 2 . Using ultrafast optoelectronic circuitry, we measured coherent near-field THz emission resulting from nonlinear photocurrents excited at the sample edges. We observed enhanced emission at finite frequencies, tunable via excitation fluence and sample geometry, which we attribute to plasmonic interference effects controlled by the cavity boundaries. We developed an analytical theory that captures the cavity resonance conditions and spectral response across multiple devices. Our findings establish WTe 2 as a bias-free, geometry-tunable THz emitter and demonstrate the potential of self-cavity engineering for controlling nonlinear, nonequilibrium dynamics in quantum materials.

condensed-matter physics↗

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↗

Light storage, retrieval, and controllable interference in an atomic tripod system

Highly efficient quantum memories are essential for advancing quantum information processing technologies, including scalable quantum computing and quantum networks. We experimentally demonstrate a light storage and retrieval protocol in a tripod system using an ensemble of laser-cooled 87 Rb atoms. The tripod system, which consists of three ground states and an excited state, offers rich dynamics: its use to coherently store and retrieve a weak probe pulse in the 87 Rb 𝐹 = 1 ground-state manifold leads to the interference of two spin-wave excitations during storage time that translate to an interference in the peak intensity of the retrieved probe pulse. Our work shows that these interferences, which manifest when varying the pulse sequence or energy level structure, can be controlled experimentally by varying the storage time, optical phase, and magnetic field strength. Theoretical simulations exhibit excellent agreement with the experimental results. In conclusion, this work demonstrates the rich dynamics and versatile capabilities of atomic tripod systems for light storage and retrieval, with key advantages over conventional Λ systems, highlighting the potential of atomic tripod systems for applications in quantum information processing, quantum synchronization, and atomic memory protocols.

Coherent control↗

Physics of Hard Spheres Experiment: Significant and Quantitative Findings Made

Direct examination of atomic interactions is difficult. One powerful approach to visualizing atomic interactions is to study near-index-matched colloidal dispersions of microscopic plastic spheres, which can be probed by visible light. Such spheres interact through hydrodynamic and Brownian forces, but they feel no direct force before an infinite repulsion at contact. Through the microgravity flight of the Physics of Hard Spheres Experiment (PHaSE), researchers have sought a more complete understanding of the entropically driven disorder-order transition in hard-sphere colloidal dispersions. The experiment was conceived by Professors Paul M. Chaikin and William B. Russel of Princeton University. Microgravity was required because, on Earth, index-matched colloidal dispersions often cannot be density matched, resulting in significant settling over the crystallization period. This settling makes them a poor model of the equilibrium atomic system, where the effect of gravity is truly negligible. For this purpose, a customized light-scattering instrument was designed, built, and flown by the NASA Glenn Research Center at Lewis Field on the space shuttle (shuttle missions STS 83 and STS 94). This instrument performed both static and dynamic light scattering, with sample oscillation for determining rheological properties. Scattered light from a 532- nm laser was recorded either by a 10-bit charge-coupled discharge (CCD) camera from a concentric screen covering angles of 0 to 60 or by sensitive avalanche photodiode detectors, which convert the photons into binary data from which two correlators compute autocorrelation functions. The sample cell was driven by a direct-current servomotor to allow sinusoidal oscillation for the measurement of rheological properties. Significant microgravity research findings include the observation of beautiful dendritic crystals, the crystallization of a "glassy phase" sample in microgravity that did not crystallize for over 1 year in 1g (Earth's gravity), and the emergence of face-centered-cubic (FCC) crystals late in the coarsening process (as small crystallites lost particles to the slow ripening of large crystallites). Significant quantitative findings from the microgravity experiments have been developed describing complex interactions among crystallites during the growth process, as concentration fields overlap in the surrounding disordered phase. Time-resolved Bragg scattering under microgravity captures one effect of these interactions quite conclusively for the sample at a volume fraction of 0.528. From the earliest time until the sample is almost fully crystalline, the size and overall crystallinity grow monotonically, but the number of crystallites per unit volume (number density) falls. Apparently nucleation is slower than the loss of crystallites because of the transfer of particles from small to large crystals. Thus, coarsening occurs simultaneously with growth, rather than following the completion of nucleation and growth as is generally assumed. In the same sample, an interesting signature appears in the apparent number density of crystallites and the volume fraction within the crystallites shortly before full crystallinity is reached. A brief upturn in both indicates the creation of more domains of the size of the average crystallite simultaneous with the compression of the crystallites. Only the emergence of dendritic arms offers a reasonable explanation. The arms would be "seen" by the light scattering as separate domains whose smaller radii of curvature would compress the interior phase. In fiscal year 1999, numerous papers, a doctoral dissertation, and the PHaSE final report were produced. Although this flight project has been completed, plans are in place for a follow-on colloid experiment by Chaikin and Russel that employs a light microscope within Glenn's Fluids and Combustion Facility on the International Space Station. PHaSE is providing us with a deeper understanding of the nure of phase transitions. The knowledge derived has added to the understanding of condensed matter. In addition, the burgeoning study of the dynamics of colloidal self-assembly may lead to the development of a range of photonic materials that control the desirable properties of light. Thus, applications of ordered colloidal structures include not only ultrastructure ceramics, but also photonic crystals and photothermal nanosecond light-switching devices. Industries dealing with semiconductors, electro-optics, ceramics, and composites stand to benefit from such advancements.

Doherty, Michael P.↗

TRACER Carbonaceous Aerosols Thrust – University of California, Davis Field Campaign Report

The broader U.S. Department of Energy Atmospheric Radiation Measurement (ARM) user facility’s TRacking Aerosol Convection interactions ExpeRiment (TRACER) campaign aims to increase our understanding of convective cloud life cycles and aerosol-convection interactions. Our TRACER Carbonaceous Aerosols Thrust-University of California, Davis (TRACER-CAT-UCDavis) study complemented these broader aims by characterizing and quantifying the optical properties and composition of carbonaceous aerosols during part of the TRACER intensive sampling period (July 1- July 31, 2022) at the first ARM Mobile Facility (AMF1) main site (M1) in La Porte, Texas. Our measurements complemented the suite of instrumentation already provided by the AMF1, expanding the capabilities through deployment of unique, state-of-the-science instrumentation. The instrumentation included: (i) two cavity-attenuated phase shift spectroscopy single-scatter albedo (CAPS-SSA) instruments operating at 530 nm and 630 nm, and that were modified to characterize particle light absorption, extinction, and scattering at elevated humidities; (ii) the UC Davis dual-wavelength cavity ringdown-photoacoustic spectrometer (CRD-PAS), which characterizes dry particle extinction and absorption at 405 nm and 532 nm; (iii) a soot particle aerosol mass spectrometer (SP-AMS) that operated in “laser only” mode that characterized the size-dependent compositions of black carbon (BC)-containing particles; (v) a thermal denuder, to remove coatings on particles; and (vi) a scanning electrical mobility sizer (SEMS), to characterize particle mobility diameters from 10-1300 nm. Our measurements occurred alongside complementary observations made by Los Alamos National Laboratory (LANL) during the TRACER-CAT-LANL study, including a humidified CAPS-SSA instrument operating at 450 nm. Our primary scientific interest is in understanding the relationship between particle composition and light absorption, with a particular focus on the influence of water uptake. While it is known that coatings on BC can enhance absorption, the extent to which this occurs in the atmosphere and the specific role that water plays as a coating remain unclear. The TRACER-CAT-UCDavis measurements were made with near-complete coverage for the CRD-PAS, SP-AMS, and SEMS throughout the intensive period. The UC Davis humidified CAPS-SSA instruments had significant challenges with operation owing to the demanding conditions (large temperature fluctuations, high humidity), exacerbated by supply chain issues that delayed resolution of these challenges. However, the humidified CAPS-SSA instrument operated by LANL operated throughout the intensive period with near-complete coverage. The dry light extinction measurements from the CRD-PAS measurements and the LANL CAPS-SSA exhibited a good correlation, although the CAPS-SSA systematically measured greater extinction values than expected. While all instruments, with the exception of an aerodynamic particle sizer (APS), measured behind a common particulate matter (PM)2.5 μm cyclone, the greater extinction measured by the LANL CAPS-SSA compared to the CRD-PAS may have resulted from different losses of larger particles in the sampling lines from the cyclone to the instruments; the tubing length was shorter from the cyclone to the LANL CAPS-SSA, consistent with this idea. A summary of the TRACER-CAT-UCDavis measurements, along with some of the TRACER-CAT-LANL measurements, are shown in the figure below. Notably, there were periods when the contributions of presumed dust were substantial and even dominated the observed light extinction and absorption. Also, there was a clear shift in the behavior of submicron particles from before July 16, 2022 to after, with the prior period exhibiting regular episodes of new particle formation and the latter period exhibiting rapid variations in the concentrations of small particles.

54 ENVIRONMENTAL SCIENCES↗

Unraveling electronic correlations in warm dense quantum plasmas

The study of matter at extreme densities and temperatures has emerged as a highly active frontier at the interface of plasma physics, material science and quantum chemistry with relevance for planetary modeling and inertial confinement fusion. A particular feature of such warm dense matter is the complex interplay of Coulomb interactions, quantum effects, and thermal excitations, making its rigorous theoretical description challenging. Here, we demonstrate how ab initio path integral Monte Carlo simulations allow us to unravel this intricate interplay for the example of strongly compressed beryllium, focusing on two X-ray Thomson scattering data sets obtained at the National Ignition Facility. We find excellent agreement between simulation and experiment with a very high level of consistency between independent observations without the need for any empirical input parameters. Our results call into question previously used chemical models, with important implications for the interpretation of scattering experiments and radiation hydrodynamics simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A portable and monoenergetic 24 keV neutron source based on 124Sb-9Be photoneutrons and an iron filter

A portable monoenergetic 24 keV neutron source based on the 124Sb-9Be photoneutron reaction and an iron filter has been constructed and characterized. The coincidence of the neutron energy from SbBe and the low interaction cross-section with iron (mean free path up to 29 cm) makes pure iron specially suited to shield against gamma rays from 124Sb decays while letting through the neutrons. To increase the 124Sb activity and thus the neutron flux, a >1 GBq 124Sb source was produced by irradiating a natural Sb metal pellet with a high flux of thermal neutrons in a nuclear reactor. The design of the source shielding structure makes for easy transportation and deployment. A hydrogen gas proportional counter is used to characterize the neutrons emitted by the source and a NaI detector is used for gamma background characterization. At the exit opening of the neutron beam, the characterization determined the neutron flux in the energy range 20–25 keV to be 6.00±0.30 neutrons per cm2 per second and the total gamma flux to be 245±8 gammas per cm2 per second (numbers scaled to 1 GBq activity of the 124Sb source). A liquid scintillator detector is demonstrated to be sensitive to neutrons with incident kinetic energies from 8 to 17 keV, so it can be paired with the source as a backing detector for neutron scattering calibration experiments. This photoneutron source provides a good tool for in-situ low energy nuclear recoil calibration for dark matter experiments and coherent elastic neutrino-nucleus scattering experiments.

Dark Matter detectors (WIMPs, axions, etc.)↗

COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics

The COLUMBUS program system provides the tools for performing high-level multireference (MR) computations, including the multireference configuration interaction (MRCI) method and its multireference averaged quadratic coupled cluster (MR-AQCC) extension, allowing computations on a wide range of fascinating atomic and molecular systems, including the treatment of open-shells and complicated excited state phenomena. The inclusion of spin−orbit coupling (SOC) directly within the MRCI step enables the description of systems containing heavy elements, such as lanthanides and actinides, whose properties are strongly influenced by SOC. Analytic energy gradients and nonadiabatic couplings at the correlated MRCI level provide the foundation for a variety of dynamics studies, giving insight into ultrafast photochemistry. New and ongoing method developments in COLUMBUS include the computation of spin densities, improved descriptions of ionic states, enhancements to the AQCC method, and the porting of COLUMBUS to graphical processing units (GPUs). New external interfaces enable an enhanced description of electronic resonances and molecules in strong laser fields. This work highlights these new developments while providing a detailed account of the diverse applications of COLUMBUS in recent years.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Intrinsic nonlocality of spin- and polarization-resolved probabilities in strong-field quantum electrodynamics

Spin and polarization are central to precision tests of fundamental physics and for interpreting radiation from astrophysical sources and ultraintense laser-matter experiments. Here, focusing on the fundamental process of nonlinear Compton scattering, we demonstrate that a key assumption underlying current strong-field quantum electrodynamics models, i.e., that emission can be treated as an instantaneous random event sampled from a local differential rate, is inconsistent once emission angles, electron spin, and/or photon polarization are resolved. Namely, even in strictly constant and uniform fields , the resulting fully differential distribution is sign indefinite, yielding negative inferred probabilities. The physical reason is that the photon emission probability builds up over a finite length of the electron trajectory, the formation region, during which the electron direction changes by roughly the same small angle that defines the radiation cone. Therefore, we put forward a new method where we integrate over this formation region analytically to obtain a physically consistent electron spin and photon polarization model. We show that the implementation of our model is compatible with existing Monte Carlo and particle-in-cell workflows. Simulations of a GeV-class electron-laser collision accessible at current petawatt facilities and of emission in a pulsarlike magnetic field are shown to reveal spin and polarization patterns that differ even qualitatively from state-of-the-art local models. In particular, our new model predicts substantial angle-dependent circular photon polarization where the well-known collinear-emission approach yields none, and a pronounced helicity bias in the recoiling electrons absent from current predictions. These findings have direct implications for upcoming strong-field QED experiments and for interpreting polarized radiation from extreme astrophysical environments.

astrophysical electromagnetic fields↗

Space-Time Quantum Information from the Entangled States of Magnetic Molecule (STI Product)

This collaborative project combines synthesis, measurement, and theory by three faculty members at the Eddleman Quantum Institute of UC Irvine to effectively investigate the quantum properties of molecules in the space, time, and frequency domains. Through synthetic chemistry, molecules are tailored for their magnetic and coherent properties. By combining femtosecond (fs) terahertz (THz) light and a continuous wave (cw) THz laser with a low temperature scanning tunneling microscope (STM), quantum phenomena are probed with simultaneous femtosecond temporal and atomic-scale spatial resolution. In particular, the invention of the quantum superposition microscope (QSM) advances quantum sensing for enhanced spectroscopy and imaging capabilities. Coupling theory to the experimental efforts offers a deeper understanding and predictive power for the molecular systems. The phenomena of superposition, entanglement, and coherence is central to quantum information science and can be realized in qubit states. Many systems can be modeled by a double-well potential in which two levels are formed in the two lowest energy states interacting with the environment and external radiation. In focusing on molecules as two-level systems, the underlying expectation is that their tunable composition and structure allows an effective parameter space to optimize their use as qubits for quantum sensing and computing. The THz radiation induces the superposition between the two states, appearing as temporal oscillations that damp in amplitude. Enhanced spectroscopy and imaging in the time and frequency domains is achieved through the extreme sensitivity of the frequency and damping of coherence of two-level systems to its environment. A single hydrogen molecule trapped in the STM tunneling gap experiences a double-well potential and absorption of THz femtosecond pulses of light creates the superposition of its two levels, appearing as damped oscillations in the light induced direct current (DC). The oscillation frequency depends sensitively on the electric field distribution of the copper nitride (Cu 2 N) surface, through the Stark effect, and associated with the different charge distributions at the copper and nitrogen sites and in between. This QSM can resolve variation in the surface electric field with 0.02 nanometer resolution. In addition, the single hydrogen molecule entaes with nearby hydrogen molecules as seen in the avoided level crossings of energy (oscillation frequency) versus the voltage across the tunneling gap. Thus, the first application of the QSM senses and images the surface electric field at the atomic scale. Results from this project advance fundamental understanding of quantum phenomena, develop novel synthesis, measurement, and theory, provide the knowledge foundation for molecule-based qubits and sensing that enable the development of the QSM and emergent technologies. This project trained researchers in quantum information science, extended knowledge in classrooms, and outreached to the community.

47 OTHER INSTRUMENTATION↗

Aluminum-Based Superconducting Tunnel Junction Sensors for Nuclear Recoil Spectroscopy

The BeEST experiment is searching for sub-MeV sterile neutrinos by measuring nuclear recoil energies from the decay of 7 Be implanted into superconducting tunnel junction (STJ) sensors. The recoil spectra are affected by interactions between the radioactive implants and the sensor materials. We are therefore developing aluminum-based STJs (Al-STJs) as an alternative to existing tantalum devices (Ta-STJs) to investigate how to separate material effects in the recoil spectrum from potential signatures of physics beyond the Standard Model. Three iterations of Al-STJs were fabricated. The first had electrode thicknesses similar to existing Ta-STJs. They had low responsivity and reduced resolution, but were used successfully to measure 7 Be nuclear recoil spectra. The second iteration had STJs suspended on thin SiN membranes by backside etching. These devices had low leakage current, but also low yield. The final iteration was not backside etched, and the Al-STJs had thinner electrodes and thinner tunnel barriers to increase signal amplitudes. These devices achieved 2.96 eV FWHM energy resolution at 50 eV using a pulsed 355 nm (~3.5 eV) laser. These results establish Al-STJs as viable detectors for systematic material studies in the BeEST experiment.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗