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At least 91 records · Page 5

The coherent Cerenkov radiated power from a group of field-aligned test particles in a magnetoplasma

An expression is derived that describes the coherent Cerenkov radiated power from a group of test particles in a plasma medium moving parallel to a magnetic field. In this analysis, each particle has an arbitrary position and velocity along a field line and, as a consequence, both the spatial and temporal coherence of the radiation are considered. As an example, it is demonstrated that a monoenergetic electron beam consisting of small pulses can generate wave powers well above incoherent levels if the pulse spacing is comparable to an integer number of emission wavelengths. It is also shown that, if the beam particles have a velocity spread, Delta-V, the wave powers will decrease in time due to the reduced temporal coherence of the particle radiators, where this coherence scales as 1/Delta-V. This latter effect applies to any charged particle beam propagating in a magnetoplasma, because even an initially monoenergetic beam becomes thermalized by electrostatic wave-particle interactions reducing the radiated power.

Farrell, W. M.↗

Plasmonically assisted channels of photoemission from metals

We analyze recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbar$ω p above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbar$ω p and nonlinear 2$\hbar$ω p electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters

Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe 2+ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Furthermore, our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Skopi: a simulation package for diffractive imaging of noncrystalline biomolecules

X-ray free-electron lasers (XFELs) have the ability to produce ultra-bright femtosecond X-ray pulses for coherent diffraction imaging of biomolecules. While the development of methods and algorithms for macromolecular crystallography is now mature, XFEL experiments involving aerosolized or solvated biomolecular samples offer new challenges in terms of both experimental design and data processing. Skopi is a simulation package that can generate single-hit diffraction images for reconstruction algorithms, multi-hit diffraction images of aggregated particles for training machine learning classifiers using labeled data, diffraction images of randomly distributed particles for fluctuation X-ray scattering algorithms, and diffraction images of reference and target particles for holographic reconstruction algorithms. Skopi is a resource to aid feasibility studies and advance the development of algorithms for noncrystalline experiments at XFEL facilities.

59 BASIC BIOLOGICAL SCIENCES↗

Optical control of ultrafast structural dynamics in a fluorescent protein

The photoisomerization reaction of a fluorescent protein chromophore occurs on the ultrafast timescale. The structural dynamics that result from femtosecond optical excitation have contributions from vibrational and electronic processes and from reaction dynamics that involve the crossing through a conical intersection. The creation and progression of the ultrafast structural dynamics strongly depends on optical and molecular parameters. When using X-ray crystallography as a probe of ultrafast dynamics, the origin of the observed nuclear motions is not known. Now, high-resolution pump–probe X-ray crystallography reveals complex sub-ångström, ultrafast motions and hydrogen-bonding rearrangements in the active site of a fluorescent protein. However, we demonstrate that the measured motions are not part of the photoisomerization reaction but instead arise from impulsively driven coherent vibrational processes in the electronic ground state. A coherent-control experiment using a two-colour and two-pulse optical excitation strongly amplifies the X-ray crystallographic difference density, while it fully depletes the photoisomerization process. A coherent control mechanism was tested and confirmed the wave packets assignment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spectral and Spatial Properties of Amplified Radiation in High Gain Tapering Enhanced Stimulated Super-radiant Amplification Regime (Technical Report)

There is a wide convergence of scientific and industrial interests in understanding the physics of high efficiency conversion of relativistic electron beam power into coherent radiation. Improved understanding would open the door to ultrahigh intensity X-ray laser pulses (single shot coherent imaging and Schwingerfield physics), as well as at longer wavelength for fast throughput material processing (EUV-lithography). Modern particle accelerators can be extremely efficient (approaching 50 %) in terms of wall-plug energy use. State-of-the-art light sources on the other hand do not take advantage of all the available power and most of it is left in the beam and simply wasted on the beam dump. This proposal aimed at developing a program based on Tapered Enhanced Stimulated Superradiant Amplification to address the current limitation in electron-based coherent radiation generation exploiting the progress in high brightness beam generation and strong coupling with the electromagnetic field in a strongly tapered undulator system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Aerosol Wind Profiler (AWP) Doppler Wind Lidar Airborne Observations During the NOAA Joint Venture 3-D Wind Measurement Demonstration and NASA Active-Passive Profiling Experiment (APEX)

The NASA Langley Research Center (LaRC) has recently completed development of the Aerosol Wind Profiler (AWP) airborne Doppler wind lidar (DWL) instrument. AWP was supported by the NASA Earth Science Technology Office and the Earth Science Division, a project that adapted the Wind-Space Pathfinder (Wind-SP) DWL transceiver onto a structure for flight aboard a variety of NASA research aircraft. AWP demonstrates many technologies required for a space DWL mission, including a coherent-detection, optical heterodyne laser transmitter with high pulse energy (up to ~55 mJ) and repetition rate (200 Hz), electronic control of the beam path allowing for multiple viewing angles (allowing vector wind measurements) with no moving parts, compact highly-stable and tunable reference lasers allowing for high-precision measurement of velocity at long ranges while mitigating the impact of satellite platform velocity, and many others. AWP represents NASA’s only currently operational airborne 3-D wind profiling sensor. NASA LaRC was selected by the NOAA Joint Venture (JV) program to conduct a suborbital 3-D Wind measurement campaign demonstrate how data from a coherent-detection DWL like AWP could serve NOAA’s weather analysis and forecasting needs. The NOAA JV program is designed to work with the private sector, academia and other federal agencies to explore the feasibility and capability of emerging technologies spacecraft and other mission-specific tools to meet NOAA’s mission requirements. AWP was initially demonstrated on the NASA DC-8 within this JV program in October 2023, piggybacking on the NASA EcoDemonstrator mission focused on in-situ sampling of jet aircraft emissions and contrail formation from Everett, Washington. The in-situ sampling resulted in very frequent and rapid aircraft attitude changes which unfortunately degraded AWP data quality. But, during times with level flight and AVAPS dropsonde operations, AWP demonstrated excellent precision (< 2 m/s RMS) with high vertical (< 100 meter) resolution and 2 km spacing between profiles. AWP will be flown again on the NASA LaRC Gulfstream-3 from mid-September to mid-October 2024 out of Hampton, VA to complete the NOAA JV 3-D wind demonstration. Additional AWP flights will occur in early November from southern California during the NASA Active-Passive Profiling Experiment (APEX), focused on underflights of the NASA ER-2 equipped with many atmospheric profiling sensors. This presentation will summarize AWP measurements collected during these two fall 2024 flight campaigns, and how the AWP data compares with AVAPS dropsonde, NOAA weather prediction model, and GOES atmospheric motion vector data.

Kristopher Bedka↗

Nonlinear X-ray Optics

Novel X-ray free-electron lasers (XFELs) are capable of producing radiation with unprecedented properties. Specifically, their ultrashort coherent X-ray pulses can generate extreme peak intensities where ordinary rules of light-matter interaction may no longer apply, and nonlinear processes start to become important. XFELs have made it possible to observe some of the most important coherent non-sequential nonlinearities, including X-ray-optical sum frequency generation (SFG), X-ray second harmonic generation (XSHG), two-photon absorption (TPA) and nonlinear two-photon Compton scattering (2PCS). In particular, the 2PCS experiment has led to unexpected results, namely the observation of a substantial anomalous red shift in the energy of photons generated by nonlinear two-photon X-ray Compton scattering in beryllium. The energy shift is in addition to the predicted nonlinear Compton shift and was neither expected from extrapolations from linear X-ray interactions nor from nonlinear effects at optical wavelengths. Our results suggest a novel nonlinear scattering mechanism that can only be observed at high fields at X-ray wavelengths, where the photon energy is a significant fraction of the electron rest mass (and thus a significant momentum transfer to the electron occurs during the scattering) and where the interaction is not dominated by the quiver motion of the electron in the field (ponderomotive potential) as is usually the case at longer (optical) wavelengths. The goal of this research project was the investigation of fundamental nonlinear X-ray-matter interactions. As these processes are typically weak, part of this research is the exploration of more efficient nonlinear X-ray processes by studying novel mechanisms including solid-state effects, the assistance of optical radiation and novel phase-matching techniques. These experiments require extremely large X-ray field strengths, such as produced by XFELs. Nonlinear X-ray effects can lead to important applications in many research fields. For example, it could lead to instantaneous plasma diagnostics for materials in extreme conditions, as a method for combining atomic-scale structural sensitivity with chemical specificity, or as a probe of electron dynamics in solids on the attosecond (1 as = 10 -18 s) time- and Ångstrom (10 -10 m) length scales. In addition, a detailed understanding of nonlinear X-ray matter interactions is crucial for understanding and extending the limits of structural determination at high intensity such as in serial femto-crystallography. The results could have a profound impact on advanced XFEL light sources such as the LCLS-II.

47 OTHER INSTRUMENTATION↗

Production of high fluence laser beams using ion wave plasma optics

Optical components for laser beams with high peak and averaged powers are being developed worldwide using stimulated plasma scattering that occurs when plasmas interact with intense, coherent light. After decades of pursuit of pulse compressors, mirrors, and other plasma based components that can be created by stimulated scattering from electron density perturbations forming on ultra-short time scales (e.g., via Stimulated Raman Scattering), more recent work has produced optical components on longer time scales allowing ion motion as well [via Stimulated Brillouin Scattering (SBS)]. In the most recent work, ion wave plasma optics have had success in producing pulses of focusable coherent light with high energy and fluence by operating on ns time scales and now promise to enable numerous applications. Experiments have further shown that in some parameter regimes, even simple plasma response models can describe the output of such optics with sufficient accuracy that they can be used as engineering tools to design plasma optics for future applications, as is already being done to control power deposition in fusion targets. In addition, the development of more sophisticated models promises to enable still higher performance from SBS driven plasma optical components under a wider range of conditions. The present status and most promising directions for future development of ion wave plasma optic techniques are discussed here.

47 OTHER INSTRUMENTATION↗

Characterizing coherences in chemical dynamics with attosecond time-resolved x-ray absorption spectroscopy

Coherence can drive wave-like motion of electrons and nuclei in photoexcited systems, which can yield fast and efficient ways to exert materials’ functionalities beyond the thermodynamic limit. The search for coherent phenomena has been a central topic in chemical physics although their direct characterization is often elusive. Here, we highlight recent advances in time-resolved x-ray absorption spectroscopy (tr-XAS) to investigate coherent phenomena, especially those that utilize the eminent light source of isolated attosecond pulses. The unparalleled time and state sensitivities of tr-XAS in tandem with the unique element specificity render the method suitable to study valence electronic dynamics in a wide variety of materials. The latest studies have demonstrated the capabilities of tr-XAS to characterize coupled electronic–structural coherence in small molecules and coherent light–matter interactions of core-excited excitons in solids. Furthermore, we address current opportunities and challenges in the exploration of coherent phenomena, with potential applications for energy- and bio-related systems, potential crossings, strongly driven solids, and quantum materials, and so with the ongoing developments in both theory and light sources, tr-XAS holds great promise for revealing the role of coherences in chemical dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Measurement Capabilities of Planar Doppler Velocimetry in Large-Scale Wind Tunnels

Over the past few years, Planar Doppler Velocimetry (PDT) has been shown by several laboratories to offer an attractive means for measuring three-dimensional velocity vectors everywhere in a light sheet placed in a flow. Unlike some other optical means of measuring flow velocities, PDT is particularly attractive for use in large wind tunnels where distances to the sample region may be several meters, because it does not require the spatial resolution and tracking of individual scattering particles or the alignment of crossed beams at large distances. To date, demonstrations of PDT (also called Doppler Global Velocimetry by some authors) have been made either in low speed flows without quantitative comparison to other measurements, or in supersonic flows where the Doppler shift is large and its measurement is relatively insensitive to instrumental errors. Moreover, most reported applications have relied on the use of continuous-wave lasers, which limit the measurement to time-averaged velocity fields. This work summarizes the results of two previous studies of PDT in which the use of pulsed lasers to obtain instantaneous velocity vector fields is evaluated. The objective has been to quantitatively define and demonstrate PDT capabilities for applications in large-scale wind tunnels that are intended primarily for the testing of rotorcraft and subsonic aircraft at speeds typically less than 100 m/s. For such applications, the adequate resolution of low-speed flow fields requires accurate measurements of small Doppler shifts that are obtained at distances of several meters from the sample region and with a field of view that is sufficient to encompass the entire region of interest. The use of pulsed lasers provides the unique capability to obtain not only time-averaged fields, but also their statistical fluctuation amplitudes and the spatial excursions of unsteady flow regions such as wakes, separations, and rotor-tip vortices. To accomplish the objectives of these studies, the PDT measurement process was first modeled and its performance evaluated computationally. The noise sources considered included those related to the optical and electronic properties of Charge-Coupled Device (CCD) arrays and to speckle effects associated with the coherent illumination of aerosols from pulsed lasers. The signal noise estimates were incorporated into the PDT signal analysis process and combined with computed scattering signals using a Mae scattering theory for a distributed range of aerosol particle sizes. The results are used to define the necessary instrument configuration, to show that the expected signal levels from a practical PDT system are sufficiently large to allow its useful application in large facilities, and to show that the expected velocity measurement uncertainties are small compared to the mean velocities of interest for most subsonic, large-scale wind tunnel testing, Experimental studies using several bench-top setups are then described that validate the physics of the PDT model and demonstrate the ability to obtain accurate PDT measurements using procedures that are compatible with large-scale wind tunnel operations. The PDT measurement capabilities found in this study lead to the conclusion that PDT offers significant advantages compared to other means of measuring velocity fields in large-scale wind tunnels, including those operating at low speeds.

McKenzie, Robert L.↗

Quantum coherence tomography of light-controlled superconductivity

The coupling between superconductors and oscillation cycles of light pulses, i.e., lightwave engineering, is an emerging control concept for superconducting quantum electronics. Although progress has been made towards terahertz-driven superconductivity and supercurrents, the interactions able to drive non-equilibrium pairing are still poorly understood, partially due to the lack of measurements of high-order correlation functions. In particular, the sensing of exotic collective modes that would uniquely characterize light-driven superconducting coherence, in a way analogous to the Meissner effect, is very challenging but much needed. Here we report the discovery of parametrically driven superconductivity by light-induced order-parameter collective oscillations in iron-based superconductors. The time-periodic relative phase dynamics between the coupled electron and hole bands drives the transition to a distinct parametric superconducting state out-of-equalibrium. This light-induced emergent coherence is characterized by a unique phase–amplitude collective mode with Floquet-like sidebands at twice the Higgs frequency. We measure non-perturbative, high-order correlations of this parametrically driven superconductivity by separating the terahertz-frequency multidimensional coherent spectra into pump–probe, Higgs mode and bi-Higgs frequency sideband peaks. We find that the higher-order bi-Higgs sidebands dominate above the critical field, which indicates the breakdown of susceptibility perturbative expansion in this parametric quantum matter.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Coherent high-power RF wakefield generation by electron bunch trains in a metamaterial structure

In this paper, we present an experimental study of coherent high-power wakefield generation in a metamaterial (MTM) structure at 11.7 GHz by 65 MeV electron bunch trains at the Argonne Wakefield Accelerator (AWA), following a previous experiment, the Stage-I experiment, at the AWA. Both the Stage-II experiment, reported in this paper, and the Stage-I experiment were conducted using MTM structures, which are all-metal periodic structures with the period being much smaller than the wavelength. Differences between the two experiments include (1) structure length (Stage-I 8 cm and Stage-II 20 cm); (2) number of bunches used to excite the structure (Stage-I with two bunches, up to 85 nC of total charge; Stage-II with eight bunches, up to 224 nC of total charge); and (3) highest peak power measured (Stage-I 80 MW in a 2 ns pulse and Stage-II 380 MW in a 10 ns pulse). High-power radio frequency pulses were generated by reversed Cherenkov radiation of the electron beam due to the negative group velocity in the MTM structures. Because the radiation is coherent, a train of bunches with a proper spacing can build up to achieve a high peak power. The observed output power levels are very promising for future applications in direct collinear wakefield acceleration or in transfer to a second accelerator for two-beam acceleration.

36 MATERIALS SCIENCE↗

Illuminating Ligand Field Contributions to Molecular Qubit Spin Relaxation via T 1 Anisotropy

Electron spin relaxation in paramagnetic transition metal complexes constitutes a key limitation on the growth of molecular quantum information science. However, there exist very few experimental observables for probing spin relaxation mechanisms, leading to a proliferation of inconsistent theoretical models. Here we demonstrate that spin relaxation anisotropy in pulsed electron paramagnetic resonance is a powerful spectroscopic probe for molecular spin dynamics across a library of highly coherent Cu(II) and V(IV) complexes. Here, neither the static spin Hamiltonian anisotropy nor contemporary computational models of spin relaxation are able to account for the experimental T 1 anisotropy. Through analysis of the spin-orbit coupled wavefunctions, we derive an analytical theory for the T 1 anisotropy that accurately reproduces the average experimental anisotropy of 2.5. Furthermore, compound-by-compound deviations from the average anisotropy provide a promising approach for observing specific ligand field and vibronic excited state coupling effects on spin relaxation. Finally, we present a simple density functional theory workflow for computationally predicting T 1 anisotropy. Analysis of spin relaxation anisotropy leads to deeper fundamental understanding of spin-phonon coupling and relaxation mechanisms, promising to complement temperature-dependent relaxation rates as a key metric for understanding molecular spin qubits.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti 3 O 5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti 3 O 5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

36 MATERIALS SCIENCE↗

Ultrafast optically induced spin transfer in ferromagnetic alloys

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Prelaunch testing of the laser geodynamic satellite (LAGEOS)

The LAGEOS was extensively tested optically prior to launch. The measurement techniques used are described and resulting data is presented. Principal emphasis was placed on pulse spreading characteristics, range correction for center of mass tracking, and pulse distortion due to coherent effects. A mode-locked freqeuncy doubled Nd:YAG laser with a pulse width of about 60 ps was used as the ranging transmitter and a crossfield photo-multiplier was used in the receiver. High speed sampling electronics were employed to increase receiver bandwidth. LAGEOS reflected pulses typically had a width of 250 ps with a variability in the range correction of less than 2 mm rms. Pulse distortion due to coherent effects was inferred from average waveforms and appears to introduce less than + or - 50 ps jitter in the location of the pulse peak. Analytic results on this effect based on computer simulations are also presented. Theoretical and experimental data on the lidar cross section were developed in order to predict the strength of lidar echoes from the satellite. Cross section was measured using a large aperture laser collimating system to illuminate the LAGEOS. Reflected radiation far-field patterns were measured using the collimator in an autocollimating mode. Data were collected with an optical data digitzer and displayed as a three-dimensional plot of intensity versus the two far-field coordinates. Measurements were made at several wavelengths, for several types of polarizations, and as a function of satellite orientation.

Fitzmaurice, M. W.↗

Potential of Attosecond Coherent Diffractive Imaging

Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules, and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond pulses have intrinsically very broad spectra due to the uncertainty principle and are incompatible with conventional imaging systems. In this paper we report an important advance towards achieving attosecond coherent diffractive imaging. Using simulated attosecond pulses, we simultaneously reconstruct the spectrum, 17 probes, and 17 spectral images of extended objects from a set of ptychographic diffraction patterns. We further confirm the principle and feasibility of this method by successfully performing a ptychographic coherent diffractive imaging experiment using a light-emitting diode with a broad spectrum. We believe this work clears the way to an unexplored domain of attosecond imaging science, which could have a far-reaching impact across different disciplines.

36 MATERIALS SCIENCE↗