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At least 1,243 records · Page 69

Time-resolved experiments on gas-phase atoms and molecules with XUV and X-ray free-electron lasers

Over the last 20 years, XUV and X-ray free-electron lasers have enabled a wide variety of time-resolved experiments that have dramatically advanced our understanding of ultra-fast molecular dynamics on atomic length scales and femto-second time scales. This review focuses on experimental studies of ultrafast dynamics of atoms and molecules in the gas phase, tracing the development of the field from early proof-of-principle studies to recent pump-probe experiments that elucidate the coupled electronic and nuclear dynamics during photochemical reactions with a temporal resolution that is now extending into the attosecond domain.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Investigating Powder Spreading Dynamics in Additive Manufacturing Processes by In-situ High-speed X-ray Imaging

The quality of the powder bed is known to be one of the main factors that influence the quality of the part being manufactured by powderbed- based additive manufacturing processes. For example, in the laser powder bed fusion process, it has been demonstrated that improving the powder bed density and homogeneity improves the final quality of the part. Understanding powder spreading dynamics in the powder-bed-based additive manufacturing processes is critical for designing spreading structures and spreading parameters, identifying defect formation mechanisms in the powder bed, and guiding the design of optimized feedstock powders. Extensive efforts have been devoted to understand the fundamental mechanism of the powder flow and spreading process. Various powder flow testers were used to study the flow behavior of powders used in additive manufacturing. However, the powder flow conditions in flow meters are different from those in real additive manufacturing conditions. Models have also been developed to simulate and study the spreading process. The discrete element method (DEM) is currently the main tool for computationally simulating the spreading process. However, these models are based on many physical assumptions. Visible light cameras have been used recently to conduct in-situ study of powder spreading in additive manufacturing. Due to the limited resolution and penetration depth of visible light, it is extremely difficulty to study the particle-scale powder spreading dynamics. Here, to overcome the challenges of studying powder spreading dynamics under real additive manufacturing conditions, we developed an experimental approach to study the particle-scale powder spreading process with high spatial and temporal resolution using the high-speed high-energy X-ray imaging facility at beamline 32-ID-B of the APS. Figure 1 shows an overview of the research setup. It is composed of a vacuum chamber (building environment), an automatic powder spreading system, a laser system, an X-ray source (X-ray outlet), and an X-ray detection/imaging system.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nonlinear dynamics of topological Dirac fermions in 2D spin-orbit coupled materials

Abstract The graphene family materials are two-dimensional staggered monolayers with a gapped energy band structure due to intrinsic spin-orbit coupling. The mass gaps in these materials can be manipulated on-demand via biasing with a static electric field, an off-resonance circularly polarized laser, or an exchange interaction field, allowing the monolayer to be driven through a multitude of topological phase transitions. We investigate the dynamics of spin-orbit coupled graphene family materials to unveil topological phase transition fingerprints embedded in the nonlinear regime and show how these signatures manifest in the nonlinear Kerr effect and in third-harmonic generation processes. We show that the resonant nonlinear spectral response of topological fermions can be traced to specific Dirac cones in these materials, enabling characterization of topological invariants in any phase by detecting the cross-polarized component of the electromagnetic field. By shedding light on the unique processes involved in harmonic generation via topological phenomena our findings open an encouraging path towards the development of novel nonlinear systems based on two-dimensional semiconductors of the graphene family.

36 MATERIALS SCIENCE↗

Low-power millimeter-wave radar observations of the atmosphere

Historically, cloud structures, dynamics, and precipitation processes have been observed and measured with sensors from two different spatial resolutions. Laser-based sensors have volume resolutions on the order of 10(exp -4) to 10(exp -2) cubic meters for a 1-s sample. Radar systems operating at wavelengths between 1 and 10 cm have resolutions on the order of 10(exp 4) to 10(exp 7) cubic meters. The resolutions of micro-wave systems depend primarily on the system RF bandwidth and antenna bandwidth. Both resolution regimes were useful in the study of cloud structures and processes - the former for determining resolution on the individual cloud particle scale and the latter for studying the coarse characteristics of cloud dynamics and structure. There are, however, cloud processes and structures that occur on scales that lie between these two regimes: the process of entrainment, where outside air is brought within the cloud boundaries; the mixing of in-cloud particles with different histories; cloud particle coalescence; and ice formation. The use of mm-wave (30- to 300-GHz) radars offers an opportunity to observe cloud processes at these scales and determine their influence on precipitation development, cloud albedos, cloud lifetimes, chemical cycling of tract substances, aircraft icing, and other meteorological phenomena. To determine the usefulness of a 35-GHz radar for observing these precipitation and cloud processes, a research program was initiated. The objectives of this program are to develop a 35-GHz radar, to measure scattering from precipitation and clouds, and to develop a model to compute scattering from clouds using the finite-difference time-domain (FDTD) technique.

Ronnau, James F.↗

Laser, vacuum and gas reaction chamber for operando measurements at NSLS-II's 28-ID-2

We present a laser reaction chamber that we have developed for in situ/operando X-ray diffraction measurements at the NSLS-II 28-ID-2 X-ray powder diffraction beamline. This chamber allows for rapid and dynamic sample heating under specialized gas environments, spanning ambient conditions down to vacuum pressures. We demonstrate the capabilities of this setup through two applications: laser-driven heating in polycrystalline iron oxide and in single-crystal WTe 2 . Our measurements reveal the ability to resolve chemical reaction kinetics over minutes with 1 s time resolution. This setup advances opportunities for in situ/operando X-ray diffraction studies of both bulk and single-crystal materials.

36 MATERIALS SCIENCE↗

Ultrafast formation of topological defects in a two-dimensional charge density wave

Topological defects play a central role in dynamical systems undergoing a non-adiabatic transition. In solids, topological defects as a result of femtosecond laser excitation have attracted increasing interest not only because they are key to understanding phase transitions but also because they can generate a variety of hidden orders that are not accessible in thermal equilibrium. Despite the common occurrence of these defects in a non-equilibrium system, the fundamental limit on how fast they can emerge in solids and the generic pathway for defect creation at such fast timescales have remained open questions. Here we apply ultrafast electron diffraction to study the reciprocal-space signatures of transient defects in a two-dimensional charge density wave, where simultaneous measurements of both defect and phonon dynamics yield a microscopic view of defect formation in the femtosecond regime. We find that one-dimensional domain walls are generated well within 1 ps following photoexcitation, during which the defect growth is not dictated by the amplitude of the order parameter but is mediated by a non-thermal population of longitudinal optical phonons. In conclusion, our work provides a framework for the ultrafast engineering of topological defects that are coupled to specific collective modes, which will prove useful for the dynamical control of non-equilibrium phases in correlated materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dual use of image based tracking techniques: Laser eye surgery and low vision prosthesis

With a concentration on Fourier optics pattern recognition, we have developed several methods of tracking objects in dynamic imagery to automate certain space applications such as orbital rendezvous and spacecraft capture, or planetary landing. We are developing two of these techniques for Earth applications in real-time medical image processing. The first is warping of a video image, developed to evoke shift invariance to scale and rotation in correlation pattern recognition. The technology is being applied to compensation for certain field defects in low vision humans. The second is using the optical joint Fourier transform to track the translation of unmodeled scenes. Developed as an image fixation tool to assist in calculating shape from motion, it is being applied to tracking motions of the eyeball quickly enough to keep a laser photocoagulation spot fixed on the retina, thus avoiding collateral damage.

Juday, Richard D.↗

Dual Use of Image Based Tracking Techniques: Laser Eye Surgery and Low Vision Prosthesis

With a concentration on Fourier optics pattern recognition, we have developed several methods of tracking objects in dynamic imagery to automate certain space applications such as orbital rendezvous and spacecraft capture, or planetary landing. We are developing two of these techniques for Earth applications in real-time medical image processing. The first is warping of a video image, developed to evoke shift invariance to scale and rotation in correlation pattern recognition. The technology is being applied to compensation for certain field defects in low vision humans. The second is using the optical joint Fourier transform to track the translation of unmodeled scenes. Developed as an image fixation tool to assist in calculating shape from motion, it is being applied to tracking motions of the eyeball quickly enough to keep a laser photocoagulation spot fixed on the retina, thus avoiding collateral damage.

Juday, Richard D.↗

Decoding THz‐Driven Dynamic Fingerprints of Ferroelectric Nanotwin Networks

Ultrafast polarization dynamics in ferroelectrics are of considerable interest for high-speed tunable dielectrics and electro-optics. Extended domain wall networks formed in ferroelectric twin nanodomains can support collective dynamics in the terahertz regime but require techniques that track polarization and strain evolution driven by ultrafast stimulus. Here, we use multi-modal probing of THz-pulse-driven excitations in PbTiO 3 /SrTiO 3 superlattices by combining X-ray free electron laser measurements that directly tracks lattice changes, with optical second harmonic generation that tracks the electronic potential coupled with the lattice potential. Dynamical phase-field modeling enables fingerprinting of these collective modes as superpositions of domain “breathing” through wall oscillations and polarization “rotations” with still walls. Ultrafast domain wall motion at 0.1–0.5 THz is observed at practical fields of 100 kV/cm with wall velocities of >4000 m/s, approaching typical speed of sound in PbTiO 3 . A unique “charging” mode is discovered that can electrically charge and discharge domain walls on ∼4 ps time scale thus dynamically tuning wall conductivity. Integrated experimental and theoretical fingerprinting of the dynamical landscape presented here enables ultrafast control of ferroics for high-speed microelectronics and optical applications.

THz dynamics↗

Multichannel photodissociation dynamics in CS 2 studied by ultrafast electron diffraction

In this study, the structural dynamics of photoexcited gas-phase carbon disulfide (CS 2 ) molecules are investigated using ultrafast electron diffraction. The dynamics were triggered by excitation of the optically bright 1 B 2 ( 1 Σ u + ) state by an ultraviolet femtosecond laser pulse centred at 200 nm. In accordance with previous studies, rapid vibrational motion facilitates a combination of internal conversion and intersystem crossing to lower-lying electronic states. Photodissociation via these electronic manifolds results in the production of CS fragments in the electronic ground state and dissociated singlet and triplet sulphur atoms. The structural dynamics are extracted from the experiment using a trajectory-fitting filtering approach, revealing the main characteristics of the singlet and triplet dissociation pathways. Finally, the effect of the time-resolution on the experimental signal is considered and an outlook to future experiments provided.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Anomalously slow hot carrier cooling and insulator-to-metal transition in a photo-doped Mott insulator

Photo-doped Mott insulators can exhibit novel photocarrier transport and relaxation dynamics and non-equilibrium phases. However, time-resolved real-space imaging of these processes are still lacking. Here, we use scanning ultrafast electron microscopy (SUEM) to directly visualize the spatial-temporal evolution of photoexcited species in a spin-orbit assisted Mott insulator α-RuCl 3 . At low optical fluences, we observe extremely long hot photocarrier transport time over one nanosecond, almost an order of magnitude longer than any known values in conventional semiconductors. At higher optical fluences, we observe nonlinear features suggesting a photo-induced insulator-to-metal transition, which is unusual in a large-gap Mott insulator. Our results demonstrate the rich physics in a photo-doped Mott insulator that can be extracted from spatial-temporal imaging and showcase the capability of SUEM to sensitively probe photoexcitations in strongly correlated electron systems.

42 ENGINEERING↗

In-situ Nondestructive Evaluation of In-flight Particle Dynamics and Intrinsic Properties for Directed Energy Deposition

The objective of this exploratory project is to determine the feasibility of using laser diffraction, structured light 3D scanning, and x-ray diffraction for in-situ assessment and inspection of metal directed energy deposition (DED) that is applied to repair components such as engine parts in remanufacturing. During this project, we have successfully published or submitted at least one journal article for each subtask that we identified. One of our conference paper and presentation has won “best paper award” from Manufacturing & Design Division in the Institute of Industrial and Systems Engineers (IISE) Annual Conference 2021. Through this seed grant, we successfully validated the concepts and proved the three in-situ monitoring techniques work well to predict some defects generation during direct energy deposition. We submitted follow-up proposals to continue work on this topic.

36 MATERIALS SCIENCE↗

Doppler lidar studies of atmospheric wind field dynamics

For the past 5 years the Wave Propagation Lab. has operated a pulsed CO2 Doppler lidar system to evaluate coherent laser radar technology and to investigate applications of the technique in atmospheric research. The capability of the system to provide measurements of atmospheric winds, backscatter, and water vapor has been extensively studied over this period. Because Doppler lidar can measure atmospheric wind structure in the clear air without degradation by terrain features, it offers a unique capability as a research tool for studies of many transient or local scale atmospheric events. This capability was demonstrated in recent field experiments near Boulder, Colo. and Midland, Tex., in which the lidar clearly depicted the wind field structure associated with several types of phenomena, including thunderstorm microbursts, valley drainage flow, and passage of a dryline front. To improve sensitivity during the periods of low aerosol backscatter, the system has recently been upgraded with new transmitter/receiver hardware. The upgraded system, which transmit 2 J per pulse of output energy at a rate of 50 Hz and incorporates computer control for automated operation, underwent calibration testing during the spring of 1986.

Hardesty, R. M.↗

Simulation of Laser Cooling and Trapping in Engineering Applications

An advanced computer code is undergoing development for numerically simulating laser cooling and trapping of large numbers of atoms. The code is expected to be useful in practical engineering applications and to contribute to understanding of the roles that light, atomic collisions, background pressure, and numbers of particles play in experiments using laser-cooled and -trapped atoms. The code is based on semiclassical theories of the forces exerted on atoms by magnetic and optical fields. Whereas computer codes developed previously for the same purpose account for only a few physical mechanisms, this code incorporates many more physical mechanisms (including atomic collisions, sub-Doppler cooling mechanisms, Stark and Zeeman energy shifts, gravitation, and evanescent-wave phenomena) that affect laser-matter interactions and the cooling of atoms to submillikelvin temperatures. Moreover, whereas the prior codes can simulate the interactions of at most a few atoms with a resonant light field, the number of atoms that can be included in a simulation by the present code is limited only by computer memory. Hence, the present code represents more nearly completely the complex physics involved when using laser-cooled and -trapped atoms in engineering applications. Another advantage that the code incorporates is the possibility to analyze the interaction between cold atoms of different atomic number. Some properties that cold atoms of different atomic species have, like cross sections and the particular excited states they can occupy when interacting with each other and light fields, play important roles not yet completely understood in the new experiments that are under way in laboratories worldwide to form ultracold molecules. Other research efforts use cold atoms as holders of quantum information, and more recent developments in cavity quantum electrodynamics also use ultracold atoms to explore and expand new information-technology ideas. These experiments give a hint on the wide range of applications and technology developments that can be tackled using cold atoms and light fields. From more precise atomic clocks and gravity sensors to the development of quantum computers, there will be a need to completely understand the whole ensemble of physical mechanisms that play a role in the development of such technologies. The code also permits the study of the dynamic and steady-state operations of technologies that use cold atoms. The physical characteristics of lasers and fields can be time-controlled to give a realistic simulation of the processes involved such that the design process can determine the best control features to use. It is expected that with the features incorporated into the code it will become a tool for the useful application of ultracold atoms in engineering applications. Currently, the software is being used for the analysis and understanding of simple experiments using cold atoms, and for the design of a modular compact source of cold atoms to be used in future research and development projects. The results so far indicate that the code is a useful design instrument that shows good agreement with experimental measurements (see figure), and a Windows-based user-friendly interface is also under development.

Ramirez-Serrano, Jaime↗

Kinetic simulations of piston-driven collisionless shock formation in magnetized laboratory plasmas

Laboratory laser experiments offer a novel approach to studying magnetized collisionless shocks, and a common method in recent experiments is to drive shocks using a laser-ablated piston plasma. However, current experimental capabilities are still limited to spatio-temporal scales on the order of shock formation, making it challenging to distinguish piston and shock dynamics. We present quasi-1D particle-in-cell simulations of piston-driven, magnetized collisionless shock formation using the code psc , which includes a model of laser-driven plasmas that can be well-matched to experimental conditions. The simulations cover a range of upstream and ablation parameters and yield several robust signatures of shock formation that can provide a reference for experimental results.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Simulation studies of the interaction of laser radiation with additively manufactured foams

The interaction of laser radiation with foams of various porosities and low densities has been the subject of several numerical and experimental studies. In all cases, the modeling of low-Z under-dense foams as uniform gases of equivalent average density using standard radiation-hydrodynamics codes has resulted in heat-front velocities that are considerably faster than those observed experimentally. It has been theoretically conjectured that this difference may be attributed to the breakdown of the foam’s morphology, leading to a dynamics of filament expansion where the ion and electron energy partitions are significantly different from those calculated using the uniform gas model. We found that 3D computer simulations employing a disconnected representation of the foam’s microstructure which allowed for the dynamics of foam element heating, expansion, and stagnation largely supported the theoretical picture. Simulations using this model for laser experiments on under-dense 2 mg cc -1 SiO 2 aerogel foams reproduced the experimental data fairly well. We used the validated model in simulations of low-density structured foam-like materials (produced via additive manufacturing) with a variety of morphologies. We found that the log-pile configurations were consistent with the analytical propagation model of Gus’kov et al. Further validation of the model was obtained by simulating experiments performed at the Jupiter Laser Facility using the log-pile and octet-truss foam morphologies. Simulations of the foam-laser interaction using a wave propagation code showed that the microstructure was able to enhance stimulated Brillouin scattering (SBS) by concentrating the light energy into density holes. In turn, this promotes laser filamentation, reducing SBS and bringing the predicted values closer to the experimental data.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Microstructural evolution of rapidly solidified hypoeutectic Al 10Cu alloy during non-isothermal annealing transients induced by nano-second laser pulses

The evolution of characteristic nonequilibrium features presenting in morphologically distinct regions of rapid solidification (RS) microstructures in a hypoeutectic Al—10Cu (atomic %) in response to non-isothermal annealing transients has been studied by transmission electron microscopy (TEM). The capabilities of the Movie-Mode Dynamic TEM (MM-DTEM) instrument were used to expose select regions of the RS microstructure to sequences of rapid heating and cooling transients induced by nanosecond laser pulses while permitting in-situ observation. Partial melting, microstructural scale coarsening, morphological changes of the nonequilibrium features in the multi-phase RS microstructure, and solid-state phase transformation were observed. Heterogeneous nucleation of nanoscale θ-Al 2 Cu phase involved metastable supersaturated α-Al and the θ'-Al 2 Cu phases, establishing different sets of orientation relationships for the stable θ-Al 2 Cu and α-Al phases. Replacement of banded morphology grains that formed under conditions driven farthest from equilibrium by an equiaxed nanocrystalline structure comprised of α-Al phase, the primary solidification product, and an intergranular network of Al 2 Cu crystals has been attributed to local remelting. Here the experimental approach explored, permitted discovery of mechanistic details of location-specific transformation pathways activated in the multi-phase RS microstructure of hypoeutectic Al—Cu during subsequent nonisothermal transients.

36 MATERIALS SCIENCE↗