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DOE OSTI2023

Toward a fully coherent tender and hard X-ray free-electron laser via cascaded EEHG in fourth-generation synchrotron light sources

Free-electron-laser-based beamlines utilize fully coherent laser pulses with extremely narrow bandwidth allowing direct use of X-rays without monochromators. This could be very beneficial for all users of current and future fourth-generation diffraction-limited synchrotron light sources (DL-SLSs) who need narrowband full-coherence high-brightness X-ray pulses. Based on our previous finding, i.e. that separating the two stages of echo-enabled harmonic generation (EEHG) with a few extra bending-magnet sections provides an effective way to increase the momentum compaction of chicane 1, one can simultaneously achieve adequate prebunching at extremely high harmonics as well as keep the energy modulation to the ideal minimum. This could open the door for cascaded EEHG, toward fully coherent tender and hard X-ray wavelengths. Built on our compact design of a twin-pulse seeding electron beam with an adjustable delay and timing jitter at the level of a few femtoseconds, a cascaded EEHG can be implemented, which includes two EEHG beamlines, where the radiation pulse generated by the first beamline with harmonic $h$ 1 could be used as the input seed laser pulse to the second beamline with harmonic $h$ 2 . Hence, the second radiator could potentially reach very high harmonics [$h$ = $h$ 1 (20)$h$ 2 (25–100)] from 500 to 2000, corresponding to tender and hard X-ray wavelengths. It is demonstrated that the cascaded EEHG scheme is compatible with almost any current or planned fourth-generation DL-SLS, with significant benefits for space-limited storage rings in particular. The main advantage is that this scheme requires almost no change of the storage-ring lattice and is fully compatible with other beamlines. Current proposals for rings with much longer straight sections would add self-amplified spontaneous emission as another viable option for storage-ring-based free-electron lasers.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Scalable single-mode surface-emitting laser via open-Dirac singularities

Single-aperture cavities are a key component of lasers that are instrumental for the amplification and emission of a single light mode. However, the appearance of high-order transverse modes as the size of the cavities increases has frustrated efforts to scale-up cavities while preserving single-mode operation since the invention of the laser six decades ago. A suitable physical mechanism that allows single-mode lasing irrespective of the cavity size-a 'scale invariant' cavity or laser-has not been identified yet. Here we propose and demonstrate experimentally that open-Dirac electromagnetic cavities with linear dispersion-which in our devices are realized by a truncated photonic crystal arranged in a hexagonal pattern-exhibit unconventional scaling of losses in reciprocal space, leading to single-mode lasing that is maintained as the cavity is scaled up in size. The physical origin of this phenomenon lies in the convergence of the complex part of the free spectral range in open-Dirac cavities towards a constant governed by the loss rates of distinct Bloch bands, whereas for common cavities it converges to zero as the size grows, leading to inevitable multimode emission. An unconventional flat-envelope fundamental mode locks all unit cells in the cavity in phase, leading to single-mode lasing. We name such sources Berkeley surface-emitting lasers (BerkSELs) and demonstrate that their far-field corresponds to a topological singularity of charge two, in agreement with our theory. Open-Dirac cavities unlock avenues for light-matter interaction and cavity quantum electrodynamics.

42 ENGINEERING↗

DOE OSTI2023

Density variance dynamics in disparate shock tubes

This report discusses two experiments which investigate thin layer, heavy curtain fragmentation from the perspective of a Reynolds-Averaged mix model, in drastically disparate experimental regimes. The first, the centimeter/millisecond-scale “Horizontal Shock Tube” (HST) is a compressed-gas piston-driven shock tube experiment. The second, the “Multishock thin layer” (Mshock) experiment performed at the National Ignition Facility, is a micrometer/nanosecond-scale laser-driven shock tube experiment. Both are situations in which a heavy plane layer (a ‘curtain’) is initially suspended in a lighter medium. After being shocked from at least one side, the layer translates while its interfaces evolve due to the excitation of the Richtmyer-Meshkov instability at its surfaces. The evolution of density variance, which initially exists only on the surface of the layer, as it comes to encompass the whole layer interior is used as a description of layer fragmentation and dissolution. These experiments have each been simulated in the Los Alamos National Laboratory multi-physics code xRAGE, which includes fundamental hydrodynamics, extended plasma physics and radiation effects which are important to drive the high-energy density experiment, and the Besnard-Harlow-Rauenzahn (BHR) turbulence model. In each, the principal diagnostic for comparison is an experimental metric for the density (co)variance, b, which tracks the moments of the density field at the curtain interfaces and body. Due to experimental constraints in different regimes (i.e. optical diagnostics can be deployed on conventional shock tubes, while the plasma shock tubes must be imaged by x-rays; interfaces can be imposed to specification on laser-driven experiments, which are stored in the solid phase, while conventional experiments have imperfect control of the flow fields which separate the layer, etc.) the experiments are not designed to be perfect scaled cognates of one another. However, despite the separation of six orders of magnitude of scaling in time, and four in space, we are able to demonstrate that the same turbulence model, operating in the same fashion in the same computer code, is able to reproduce results in each experiment, by tracking evolution due to common relevant physics. Additionally, we will present preliminary work toward density variance comparisons in a single-interface Richtmyer-Meshkov configuration, the conventional fluid “Vertical Shock Tube” (VST) experiment, and the Modal Initial Conditions (ModCons) campaign fielded at the OMEGA-EP laser facility.

42 ENGINEERING↗

DOE OSTI2021

Toward Å-fs-meV Resolution in Electron Microscopy: Systematic Simulation of the Temporal Spread of Single-Electron Packets

Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å-fs-meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform – attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales. With General Particle Tracer, we studied the statistical temporal distributions of single-electron packets as a function of various fs pulsed-laser parameters and electron-gun configurations and fields for the exact architecture and dimensions of a Thermo Fisher Tecnai Femto ultrafast electron microscope. We focused on easily-adjustable parameters, such as laser pulse duration, laser spot size, photon energy, Wehnelt aperture diameter, and photocathode size. In addition to establishing trends and dispersion behaviors, we identify regimes within which packet duration can be 100s of fs and approach the 300-fs laser limit employed here. Overall, the results provide a detailed picture of the temporal behavior of single-electron packets in the Tecnai Femto gun region, forming the initial contribution of a larger effort.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

High-Throughput Microstructural Characterization and Process Correlation Using Automated Electron Backscatter Diffraction

The need to optimize the processing conditions of additively manufactured (AM) metals and alloys has driven advances in throughput capabilities for material property measurements such as tensile strength or hardness. High-throughput (HT) characterization of AM metal microstructure has fallen significantly behind the pace of property measurements due to intrinsic bottlenecks associated with the artisan and labor-intensive preparation methods required to produce highly polished surfaces. This inequality in data throughput has led to a reliance on heuristics to connect process to structure or structure to properties for AM structural materials. In this study, we show a transformative approach to achieve laser powder bed fusion (LPBF) printing, HT preparation using dry electropolishing and HT electron backscatter diffraction (EBSD). This approach was used to construct a library of > 600 experimental EBSD sample sets spanning a diverse range of LPBF process conditions for AM Kovar. This vast library is far more expansive in parameter space than most state-of-the-art studies, yet it required only approximately 10 labor hours to acquire. Build geometries, surface preparation methods, and microscopy details, as well as the entire library of >600 EBSD data sets over the two sample design versions, have been shared with intent for the materials community to leverage the data and further advance the approach. Using this library, we investigated process–structure relationships and uncovered an unexpected, strong dependence of microstructure on location within the build, when varied, using otherwise identical laser parameters.

Characterization and Analytical Technique↗

DOE OSTI2022

Photoinduced evolution of lattice orthorhombicity and conceivably enhanced ferromagnetism in LaMnO 3 membranes

Ultrashort laser pulses have been utilized to dynamically drive phase transitions in correlated quantum materials. Of particular interest is whether phases not achievable in thermal equilibrium can be induced in complex oxides with intricately coupled lattice, electron and spin degrees of freedom. Here, we tracked atomic motions in LaMnO 3 following photoexcitation with MeV ultrafast electron diffraction (MeV-UED) technique. We found that the light excited state exhibits numerous signatures different from thermal equilibrium ones, including nearly conserved Bragg intensities, strongly suppressed La cation and oxygen anion displacements, and the long-range lattice orthorhombicity evolution. Furthermore, using first-principles calculations, we predict that the ferromagnetic ordering and conductivity are both enhanced upon laser excitation due to the reduction of the lattice orthorhombicity. This work benefits from recent advance in fabrication of membrane films with high epitaxial quality and in MeV-UED with large momentum space access and high temporal resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Accurate and confident prediction of electron beam longitudinal properties using spectral virtual diagnostics

Abstract Longitudinal phase space (LPS) provides a critical information about electron beam dynamics for various scientific applications. For example, it can give insight into the high-brightness X-ray radiation from a free electron laser. Existing diagnostics are invasive, and often times cannot operate at the required resolution. In this work we present a machine learning-based Virtual Diagnostic (VD) tool to accurately predict the LPS for every shot using spectral information collected non-destructively from the radiation of relativistic electron beam. We demonstrate the tool’s accuracy for three different case studies with experimental or simulated data. For each case, we introduce a method to increase the confidence in the VD tool. We anticipate that spectral VD would improve the setup and understanding of experimental configurations at DOE’s user facilities as well as data sorting and analysis. The spectral VD can provide confident knowledge of the longitudinal bunch properties at the next generation of high-repetition rate linear accelerators while reducing the load on data storage, readout and streaming requirements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2022

A machine learning photon detection algorithm for coherent x-ray ultrafast fluctuation analysis

X-ray free electron laser experiments have brought unique capabilities and opened new directions in research, such as creating new states of matter or directly measuring atomic motion. One such area is the ability to use finely spaced sets of coherent x-ray pulses to be compared after scattering from a dynamic system at different times. This enables the study of fluctuations in many-body quantum systems at the level of the ultrafast pulse durations, but this method has been limited to a select number of examples and required complex and advanced analytical tools. By applying a new methodology to this problem, we have made qualitative advances in three separate areas that will likely also find application to new fields. As compared to the “droplet-type” models, which typically are used to estimate the photon distributions on pixelated detectors to obtain the coherent x-ray speckle patterns, our algorithm achieves an order of magnitude speedup on CPU hardware and two orders of magnitude improvement on GPU hardware. We also find that it retains accuracy in low-contrast conditions, which is the typical regime for many experiments in structural dynamics. Finally, it can predict photon distributions in high average-intensity applications, a regime which up until now has not been accessible. Our artificial intelligence-assisted algorithm will enable a wider adoption of x-ray coherence spectroscopies, by both automating previously challenging analyses and enabling new experiments that were not otherwise feasible without the developments described in this work.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

High Harmonic Generation Seeding Echo-Enabled Harmonic Generation toward a Storage Ring-Based Tender and Hard X-ray-Free Electron Laser

To align with the global trend of integrating synchrotron light source (SLS) and free electron laser (FEL) facilities on one site, in line with examples such as SPring-8 and SACLA in Japan and ELETTRA and FERMI in Italy, we actively explore FEL options leveraging the ultralow-emittance electron beam of the NSLS-II upgrade. These options show promising potential for synergy with storage ring (SR) operations, thereby significantly enhancing our facility’s capabilities. Echo-enabled harmonic generation (EEHG) is well-suited to SR-based FELs, and has already been demonstrated with the capability of generating extremely narrow bandwidth as well as high brightness, realized using diffraction-limited short pulses in transverse planes and Fourier transform-limited bandwidth in the soft X-ray spectrum. However, regarding a conventional EEHG scheme, the combination of the shortest seed laser wavelength (256 nm) and highest harmonic (200) sets the short wavelength limit to λ = 1.28 nm. To further extend the short wavelength limit down to the tender and hard X-ray region, a vital option is to shorten the seed laser wavelength. Thanks to recent advances in high harmonic generation (HHG), packing 10 9 photons at one harmonic within a few-femtosecond pulse could turn such a novel HHG source into an ideal seeding for EEHG. Thus, compared to the cascaded EEHG, the HHG seeding option could not only lower the cost, but also free the SR space for accommodating more user beamlines. Moreover, to mitigate the SASE background noise on the sample and detector, we combine the HHG seeding EEHG with the crab cavity short pulse scheme for maximum benefit.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Folding at the Microscale: Enabling Multifunctional 3D Origami‐Architected Metamaterials

Abstract Mechanical metamaterials inspired by the Japanese art of paper folding have gained considerable attention because of their potential to yield deployable and highly tunable assemblies. The inherent foldability of origami structures enlarges the material design space with remarkable properties such as auxeticity and high deformation recoverability and deployability, the latter being key in applications where spatial constraints are pivotal. This work integrates the results of the design, 3D direct laser writing fabrication, and in situ scanning electron microscopic mechanical characterization of microscale origami metamaterials, based on the multimodal assembly of Miura‐Ori tubes. The origami‐architected metamaterials, achieved by means of microfabrication, display remarkable mechanical properties: stiffness and Poisson’s ratio tunable anisotropy, large degree of shape recoverability, multistability, and even reversible auxeticity whereby the metamaterial switches Poisson’s ratio sign during deformation. The findings here reported underscore the scalable and multifunctional nature of origami designs, and pave the way toward harnessing the power of origami engineering at small scales.

Lin, Zhaowen↗

DOE OSTI2022

Thermal conductivity evaluation of ion irradiated Si 3 N 4 and ZrN ceramics using spatial domain thermoreflectance

Nitride ceramics have been investigated for different applications in the nuclear industry, such as space nuclear power, fusion reactor diagnostics and plasma heating, inert matrix fuels, and accident tolerant fuels. Although thermal conductivity remains one of the most important properties to track following irradiation, traditional techniques such as laser flash and xenon flash are limited to bulk sample characterization, which requires lengthy and cost-consuming neutron irradiation. This work used spatial domain thermoreflectance (SDTR) for the micrometer-scale measurement of thermal conductivity in 15 MeV Ni ion-irradiated silicon nitride and zirconium nitride from 1 to 50 dpa and 300 to 700 °C. Here, the SDTR-measured unirradiated thermal conductivity was found to be consistent with the published data on bulk samples. Electrically conductive ZrN exhibits modest reduction after irradiation which is minimal at the highest irradiation temperatures. In electrically insulating Si 3 N 4 , the reduction is more significant and unlike ZrN, the reduction remains significant even at a higher irradiation temperature. The thermal resistance evolution following irradiation was compared with lattice swelling, which was determined using grazing incidence x-ray diffraction, and radiation-induced defects were observed using transmission electron microscopy. A saturation value was observed between 15 and 50 dpa for thermal conductivity degradation in both nitride ceramics and a direct correlation with high-temperature defect recombination was observed, as well as the potential presence of additional carrier scattering mechanisms.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Accelerating the rate of discovery: toward high-repetition-rate HED science

As high-intensity short-pulse lasers that can operate at high-repetition-rate (HRR) (>10 H z ) come online around the world, the high energy density (HED) science they enable will experience a radical paradigm shift. The >10 3 increase in shot rate over today's shot-per-hour drivers translates into dramatically faster data acquisition, more experiments, and the ability to exploit machine learning, and thus the potential to significantly accelerate the advancement of HED science. A wide range of HED experiments, from opacity investigations to secondary source generation to plasma nuclear physics, will benefit from the increased statistics, precision, and exploration of phase space. Besides increasing the rate at which scientific experiments can be performed, HRR also allows for the rapid delivery of optimal experiments supported by simulations and modeling augmented by close coupling to empirical data. To fully realize such an HRR framework, numerous subsystems must be developed and brought together, including feedback laser control loops, high-throughput targetry and diagnostics, cognitive simulation, enhanced HED codes, and advanced data analytics. This paper describes the vision for an integrated HRR laser experimental HED system and outlines some of the major considerations and challenges for realizing it.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Dark matter clumps as sources of gravitational-wave glitches in LIGO-Virgo-KAGRA data

We consider the hypothetical possibility that nonstationary glitch features in the noise of ground-based gravitational-wave detectors could be produced by small dark matter clumps that pass through the earth in the vicinity of gravitational-wave detectors. Here, we first derive the gravitational-wave strain that would be generated by the passage of such a dark matter clump. We find that the strain is primarily sourced by the Newtonian gravitational acceleration of the mirrors toward the clump and by the Shapiro time delay of the photons in the laser beams as they pass through the gravitational potential created by the dark matter clump. We also find that the Newtonian acceleration effect dominates the gravitational-wave strain for both ground and space-based interferometers. We then compare our dark matter clump, gravitational-wave strain model to 84 Koi-Fish glitches detected during the second observing run of the LIGO/Virgo/KAGRA Collaboration through a Markov chain Monte Carlo Bayesian analysis. We find that all glitches but nine can be confidently rejected as having originated from dark matter clumps. For the remaining glitches, the dark matter hypothesis cannot be excluded, and the maximum a posteriori parameters yield minimum densities of about 10 −7 g⁡/cm 3 , within the model. These results allow us to place the first direct upper limits with gravitational-wave detectors on the local over-density of dark matter in the form of clumps in the local neighborhood of Earth, namely 𝜌 DM ⁢clumps ≲ 10 −15 g⁡/cm −3 .

Astronomy and AstroPhysics↗

DOE OSTI2022

HP-PdF2-type FeCl2 as a potential Cl-carrier in the deep Earth

Here, we report for the first time the formation of a HP-PdF 2 -type FeCl 2 phase (space group Pa$\bar{3}$), through high pressure-temperature (P-T) reactions in the hydrous systems (Mg 0.6 Fe 0.4 )SiO 3 –H 2 O–NaCl and FeO2H–NaCl in a laser-heated diamond-anvil cell up to 108 GPa and 2000 K. Applying single-crystal X-ray diffraction (XRD) analysis to individual submicrometer-sized grains, we have successfully determined the crystal structure of the as-synthesized FeCl 2 phase, in agreement with our theoretical structure search results. In situ high P-T XRD data revealed the substitution of Cl for OH(O) in such a cubic Pa$\bar{3}$ structure, demonstrating that this topology is a potential host for both H and Cl in the deep Earth. The chemical analysis of the recovered sample showed that the post-perovskite phase contains considerable amounts of Na 2 O and Fe 2 O 3 . The coexistence of the cubic FeCl 2 phase and post-perovskite suggests that the lowermost mantle could be a potential reservoir of Cl. The possible presence of volatiles such as H and Cl in the deep lower mantle would impact the composition and iron valence state of the post-perovskite phase.

58 GEOSCIENCES↗

DOE OSTI2022

Review: Real-space analyses of local dynamics in liquid using X-ray scattering

In this review, we advocate describing the liquid dynamics using the Van Hove correlation function, a temporal and spatial correlation function. Recent progress in X-ray optics and X-ray sources makes it possible to carry out inelastic and quasi-elastic x-ray scattering whose spectra can be converted into the dynamic correlation function in real space. We describe the basic concept of the Van Hove correlation function, how it is obtained from the X-ray scattering spectra using synchrotron X-rays and X-ray free electron lasers, and the atomic dynamics in water and aqueous salt solution.

Shinohara, Yuya↗

DOE OSTI2020

Extreme ultraviolet time- and angle-resolved photoemission setup with 21.5 meV resolution using high-order harmonic generation from a turn-key Yb:KGW amplifier

Characterizing and controlling electronic properties of quantum materials require direct measurements of nonequilibrium electronic band structures over large regions of momentum space. Here, we demonstrate an experimental apparatus for time- and angle-resolved photoemission spectroscopy using high-order harmonic probe pulses generated by a robust, moderately high power (20 W) Yb:KGW amplifier with a tunable repetition rate between 50 and 150 kHz. By driving high-order harmonic generation (HHG) with the second harmonic of the fundamental 1025 nm laser pulses, we show that single-harmonic probe pulses at 21.8 eV photon energy can be effectively isolated without the use of a monochromator. The on-target photon flux can reach 5 × 1010 photons/s at 50 kHz, and the time resolution is measured to be 320 fs. The relatively long pulse duration of the Yb-driven HHG source allows us to reach an excellent energy resolution of 21.5 meV, which is achieved by suppressing the space-charge broadening using a low photon flux of 1.5 × 108 photons/s at a higher repetition rate of 150 kHz. The capabilities of the setup are demonstrated through measurements in the topological semimetal ZrSiS and the topological insulator Sb2−xGdxTe3.

Liu, Yangyang↗

DOE OSTI2026

Measurement of the QE Map

113 MHz SRF gun utilized CsK 2 Sb and Na 2 KSb cathodes, which were irradiated with a pulsed green laser with a wavelength of 0.53 microns. The drive laser generated 78 kHz pulses with an acousto-optic modulator selecting the desired number of pulses reaching the cathode. The operator can select the aperture size, defining the laser spot diameter on the cathode, and the power level, which is controlled by a rotating polarizer. The laser power reaching the cathode can be measured with a meter based on a photodiode. The quantum efficiency (QE) of a photocathode serves as a primary indicator of its state. Small QE renders the cathode unusable when the desired bunch charge cannot be achieved. Strong variations in the quantum efficiency on the cathode surface might lead to the growth of the beam emittance due to the space charge effects. We have created a routine to measure the distribution of the QE on the cathode. The operator selects the aperture size, the central spot location, and the scan ranges for both planes. The scan starts from the central spots and proceeds along a spiral-like trajectory, making N rounds. The number of rounds can be chosen, and the total number of measured points is (2N+1) 2 . The laser spot movement is shown in Fig. 1.

43 PARTICLE ACCELERATORS↗

DOE OSTI2024

Thermo-Mechanical Modeling and Evaluation of the Cracking Response of Additively Manufactured Monolithic SiC Lattice Structures Subjected to Laser Heating

Increasing operating temperatures of solar receivers is paramount to the efficiency of concentrated solar thermal (CST) and solar power (CSP) systems. Owing to its high temperature stability combined with excellent thermal and optical properties, SiC has been the material of choice for application in high-temperature solar receivers. The state-of-the-art SiC volumetric concentrating solar air receivers such as honeycomb design have been demonstrated in field tests to achieve exit air temperatures approaching 800oC. However, successful application of CST systems for decarbonization requires significant increase in temperature capability of SiC receiver technology. Supported by an award from the Solar Technology Office (SETO), US Department of Energy (DOE), GE Research in collaboration with Heliogen Holdings Inc, is engaged in the development of ultra-High Operating Temperature SiC-matrix Solar Thermal Air Receiver (HOTSSTAR) enabled by additive manufacturing. The program objective is to design and to demonstrate a techno-economically viable SiC air receiver technology to achieve exit air temperature of 1100oC for CST applications. This report summarizes the learnings of a computational study on additively manufactured SiC lattice structures subjected to laser heating. The results from this study aim to help guide the design of a SiC receiver through a better understanding of lattice structure geometric parameters and their implications on the cracking response of the structure. In the study, a heat flux was applied to the surface of a 2”-diameter cylindrical lattice structure to simulate a 4kW CO2 laser. The resulting temperature distribution was applied to a structural model to approximate the stress distribution within the lattice structure and a Weibull analysis was performed to gain insight into the probability of failure and to evaluate the cracking response of the structure. With this approach, the influence of lattice density on temperature, stress, and probability of failure was explored for two different lattice beam spacings. A discussion on modeling assumptions, a comparison with experimental results, and an evaluation of the lattice cracking response is provided.

14 SOLAR ENERGY↗