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DOE OSTI2024

Attosecond delays in X-ray molecular ionization

The photoelectric effect is not truly instantaneous, but exhibits attosecond delays that can reveal complex molecular dynamics. Sub-femtosecond duration light pulses provide the requisite tools to resolve the dynamics of photoionization. Accordingly, the past decade has produced a large volume of work on photoionization delays following single photon absorption of an extreme ultraviolet (XUV) photon. However, the measurement of time-resolved core-level photoionization remained out of reach. The required x-ray photon energies needed for core-level photoionization were not available with attosecond tabletop sources. We have now measured the x-ray photoemission delay of core-level electrons, and here report unexpectedly large delays, ranging up to 700 attoseconds in NO near the oxygen K-shell threshold. These measurements exploit attosecond soft x-ray pulses from a free-electron laser (XFEL) to scan across the entire region near the K-shell threshold. Furthermore, we find the delay spectrum is richly modulated, suggesting several contributions including transient trapping of the photoelectron due to shape resonances, collisions with the Auger-Meitner electron that is emitted in the rapid non-radiative relaxation of the molecule, and multi-electron scattering effects. Finally, the results demonstrate how x-ray attosecond experiments, supported by comprehensive theoretical modelling, can unravel the complex correlated dynamics of core-level photoionization.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Ultrafast Terahertz Field Control of the Emergent Magnetic and Electronic Interactions at Oxide Interfaces

Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.

X-ray spectroscopy and scattering↗

NASA NTRS2026

X-Ray Polarization of Z-Type Neutron Star Low-Mass X-Ray Binaries II. Spectropolarimetric Analysis

IXPE has provided for the first time detailed energy- and time-resolved X-ray polarimetry of Z-type neutron star low-mass X-ray binaries (NS-LMXBs) as they move along their color-color diagrams (CCDs). These sources can reach the highest polarization observed for NS-LXMBs in the 2–8 keV range when they move along the horizontal branch. In a previous paper, we characterized the spectral state of a sample of Z-sources using the CCD and estimated the polarization with model-independent analysis. Here, we present detailed spectropolarimetric analysis for each source on each branch using data from IXPE, NICER, and NuSTAR. The continuum X-ray emission of all the sources is well described with a combination of thermal accretion disk emission plus a harder Comptonized component. In addition, reflection features, in particular the relativistically broadened Fe Kα line, are observed for our sources, except GX 5–1. For most of the sources and branches, the main contribution to the X-ray emission and polarization is due to Comptonization: moving from the horizontal branch (HB) to the normal branch (NB), the polarization degree (PD) in the 2–8 keV band varies from about 6% to 3–4%, while the PD is loosely constrained in the flaring branch (FB), due to the shorter exposures. These PD values are significantly higher than theoretical expectations for typical spreading or boundary layer configurations. The polarization of the disk is generally lower (below 3%) but still higher than predictions for an electron scattering-dominated, plane-parallel atmosphere above the disk observed at the corresponding inclination. Moreover, the polarization angle (PA) of the disk seems to be significantly misaligned and not perpendicular to that of Comptonization. We find no correlation between the polarization signal and the inclination, nor with the contribution of reflected photons throughout the Z-track.

accretion↗

DOE OSTI2023

3D-printed sheet jet for stable megahertz liquid sample delivery at X-ray free-electron lasers

X-ray free-electron lasers (XFELs) can probe chemical and biological reactions as they unfold with unprecedented spatial and temporal resolution. A principal challenge in this pursuit involves the delivery of samples to the X-ray interaction point in such a way that produces data of the highest possible quality and with maximal efficiency. This is hampered by intrinsic constraints posed by the light source and operation within a beamline environment. For liquid samples, the solution typically involves some form of high-speed liquid jet, capable of keeping up with the rate of X-ray pulses. However, conventional jets are not ideal because of radiation-induced explosions of the jet, as well as their cylindrical geometry combined with the X-ray pointing instability of many beamlines which causes the interaction volume to differ for every pulse. This complicates data analysis and contributes to measurement errors. An alternative geometry is a liquid sheet jet which, with its constant thickness over large areas, eliminates the problems related to X-ray pointing. Since liquid sheets can be made very thin, the radiation-induced explosion is reduced, boosting their stability. These are especially attractive for experiments which benefit from small interaction volumes such as fluctuation X-ray scattering and several types of spectroscopy. Although their use has increased for soft X-ray applications in recent years, there has not yet been wide-scale adoption at XFELs. Here, gas-accelerated liquid sheet jet sample injection is demonstrated at the European XFEL SPB/SFX nano focus beamline. Its performance relative to a conventional liquid jet is evaluated and superior performance across several key factors has been found. This includes a thickness profile ranging from hundreds of nanometres to 60 nm, a fourfold increase in background stability and favorable radiation-induced explosion dynamics at high repetition rates up to 1.13 MHz. Its minute thickness also suggests that ultrafast single-particle solution scattering is a possibility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Experimental characterization of hot-electron emission and shock dynamics in the context of the shock ignition approach to inertial confinement fusion

We report on planar target experiments conducted on the OMEGA-EP laser facility performed in the context of the shock ignition (SI) approach to inertial confinement fusion. The experiment aimed at characterizing the propagation of strong shock in matter and the generation of hot electrons (HEs), with laser parameters relevant to SI (1-ns UV laser beams with I ~10 16 W/cm 2 ). Time-resolved radiographs of the propagating shock front were performed in order to study the hydrodynamic evolution. The hot-electron source was characterized in terms of Maxwellian temperature, T h , and laser to hot-electron energy conversion efficiency η using data from different x-ray spectrometers. The post-processing of these data gives a range of the possible values for T h and η [i.e., T h [keV] ϵ (20, 50) and η ϵ (2%, 13%)]. These values are used as input in hydrodynamic simulations to reproduce the results obtained in radiographs, thus constraining the range for the HE measurements. According to this procedure, we found that the laser converts ~10% ± 4% of energy into hot electrons with T h = 27 ± 8 keV. The paper shows how the coupling of different diagnostics and numerical tools is required to sufficiently constrain the problem, solving the large ambiguity coming from the post-processing of spectrometers data. The effect of the hot electrons on the shock dynamics is then discussed, showing an increase in the pressure around the shock front. Furthermore, the low temperature found in this experiment without pre-compression laser pulses could be advantageous for the SI scheme, but the high conversion efficiency may lead to an increase in the shell adiabat, with detrimental effects on the implosion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Defect-Limited Mobility and Defect Thermochemistry in Mixed A-Cation Tin Perovskites: (CH3NH3)1-xCsxSnBr3

Hybrid organic-inorganic semiconductors crystallizing in the perovskite structure present a significant opportunity for realizing defect-tolerant semiconductors. In this work, we examine the solid solution, (CH3NH3)1-xCsxSnBr3, and identify the thermochemistry dictating the intrinsic carrier concentrations and how local structural distortions influences this electronic behavior. This family of compounds exhibits the expected systematic trend in decreasing optical gap with the cesium to methylammonium A-site mixing ratio, x, in the visible region. However, the carrier mobility, as determined from time-resolved microwave conductivity measurements, trends opposite to that expected from first-principles calculations combined with Boltzmann scattering theory calculations of the carrier mobility. We propose that this is a result of increasing carrier scattering with x in (CH3NH3)1-xCsxSnBr3 due to a significant increase in the carrier density with x. By examining the dependence of the carrier density as a function of x, we infer the compositional-dependence of the average enthalpy and nonconfigurational entropy per defect. While diffraction reveals a cubic aristotypic perovskite structure as a function of x at room temperature, the pair distribution functions obtained from synchrotron X-ray total scattering from these materials are better described by symmetry-adapted displacement modes of the Pm3m crystal structure, which we attribute to a large degree of anharmonic dynamics of the atom positions. This analysis shows that CH3NH3+-rich compositions retain mostly linear Sn-Br-Sn bonding environments through the displacements, while Cs+-rich compositions lead to more significantly bent Sn-Br-Sn environments. We propose that these bent bonding arrangements in Cs-rich compositions yield a higher propensity for defect formation. This also provides a rationale for carrier trapping that gives rise to anomalous microwave transients. Together, these results provide insight into the structure-dynamics-properties relationships in this highly anharmonic system with high amplitude atomic motions and low defect formation energies.

defect thermochemistry↗

DOE OSTI2022

Structural measurement of electron-phonon coupling and electronic thermal transport across a metal-semiconductor interface

Scattering of energetic charge carriers and their coupling to lattice vibrations (phonons) in dielectric materials and semiconductors are crucial processes that determine the functional limits of optoelectronics, photovoltaics, and photocatalysts. The strength of these energy exchanges is often described by the electron-phonon coupling coefficient, which is difficult to measure due to the microscopic time- and length-scales involved. In the present study, we propose an alternate means to quantify the coupling parameter along with thermal boundary resistance and electron conductivity by performing a high angular-resolution time-resolved X-ray diffraction measurement of propagating lattice deformation following laser excitation of a nanoscale, polycrystalline metal film on a semiconductor substrate. Our data present direct experimental evidence for identifying the ballistic and diffusive transport components occurring at the interface, where only the latter participates in thermal diffusion. This approach provides a robust measurement that can be applied to investigate microscopic energy transport in various solid-state materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Three-step colloidal gelation revealed by time-resolved x-ray photon correlation spectroscopy

The gelation of PEGylated gold nanoparticles dispersed in a glycerol–water mixture is probed in situ by x-ray photon correlation spectroscopy. Following the evolution of structure and dynamics over 10 4 s, a three-step gelation process is found. First, a simultaneous increase of the Ornstein–Zernike length ξ and slowdown of dynamics is characterized by an anomalous q-dependence of the relaxation times of τ ∝q -6 and strongly stretched intermediate scattering functions. After the structure of the gel network has been established, evidenced by a constant ξ, the dynamics show aging during the second gelation step accompanied by a change toward ballistic dynamics with τ ∝ q -1 and compressed correlation functions. In the third step, aging continues after the arrest of particle motion. Our observations further suggest that gelation is characterized by stress release as evidenced by anisotropic dynamics once gelation sets in.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

A novel integrated time-resolved array avalanche photodiode detection system for nuclear resonant scattering measurements

Here, the nuclear resonant scattering (NRS) experiment requires photon-counting detectors with high time resolution, short dead time, large dynamic range, low noise, and large detection area. An 8-channel avalanche photodiode (APD) array detector system with high integrity, flexibility, and reliability has been developed to adapt to the demands of NRS experiments. The detector system mainly consists of four key parts: (i) an array-APD sensor, (ii) 8-channel integrated fast preamplifiers, (iii) the time-to-digital converter readout electronics, and (iv) a data acquisition system and EPICS support software. Remarkably, the system exhibits a time resolution of better than 500 ps and has a sufficiently low noise level, allowing for the lowest detection energy threshold of 4 keV. The performance of the new array-APD system as well as its real application in nuclear forward scattering (NFS) and nuclear resonant inelastic x-ray scattering (NRIXS) experiments was tested in two synchrotron facilities. With the new system, the NFS signal very close to the prompt electronic scattering signal can be extracted. Thanks to the customized EPICS-areaDetector-based control software, NRIXS spectra can be readily measured with time and energy information of the NRIXS signal stored in the raw data, which is promising for developing NRIXS data analysis in the time domain. The array-APD detector can be deployed for nuclear resonant scattering experiments at various synchrotron radiation facilities.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

RNA structures and dynamics with Å resolution revealed by x-ray free-electron lasers

RNA macromolecules, like proteins, fold to assume shapes that are intimately connected to their broadly recognized biological functions; however, because of their high charge and dynamic nature, RNA structures are far more challenging to determine. We introduce an approach that exploits the high brilliance of x-ray free-electron laser sources to reveal the formation and ready identification of angstrom-scale features in structured and unstructured RNAs. Previously unrecognized structural signatures of RNA secondary and tertiary structures are identified through wide-angle solution scattering experiments. With millisecond time resolution, we observe an RNA fold from a dynamically varying single strand through a base-paired intermediate to assume a triple-helix conformation. While the backbone orchestrates the folding, the final structure is locked in by base stacking. This method may help to rapidly characterize and identify structural elements in nucleic acids in both equilibrium and time-resolved experiments.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2021

Dynamic structural views in solar energy materials by femtosecond electron diffraction

Solar materials convert light into other forms of energy through excited state processes occurring on ultrafast time and atomic length scales. Understanding and controlling such nonequilibrium processes is essential for applications ranging from photovoltaics to photocatalysis. These processes are commonly studied by transient optical techniques, which resolve charge carrier dynamics. However, optical spectroscopy does not directly probe the atomic-scale motions that play a central role in the ultimate functionality of these materials. Filling this missing gap, ultrafast electron and x-ray scattering techniques enable monitoring of structural dynamics in materials with femtosecond time resolution. In this work, we focus on the use of ultrafast electron diffraction (UED) techniques to probe photoinduced energy conversion dynamics in solar energy materials. First, we discuss the use of UED as an ultrafast lattice thermometer allowing a direct probe of nonradiative relaxations such as hot carrier cooling and Auger recombination. Second, we present a time-resolved atomic pair distribution function analysis enabled by UED, which uncovers lattice deformations arising from excitation localization in materials. Finally, we provide an outlook looking toward new approaches for resolving in situ energy conversion dynamics and uncovering structure–property relationships in solar energy materials.

36 MATERIALS SCIENCE↗

DOE OSTI2022

LICS Modeling [Slides]

We propose to design a new diagnostic based on laser inverse Compton scattering (LICS) to study the dynamics of runaway electron formation during killer-pellet triggered disruptions in DIII-D, and their subsequent loss. Obtaining a better understanding of transient runaway electrons (and how to suppress them) is one of the highest priorities of the US fusion program. To enable this, we need better measurements of the runaway electron population during and after disruptions. We intend to measure point-wise time-resolved spatial profile and energy distributions of the runaway electrons while they are in the core of the tokamak plasma. While LICS measurements of relativistic e-beams have been successfully made on accelerators, they have never been done in a tokamak. We bring two innovations to this diagnostic concept which should enable 10 times better signal-to-noise ratios than previously envisioned. In particular, we will marry bright short pulse (10’s of picosecond) laser technologies with the availability of short-pulse gated x-ray imagers developed at Los Alamos for the National Ignition Facility (NIF), to reject noise generated by the tokamak and plasma environment. We will generate a Conceptual Physics Basis, a Preliminary Design, and a Final Design package, with associated DIII-D reviews, along with prototype component testing for the diagnostic over the course of the two year duration of this proposal.

42 ENGINEERING↗

DOE OSTI2026

Collaborative R&D with REEL Solar Inc (REEL) to Understand and Overcome Performance Limitations in CdTe Solar Cells: Cooperative Research and Development (Final Report)

This CRADA will focus on processing, advanced characterization, and testing of photovoltaic materials and devices to understand and improve REEL CdTe solar technology. This will include examining process variations and different buffer, absorber, and contact layers from REEL and NLR to maximize performance. The unique and diverse advanced characterization tools at NLR, such as time-resolved photoluminescence, capacitance-voltage measurements, electron beam scattered diffraction, cathodoluminescence, electron microscopy, TOF-SIMS, and other measurements will be applied to characterize REEL processing to improve understanding and guide experimental directions. Accelerated stability and potential induced degradation tests will be used to analyze metastability, short-and-long term degradation, and improve bankability. A second and major thrust this period will be joint development of Si/CdTe tandem solar cells to overcome industry wide terrestrial solar efficiency limits with the two lowest cost and manufacturable solar materials today. This will include developing novel transparent back contacts that can be incorporated into tandem structures and other novel solar applications, detailed analysis of designs and configurations for CdTe/Si tandem modules, and prototyping REEL CdTe Technology with Si bottom cells in tandem structures.

14 SOLAR ENERGY↗