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Zhu, Diling

Publications and source records attributed to Zhu, Diling.

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Broadband hard X-ray attosecond pulses from extremely chirped electron beams

Attosecond pulses from free-electron lasers have opened the doors to atomic site-specific studies of bound electronic dynamics on their natural, sub-femtosecond timescales. Key to their success has been electron beam shaping techniques enabling the generation of sub-femtosecond current spikes with peak currents on the order of 10 kA. We demonstrate in an RF linac the generation of current spikes with extreme chirps on the order of 350 MeV/micron, directly competitive with the chirps expected from beam-driven plasma wakefield accelerators. Leveraging chirp-taper compensation, we use these highly chirped beams to generate hard X-ray attosecond pulses with bandwidths exceeding 30 eV, a factor of two beyond previous demonstrations. We simultaneously present the first explicit experimental evidence of chirp-taper compensation in an attosecond XFEL, finding that optimal tapering improves the bandwidth and pulse energy by factors of two and five, respectively, for our conditions. In addition to the immediate utility of such broadband hard X-ray pulses, electron beams with such extreme chirps can be utilized for unique new experimental modalities by performing further compression after the undulators. Such post-lasing compression can enable subsequent superradiant light emission at longer wavelengths, or direct excitation of quantum systems with the beam's intense space-charge field for unique attosecond pump-probe possibilities.

43 PARTICLE ACCELERATORS↗
DOE OSTI2025

Second-order microscopic nonlinear susceptibility in a centrosymmetric material: application to imaging valence electron motion

We report measurements of phase-matched nonlinear x-ray and optical sum-frequency generation from single-crystal silicon using sub-resonant 0.95 eV laser pulses and 9.5 keV hard x-ray pulses from the LCLS free-electron laser. The sum-frequency signal appears as energy and momentum sidebands to the elastic Bragg peak. It is proportional to the magnitude squared of the relevant temporal and spatial Fourier components of the optically induced microscopic charges/currents. We measure the first- and second-order sideband to the 220 Bragg peak and find that the efficiency is maximized when the applied field is along the reciprocal lattice vector. For an optical intensity of $\sim10^{12} \text{W}/\text{cm}^2$, we measure peak efficiencies of $3\times 10^{-7}$ and $3\times 10^{-10}$ for the first and second-order sideband respectively (relative to the elastic Bragg peak). The first-order sideband is consistent with induced microscopic currents along the applied electric field (consistent with an isotropic response). The second-order sideband depends nontrivially on the optical field orientation and is consistent with an anisotropic response originating from induced charges along the bonds with C$_{3v}$ site symmetry. The results agree well with first-principles Bloch-Floquet calculations.

FOS: Physical sciences↗
DOE OSTI2024

Dynamically patterning x-ray beam by a femtosecond optical laser

Modern science and technology have greatly benefitted from our ability to precisely manipulate light waves, in both their spatial and temporal degrees of freedom. In the x-ray region, however, spatial control has been virtually static mainly due to stringent requirements for realizing high-performance optical elements. The lack of dynamic spatial control of x-ray beam has prevented researchers from realizing more sophisticated use of the wave field, which has rapidly advanced in the optical region in the past decades. In this study, we propose a practical scheme to dynamically control local x-ray reflectivity of a perfect silicon crystal by a femtosecond optical laser and demonstrate a programmable spatial x-ray modulator. Our modulator aims for spatial manipulation of the x-ray amplitude and is shown to produce arbitrary grayscale patterns with spatial frequencies up to 25 per millimeter. The proposed modulation scheme opens up a platform to enable advanced x-ray sensing and imaging techniques that can fully harness the wave nature of x-rays.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

X-ray diagnostics for the cavity-based x-ray free-electron laser project

The success of x-ray free-electron lasers (XFELs) in recent years has greatly advanced many scientific fields. However, most of these XFELs suffer from a low longitudinal coherence and instabilities due to the stochastic start-up process. A cavity-based x-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent and stable x-ray sources. One of the challenges of a CBXFEL is the requirement for the μ⁢m−sized electron bunches to fully overlap in three dimensions with the circulating μ⁢m−sized x-ray pulses in an x-ray cavity tens or hundreds of meters long. We present here the development of an x-ray diagnostics system for accurate alignment of x-ray beams in the CBXFEL cavity. The system was developed within the framework of a CBXFEL research and development collaboration among Argonne National Laboratory, SLAC National Accelerator Laboratory, and Spring-8. All the designed diagnostic components have been fully characterized at the Advanced Photon Source to demonstrate a capability for sub-μ⁢rad angular and μ⁢m spatial alignment of the CBXFEL cavity.

Free-electron lasers↗
DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2024

Non-equilibrium pathways to emergent polar supertextures

Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understand these phenomena. Here, in this work, we utilize single-shot optical pump–X-ray probe measurements to capture snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, an initially heterogeneous mixture of polar phase disorders within a few picoseconds, leading to a state composed of disordered ferroelectric and suppressed vortex orders. On the picosecond–nanosecond timescales, transient labyrinthine fluctuations develop, accompanied by the recovery of the vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single vortex supercrystal phase. Our results, corroborated by dynamical phase-field modelling, reveal non-equilibrium pathways following the ultrafast excitation of designer systems to persistent metastability.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Dynamical decoding of the competition between charge density waves in a kagome superconductor

The kagome superconductor CsV 3 Sb 5 hosts a variety of charge density wave (CDW) phases, which play a fundamental role in the formation of other exotic electronic instabilities. However, identifying the precise structure of these CDW phases and their intricate relationships remain the subject of intense debate, due to the lack of static probes that can distinguish the CDW phases with identical spatial periodicity. Here, we unveil the competition between two coexisting 2×2×2 CDWs in CsV 3 Sb 5 harnessing time-resolved X-ray diffraction. By analyzing the light-induced changes in the intensity of CDW superlattice peaks, we demonstrate the presence of both phases, each displaying a significantly different amount of melting upon excitation. The anomalous light-induced sharpening of peak width further shows that the phase that is more resistant to photo-excitation exhibits an increase in domain size at the expense of the other, thereby showcasing a hallmark of phase competition. Our results not only shed light on the interplay between the multiple CDW phases in CsV 3 Sb 5 , but also establish a non-equilibrium framework for comprehending complex phase relationships that are challenging to disentangle using static techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

X-ray optics for the cavity-based X-ray free-electron laser

A cavity-based X-ray free-electron laser (CBXFEL) is a possible future direction in the development of fully coherent X-ray sources. CBXFELs consist of a low-emittance electron source, a magnet system with several undulators and chicanes, and an X-ray cavity. The X-ray cavity stores and circulates X-ray pulses for repeated FEL interactions with electron pulses until the FEL reaches saturation. CBXFEL cavities require low-loss wavefront-preserving optical components: near-100%-reflectivity X-ray diamond Bragg-reflecting crystals, outcoupling devices such as thin diamond membranes or X-ray gratings, and aberration-free focusing elements. In the framework of the collaborative CBXFEL research and development project of Argonne National Laboratory, SLAC National Accelerator Laboratory and SPring-8, we report here the design, manufacturing and characterization of X-ray optical components for the CBXFEL cavity, which include high-reflectivity diamond crystal mirrors, a diamond drumhead crystal with thin membranes, beryllium refractive lenses and channel-cut Si monochromators. All the designed optical components have been fully characterized at the Advanced Photon Source to demonstrate their suitability for the CBXFEL cavity application.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Critical slowing of the spin and charge density wave order in thin film Cr following photoexcitation

We report on the evolution of the charge density wave (CDW) and spin density wave (SDW) orders of a chromium film following photoexcitation with an ultrafast optical laser pulse. The CDW is measured by ultrafast time-resolved x-ray diffraction of the CDW satellite that tracks the suppression and recovery of the CDW following photoexcitation. We find that as the temperature of the film approaches a discontinuous phase transition in the CDW and SDW orders, the time scales of recovery increase exponentially from the expected thermal time scales. We extend a Landau model for SDW systems to account for this critical slowing with the appropriate boundary conditions imposed by the geometry of the thin film system. This model allows us to assess the energy barrier between the available CDW/SDW states with different spatial periodicities.

36 MATERIALS SCIENCE↗
DOE OSTI2024

A versatile pressure-cell design for studying ultrafast molecular-dynamics in supercritical fluids using coherent multi-pulse x-ray scattering

Supercritical fluids (SCFs) can be found in a variety of environmental and industrial processes. They exhibit an anomalous thermodynamic behavior, which originates from their fluctuating heterogeneous micro-structure. Characterizing the dynamics of these fluids at high temperature and high pressure with nanometer spatial and picosecond temporal resolution has been very challenging. The advent of hard x-ray free electron lasers has enabled the development of novel multi-pulse ultrafast x-ray scattering techniques, such as x-ray photon correlation spectroscopy (XPCS) and x-ray pump x-ray probe (XPXP). These techniques offer new opportunities for resolving the ultrafast microscopic behavior in SCFs at unprecedented spatiotemporal resolution, unraveling the dynamics of their micro-structure. However, harnessing these capabilities requires a bespoke high-pressure and high-temperature sample system that is optimized to maximize signal intensity and address instrument-specific challenges, such as drift in beamline components, x-ray scattering background, and multi-x-ray-beam overlap. We present a pressure cell compatible with a wide range of SCFs with built-in optical access for XPCS and XPXP and discuss critical aspects of the pressure cell design, with a particular focus on the design optimization for XPCS.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Single-shot X-ray absorption spectroscopy at X-ray free electron lasers

X-ray Absorption Spectroscopy (XAS) is a widely used X-ray diagnostic method for studying electronic and structural properties of matter. At first glance, the relatively narrow bandwidth and the highly fluctuating spectral structure of X-ray Free Electron Lasers (XFEL) sources seem to require accumulation over many shots to achieve high data quality. To date the best approach to implementing XAS at XFEL facilities has been using monochromators to scan the photon energy across the desired spectral range. While this is possible for easily reproducible samples such as liquids, it is incompatible with many important systems. Here, we demonstrate collection of single-shot XAS spectra over 10s of eV using an XFEL source, with error bars of only a few percent. We additionally show how to extend this technique over wider spectral ranges towards Extended X-ray Absorption Fine Structure measurements, by concatenating a few tens of single-shot measurements. Our results pave the way for future XAS studies at XFELs, in particular those in the femtosecond regime. This advance is envisioned to be especially important for many transient processes that can only be initiated at lower repetition rates, for difficult to reproduce excitation conditions, or for rare samples, such as those encountered in high-energy density physics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Nonthermal Bonding Origin of a Novel Photoexcited Lattice Instability in SnSe

Lattice dynamics measurements are often crucial tools for understanding how materials transform between different structures. Here, we report time-resolved x-ray scattering-based measurements of the nonequilibrium lattice dynamics in SnSe, a monochalcogenide reported to host a novel photoinduced lattice instability. By fitting interatomic force models to the fluence dependent excited-state dispersion, we determine the nonthermal origin of the lattice instability to be dominated by changes of interatomic interactions along a bilayer-connecting bond, rather than of an intralayer bonding network that is of primary importance to the lattice instability in thermal equilibrium.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Low-loss stable storage of 1.2 Å X-ray pulses in a 14 m Bragg cavity

Here, we present an experimental demonstration of a stable, low-loss, large X-ray cavity operating at 1.2 Å wavelength. The cavity consists of four separate high-reflectivity single crystal diamond Bragg mirrors arranged in a rectangular configuration with a round-trip distance of 14.2 m. Femtosecond X-ray pulses from an X-ray free-electron laser were coupled into the cavity via a transmission phase grating. We show that a stable mode can be maintained with the introduction of cavity focusing and measure round-trip efficiencies approaching 88%, or >96% when excluding grating and lens losses, close to the Bragg mirror theoretical performance limit. The direct observation of sustained stable X-ray circulation provides the most direct evidence to date that cavity-based X-ray free-electron lasers and other cavity-based hard X-ray systems are feasible.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Ultrafast X-Ray Scattering Reveals Composite Amplitude Collective Mode in the Weyl Charge Density Wave Material ( TaSe 4 ) 2 I

Here we report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe 4 ) 2⁢ I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz amplitude mode derived primarily from a transverse acoustic mode of the high-symmetry structure. From our measurements we determine that this mode interacts with the valence charge indirectly through another collective mode, and that the CDW system in (TaSe 4 ) 2 ⁢I has a composite nature supporting multiple dynamically active structural degrees of freedom.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy

Abstract Femtosecond pump-probe spectroscopy using ultrafast optical and infrared pulses has become an essential tool to discover and understand complex electronic and structural dynamics in solvated molecular, biological, and material systems. Here we report the experimental realization of an ultrafast two-color X-ray pump X-ray probe transient absorption experiment performed in solution. A 10 fs X-ray pump pulse creates a localized excitation by removing a 1 s electron from an Fe atom in solvated ferro- and ferricyanide complexes. Following the ensuing Auger–Meitner cascade, the second X-ray pulse probes the Fe 1 s → 3 p transitions in resultant novel core-excited electronic states. Careful comparison of the experimental spectra with theory, extracts +2 eV shifts in transition energies per valence hole, providing insight into correlated interactions of valence 3 d with 3 p and deeper-lying electrons. Such information is essential for accurate modeling and predictive synthesis of transition metal complexes relevant for applications ranging from catalysis to information storage technology. This study demonstrates the experimental realization of the scientific opportunities possible with the continued development of multicolor multi-pulse X-ray spectroscopy to study electronic correlations in complex condensed phase systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Experimental setup for high-resolution characterization of crystal optics for coherent X-ray beam applications

Stanford Synchrotron Radiation Lightsource serves a wide scientific community with its variety of X-ray capabilities. Recently, a wiggler X-ray source located at beamline 10-2 has been employed to perform high-resolution rocking curve imaging (RCI) of diamond and silicon crystals. X-ray RCI is invaluable for the development of upcoming cavity-based X-ray sources at SLAC, including the cavity-based X-ray free-electron laser and X-ray laser oscillator. In this paper, the RCI apparatus is described and experimental results are provided to validate its design. Future improvements of the setup are also discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Influence of local symmetry on lattice dynamics coupled to topological surface states

Herein we investigate coupled electron-lattice dynamics in the topological insulator Bi 2 Te 3 with time-resolved photoemission and time-resolved x-ray diffraction. It is well established that coherent phonons can be launched by optical excitation, but selection rules generally restrict these modes to zone-center wave vectors and Raman-active branches. We find that the topological surface state couples to additional modes, including a continuum of surface-projected bulk modes from both Raman and infrared branches, with possible contributions from surface-localized modes when they exist. Our calculations show that this surface vibrational spectrum occurs naturally as a consequence of the translational and inversion symmetries broken at the surface, without requiring the splitting-off of surface-localized phonon modes. The generality of this result suggests that coherent phonon spectra are useful by providing unique fingerprints for identifying surface states in more controversial materials. These effects may also expand the phase space for tailoring surface state wave functions via ultrafast optical excitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗