Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “ultrafast electron diffraction”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

65 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Attosecond Transient Grating Spectroscopy with Near-Infrared Grating Pulses and an Extreme Ultraviolet Diffracted Probe

Transient grating spectroscopy has become a mainstay among metal and semiconductor characterization techniques. Here, we extend the technique toward the shortest achievable time scales by using tabletop high-harmonic generation of attosecond extreme ultraviolet (XUV) pulses that diffract from transient gratings generated with sub-5 fs near-infrared (NIR) pulses. We demonstrate the power of attosecond transient grating spectroscopy (ATGS) by investigating the ultrafast photoexcited dynamics in an Sb semimetal thin film. ATGS provides an element-specific, background-free signal unfettered by spectral congestion, in contrast to transient absorption spectroscopy. With ATGS measurements in Sb polycrystalline thin films, we observe the generation of coherent phonons and investigate the lattice and carrier dynamics. Among the latter processes, we extract carrier thermalization, hot carrier cooling, and electron-hole recombination, which are on the order of 20 fs, 50 fs, and 2 ps time scales, respectively. Furthermore, the simultaneous collection of transient absorption and transient grating data allows us to extract the total complex dielectric constant in the sample dynamics with a single measurement, including the real-valued refractive index, from which we are also able to investigate carrier-phonon interactions and longer-lived phonon dynamics. The outlined experimental technique expands the capabilities of transient grating spectroscopy and attosecond spectroscopies by providing a wealth of information concerning carrier and lattice dynamics with an element-selective technique at the shortest achievable time scales.

Quintero-Bermudez, Rafael↗
DOE OSTI2025

Long-lived photoinduced polar states in metal halide perovskites

Ferroic polarization in hybrid perovskites is crucial for enhancing photovoltaic performance and developing potential electronic applications. Controlling ferroic polarization with an optical field enables probing of ferroic polarization without the unwanted interface ionic effects caused by electronic contacts. This study employs ultrafast near-infrared photoexcitation to control dynamic structural transitions in soft single crystalline hybrid Cu (II) halide perovskites, achieving a long-lived polar state (beyond 104 s) at room temperature. We probe reversible long-lived polar domains under near-infrared photoexcitation using in-situ second harmonic generation microscopy. Theoretical calculation informs the polar lattice microstrain likely induced by anisotropic structure deformation in octahedral copper halide under near-infrared photoexcitation. The reversible slow structure deformation is further confirmed by in-situ photo-induced X-ray diffraction measurement. This work provides a material platform for understanding, controlling, and probing polarization under photoexcitation. Our methodology enables the identification of previously undiscovered polar phases in ferroelectric halide perovskites.

Dou, Yixuan↗
DOE OSTI2025

A Flat Analyzer Polycapillary Spectrometer for X-ray Absorption Spectroscopy of Dilute Transition Metals at X-ray-Free Electron Lasers

X-ray absorption spectroscopy (XAS) coupled with highly intense pulses from an X-ray-free electron laser (XFEL) can be used to track ultrafast chemical dynamics. Nonetheless, measurements for dilute samples (≤1 mM) have been exceptionally challenging, as scattering background signals dominate over the sample’s X-ray fluorescence. We show that femtosecond time-resolved XAS measurements of sub-millimolar transition metal solutions are now possible at the Linac Coherent Light Source (LCLS) using a high-throughput polycapillary XAS spectrometer, designed, developed, and commissioned at LCLS and the Stanford Synchrotron Radiation Lightsource (SSRL). The instrument integrates three polycapillary optics that collect and collimate X-ray fluorescence emitted from the interaction point with a high solid angle. X-ray collimated fluorescence is then selectively diffracted by coupled graphite analyzer crystals. As a result, the contribution of scattered photons is suppressed. Experiments at the Pt L 3 -edge on 0.1 mM aqueous K 2 PtCl 6 (delivered via a 100 μm liquid jet) were successfully performed in the laser pump X-ray probe configuration at the LCLS XCS and XPP instruments. We report the transient spectra of hexachloroplatinate within the first 10 ps after a 266 nm photoexcitation. We observed a short-lived reduced intermediate (≈2 ps). The polycapillary X-ray spectrometer at LCLS now enables the efficient study of the dynamics of ultradilute transition metals in solution. This capability opens the door to investigating plasmonic systems, photocatalysts, enzymes, and other scarce and dilute samples.

LCLS↗
DOE OSTI2026

Demonstration of a diamond anvil cell platform at the Linac Coherent Light Source: Capabilities and Outlook

A novel x-ray free electron laser (XFEL) diffraction setup for use with diamond anvil cells (DACs) at the Linac Coherent Light Source (LCLS) is described. Using the new diamond window at the Matter at Extreme Conditions (MEC) instrument, it allows hard x-ray experiments on DACs to be performed in air. The platform is described along with alignment and calibration procedures and details of the x-ray beam and diagnostics. Example data are presented, including a reversible XFEL induced phase transition in CsPbI3. The DAC setup was commissioned at MEC, but is applicable to most LCLS instruments where the unique pulse structures available at LCLS offer access to new ultrafast experimental techniques at high pressure.

Diamond Anvil Cells, LCLS, XFEL, High-Pressure↗
DOE OSTI2025

Single-shot spatiotemporal plasma density measurements with a chirped probe pulse

In this work, we present the development and demonstration of a diagnostic for the measurement of the spatial and temporal evolution of plasma density in a single shot. Single-shot Advanced Plasma Probe HolographIc REconstruction (SAPPHIRE) utilizes a chirped probe pulse, a diffractive optical element, a self-referenced interferometer, and an interference bandpass filter to achieve high-fidelity electron density measurements suitable for underdense plasmas that exhibit cylindrical symmetry. The method overcomes limitations in conventional diagnostics, such as reliance on shot-to-shot reproducibility, while capturing plasma dynamics on picosecond timescales with micron-level spatial resolution. The capabilities of SAPPHIRE are demonstrated through measurements of laser-driven plasma channels in helium–nitrogen gas jets. SAPPHIRE demonstrates the formation and expansion of plasma channels in a single shot and the propagation of supersonic ionization fronts while revealing shot-to-shot variations in the plasma profiles. Experimental results are validated against theoretical models and scaling laws, underscoring the robustness and accuracy of this technique. By enabling ultrafast, high-resolution plasma diagnostics in a single exposure, SAPPHIRE represents a transformative advancement in plasma measurement technology.

Grace, Elizabeth S. [Lawrence Livermore National L↗
DOE OSTI2025

Growth and characterization of high-quality Zr doped AlN epilayers

AlN stands out for its remarkable figures of merit for electronic and photonic devices, attributed to its ultrawide bandgap of ∼6.1 eV and an exceptionally high critical field of ∼15 MV/cm. More recently, zirconium (Zr) doped AlN (AlN:Zr) has also been identified as a promising material platform for the exploration of solid-state qubits for quantum information and technology, high performance piezoelectric acoustic wave resonators, and optically triggered ultrafast power switching devices facilitated by optically activating Zr related impurities. Despite the significant potential, the ability for producing AlN:Zr epitaxial structures has yet to be established. In this study, we have achieved AlN:Zr epilayers with a high Zr doping level [NZr] of up to 1020 cm−3 using industrial standard metal-organic chemical vapor deposition growth technique. High crystalline quality of AlN:Zr was confirmed by x-ray diffraction, revealing a narrow full width at half maximum of the (002) rocking curve at 216 arcsec for 1.8 μm thick epilayers deposited on sapphire at [NZr]=1020 cm−3. Zr doping was observed to slightly increase the c-lattice constant to 4.992 Å for AlN:Zr (at [NZr]=1020 cm−3) compared to 4.980 Å for undoped AlN. X-ray photoelectron spectroscopy measurement results verified the substitution of Zr at the Al site (ZrAl). The formation of (ZrAl–VN) complexes, which are predicted to possess all the desired properties required by quantum qubits, was confirmed through optical absorption studies. The realization of high-quality AlN:Zr epilayers significantly broadens the scope of technologically significant device applications for AlN.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Persistence of charge density wave fluctuations in the absence of long-range order in a hole-doped kagome metal

The kagome metals 𝐴⁢V 3 ⁢Sb 5 (𝐴=K, Rb, Cs) exhibit a complex interplay between charge density wave (CDW) order and superconductivity. Here, in this study, we use ultrafast coherent phonon spectroscopy to probe the evolution of CDW order in hole-doped CsV 3 ⁢Sb 5−𝑥 ⁢Sn 𝑥 across a broad range of compositions (0 ≤ 𝑥 ≤ 0.68). While thermodynamic and diffraction measurements show long-range CDW order vanishes above 𝑥 ≈ 0.05, we observe persistent signatures of CDW fluctuations up to the highest doping levels, with correlation times on the order of several picoseconds. These results indicate the presence of a robust fluctuating charge order that survives well beyond the established CDW phase boundary. Furthermore, these fluctuations are enhanced near a doping-tuned quantum phase transition at 𝑥* ≈ 0.15, which coincides with a local minimum in the superconducting 𝑇 c double-dome. Additional measurements on Ti- and K-substituted samples confirm that this behavior is intrinsic to hole doping and not tied to disorder. Overall, our findings suggest that CDW fluctuations play a central role in the electronic phase diagram of 𝐴⁢V 3 ⁢Sb 5 and may mediate or compete with superconductivity.

Kongruengkit, Terawit [Univ. of California, Santa ↗
DOE OSTI2025

Scalable 3D reconstruction for X-ray single particle imaging with online machine learning

X-ray free-electron lasers offer unique capabilities for measuring the structure and dynamics of biomolecules, helping us understand the basic building blocks of life. Notably, high-repetition-rate free-electron lasers enable single particle imaging, where individual, weakly scattering biomolecules are imaged under near-physiological conditions with the opportunity to access fleeting states that cannot be captured in cryogenic or crystallized conditions. Existing X-ray single particle reconstruction algorithms, which estimate the particle orientation for each image independently, are slow and memory-intensive when handling the massive datasets generated by emerging free-electron lasers. Here, we introduce X-RAI (X-Ray single particle imaging with Amortized Inference), an online reconstruction framework that estimates the structure of 3D macromolecules from large X-ray single particle datasets. X-RAI consists of a convolutional encoder, which amortizes pose estimation over large datasets, as well as a physics-based decoder, which employs an implicit neural representation to enable high-quality 3D reconstruction in an end-to-end, self-supervised manner. We demonstrate that X-RAI achieves state-of-the-art performance for small-scale datasets in simulation and challenging experimental settings and demonstrate its unprecedented ability to process large datasets containing millions of diffraction images in an online fashion. These abilities signify a paradigm shift in X-ray single particle imaging towards real-time reconstruction.

Computer science↗
DOE OSTI2025

Filling data analysis gaps in time-resolved crystallography by machine learning

There is a growing understanding of the structural dynamics of biological molecules fueled by x-ray crystallography experiments. Time-resolved serial femtosecond crystallography (TR-SFX) with x-ray Free Electron Lasers allows the measurement of ultrafast structural changes in proteins. Nevertheless, this technique comes with some limitations. One major challenge is the quality of data from TR-SFX measurements, which often faces issues like data sparsity, partial recording of Bragg reflections, timing errors, and pixel noise. To overcome these difficulties, conventionally, large volumes of data are collected and grouped into a few temporal bins. The data in each bin are then averaged and paired with the mean of their corresponding jittered timestamps. This procedure provides one structure per bin, resulting in a limited number of averaged structures for the entire time interval spanned by the experiment. Therefore, the information on ultrafast structural dynamics at high temporal resolution is lost. This has initiated research for advanced methods of analyzing experimental TR-SFX data beyond the standard binning and averaging method. To address this problem, we use a machine learning algorithm called Nonlinear Laplacian Spectral Analysis (NLSA), which has emerged as a promising technique for studying the dynamics of complex systems. In this work, we demonstrate the power of this algorithm using synthetic x-ray diffraction snapshots from a protein with significant data incompleteness, timing uncertainties, and noise. Our study confirms that NLSA is a suitable approach that effectively mitigates the effects of these artifacts in TR-SFX data and recovers accurate structural dynamics information hidden in such data.

Trujillo, Justin (ORCID:0000000285505360)↗
DOE OSTI2025

Time-resolved probing of laser-induced nanostructuring processes in liquids

Laser synthesis and processing of colloids (LSPC) in liquids has gained widespread applications in producing nanomaterials of different classes of solids. While the technical processes in different cases of ablation, fragmentation or colloidal fusion may look macroscopically different in each application, the underlying fundamental mechanisms are always the same cascade of laser interaction with matter, non-thermal or thermal energy deposition, phase transitions, and the subsequent structure formation processes. Disentangling these mechanisms represents a veritable challenge, as ultrafast and structurally sensitive experimental methods are required. This review presents a discussion of how state-of-the-art experimental protocols using ultrafast lasers and sensitive structural probes, such as electrons or X-rays are able to address this challenge. In particular, it is possible to investigate LSPC on single objects using single probe pulses and avoid accumulation effects in a heterogeneous sample. The presented results capture structure formation with femtosecond and atomic scale resolution. Ultrafast time-resolved probing approaches are key to revealing the transient states and pathways that govern material transformation in LSPC.

X-ray scattering↗
DOE OSTI2026

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↗