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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites

Abstract Interplay between structural and photophysical properties of metal halide perovskites is critical to their utility in optoelectronics, but there is limited understanding of lattice response upon photoexcitation. Here, 2D perovskites butylammonium lead iodide, (BA) 2 PbI 4 , and phenethylammonium lead iodide, (PEA) 2 PbI 4 , are investigated using ultrafast transient X‐ray diffraction as a function of optical excitation fluence to discern structural dynamics. Both powder X‐ray diffraction and time‐resolved photoluminescence linewidths narrow over 1 ns following optical excitation for the fluence range studied, concurrent with slight redshifting of the optical bandgaps. These observations are attributed to transient relaxation and ordering of distorted lead iodide octahedra stimulated mainly by electron–hole pair creation. The c axis expands up to 0.37% over hundreds of picoseconds; reflections sampling the a and b axes undergo one tenth of this expansion with the same timescale. Post‐photoexcitation appearance of the (110) reflection in (BA) 2 PbI 4 would suggest a transient phase transition, however, through new single‐crystal XRD, reflections are found that violate glide plane conditions in the reported Pbca structure. The static structure space group is reassigned as P 2 1 2 1 2 1 . With this, a nonequilibrium phase transition is ruled out. These findings offer increased understanding of remarkable lattice response in 2D perovskites upon excitation.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi 2 Te 4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi 2 Te 4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. Here, by quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

36 MATERIALS SCIENCE↗
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↗
DOE OSTI2020

One–Step Fabrication of Nanocrystalline Nanonetwork SnO 2 Gas Sensors by Integrated Multilaser Processing

An integrated multilaser process is developed to fabricate nanocrystalline nanonetwork SnO 2 gas sensors in one integrated procedure, which combines electrodes fabrication, nanomaterials deposition, and postannealing. Interdigit electrodes are fabricated on an Au-coated fused silica substrate using a picosecond (ps) laser, which ablates the Au coating from the back of the substrate to pattern the electrodes. A novel transmitted Ps laser deposition (TPLD) process is designed to deposit SnO 2 nanonetwork on the interdigit electrodes with precise deposition area control under a close target-to-substrate distance. The obtained SnO 2 nanonetwork is in situ postannealed by a CO 2 laser to improve the crystallinity, while the nano morphology and grain size keep intact. To investigate the morphology and formation process of the nanonetwork, the microstructure of the laser-deposited SnO 2 layer is characterized. As a result, the crystallization control of CO 2 laser annealing is investigated through analyzing the Raman spectrum, X-ray diffraction (XRD) patterns, and lattice structures of the samples. By exposed to H 2 atmosphere, the fabricated gas sensor is demonstrated for H 2 monitoring.

08 HYDROGEN↗
DOE OSTI2021

Deep Optical Switching on Subpicosecond Timescales in an Amorphous Ge Metamaterial

Active nanostructured optical components show promise as potential building blocks for novel light-based computing and data processing architectures. However, nanoscale all-optical switches that have low activation powers and high-contrast ultrafast switching have been elusive so far. Here, pump–probe measurements performed on amorphous-Ge-based micro-resonator metasurfaces that exhibit strong resonant modes in the mid-infrared are reported. Relative change is observed in transmittance of ΔT/T ≈ 1 with picosecond (down to τ ≈ 0.5 ps) free carrier relaxation rates, obtained with very low pump fluences of 50 μJ cm –2 . In this work, these observations are attributed to efficient free carrier promotion, affecting light transmittance via high quality-factor optical resonances, followed by an increased electron–phonon scattering of free carriers due to the amorphous crystal structure of Ge. Full-wave simulations based on a permittivity model that describes free-carrier damping through crystal structure disorder find excellent agreement with the experimental data. These findings offer an efficient and robust platform for all-optical switching at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Large-Area Lasing in Nanoscale Complex Media: The Critical Role of Local Dielectric Environment

Controlling how electromagnetic waves interact with complex media is critical for applications in imaging and focusing. Such lightwave interactions with complex media can lead to dramatic optical effects like lasing. While much work in random lasing focus on understanding how gain and scattering co-operatively generate lasing, little work has focused on how to manipulate the lasing threshold without modifying the structural disorder. Here, a simple, mostly unexplored, strategy is demonstrated that employs atomic layer deposition (ALD) to tune the local near-field environment while preserving the underpinning disorder—controlling lasing in a nanoscale complex medium on a large scale (>cm 2 ). The nanoscale complex medium is a quasi-2D system of coupled zinc oxide nanospheres with overall thickness deep in the sub-wavelength regime (≈λ/4). Near-ultraviolet femtosecond spectroscopy probes the broadband response of the gain nanomaterial, details how ALD process fundamentally modifies the fast-picosecond and slow-nanosecond carrier dynamics, and informs on the relevant timescales critical for lasing. Full-field electromagnetic simulations provide critical insights about how near-field dielectric environment modifies the nanostructure's scattering cross-section, which ultimately results in enhanced lasing. Importantly, these results highlight a simple path to control how electromagnetic waves interact in a complex medium, a key step toward large-scale implementation of complex lasers.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Insight into Pyroelectricity and Phase Transitions in Ferroelectrics from Nonequilibrium Approach: The Case of PbTiO 3

Computational methodology is proposed to simulate time dependent temperature variations via thermostat approach. Here, the methodology is applied to study pyroelectricity under nonequilibrium conditions in prototypical ferroelectric PbTiO 3 . It is found that at room temperature the nonequilibrium effects in pyroelectricity begin manifesting above 1.0 THz and originate from the overlap with the intrinsic soft mode frequency. Therefore, the proposed computational methodology can be used to predict equilibrium pyroelectric response by choosing a frequency of temperature variation below the intrinsic polar mode frequencies for the material. Probing the dynamics of ferroelectric phase transition with the proposed methodology revealed that it takes about a nanosecond for the computational supercell to undergo phase transition. It is concluded that computational techniques capable of simulating picoseconds can be used to compute pyroelectric response from nonequilibrium dynamical approach while those that can reach nanoseconds are suitable for simulating phase transitions in ferroelectrics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The Coordination Behaviour of Cu I Photosensitizers Bearing Multidentate Ligands Investigated by X-ray Absorption Spectroscopy

A systematic series of four novel homo- and heteroleptic CuI photosensitizers based on tetradentate 1,10-phenanthroline ligands of the type X^N^N^X containing two additional donor moieties in the 2,9-position (X=SMe or OMe) were designed. Their solid-state structures were assessed by X-ray diffraction. Cyclic voltammetry, UV-vis absorption, emission and X-ray absorption spectroscopy were then used to determine their electrochemical, photophysical and structural features in solution. Following, time-resolved X-ray absorption spectroscopy in the picosecond time scale, coupled with time-dependent density functional theory calculations, provided in-depth information on the excited state electron configurations. For the first time, a significant shortening of the Cu–X distance and a change in the coordination mode to a pentacoordinated geometry is shown in the excited states of the two homoleptic complexes. These findings are important with respect to a precise understanding of the excited state structures and a further stabilization of this type of photosensitizers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Site-Selective Real-Time Observation of Bimolecular Electron Transfer in a Photocatalytic System Using L-Edge X-Ray Absorption Spectroscopy

Here, time-resolved X-ray absorption spectroscopy has been utilized to monitor the bimolecular electron transfer in a photocatalytic water splitting system. This has been possible by uniting the local probe and element specific character of X-ray transitions with insights from high-level ab initio calculations. The specific target has been a heteroleptic [Ir III (ppy) 2 (bpy)] + photosensitizer, in combination with triethylamine as a sacrificial reductant and Fe 3 (CO) 12 as a water reduction catalyst. The relevant molecular transitions have been characterized via high-resolution Ir L-edge X-ray absorption spectroscopy on the picosecond time scale and restricted active space self-consistent field calculations. The presented methods and results will enhance our understanding of functionally relevant bimolecular electron transfer reactions and thus will pave the road to rational optimization of photocatalytic performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Tip‐Enhanced Imaging and Control of Infrared Strong Light‐Matter Interaction

Optical antenna resonators enable control of light‐matter interactions on the nano‐scale via electron–photon hybrid states in strong coupling. Specifically, mid‐infrared (MIR) nano‐antennas coupled to saturable intersubband transitions in multi‐quantum‐well (MQW) semiconductor heterostructures allow for the coupling strength to be tuned through antenna resonance and field intensity. Here, in this study, tip‐enhanced nano‐scale variation of antenna‐MQW coupling across the antenna is demonstrated, with a spatially‐dependent coupling strength $g_{\textrm{aq}}$ varying from 73 (strong coupling) to 24 cm -1 (weak coupling). This behavior is modeled based on the spatially dependent local constructive and destructive interference between tip and antenna fields. Using a quantum‐mechanical density‐matrix model of the MQW system with its designed values of transition dipole moment, doping density, and population decay time, the picosecond IR pulse coupling to intersubband transitions and the associated tip induced strong‐field saturation effects are described. These results present a new regime of nonlinear IR light‐matter control based on the dynamic manipulation of quantum hybrid states on the nanoscale and in the infrared, with a perspective regarding extension to molecular vibrations.

Wang, Yueying↗
DOE OSTI2024

Optical Diagnostics of Discharges in and in Contact With Liquids

Discharges in liquids have been the subject of intensive investigations for a broad range of applications and involve highly coupled and complex phenomena with timescales ranging from picoseconds to seconds and length scales from micrometers to centimeters. This review focuses on some of the challenges in optical diagnostics of discharges in and in contact with liquids; this includes the interpretation of optical emission spectra, the inherently stochastic nature of many discharge phenomena including the initial stages of plasma ignition, and the large gradients in species and plasma properties interfacing with a dynamic liquid interface. We report recent notable advances, controversies in interpretations of diagnostics, and remaining opportunities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Ultrafast Laser Welding and Terahertz Time-domain Spectroscopy of Soda Lime Silicate Glass

Joining and welding techniques of similar and dissimilar materials have reached their limits due to the inflexibility of adapting dielectric materials, e.g., glasses and ceramics, reproducibility for transparent materials, and cycle process time. The ability to join pieces of glasses using laser irradiation allows rapid processing of vacuum insulating glass (VIG) for a widening range of commercial energy-efficient applications. We have used a 1064-nm laser wavelength with 15 picoseconds pulse width and a 155-kHz repetition rate to weld commercial plate glass pieces. The welded samples were characterized via x-ray fluorescence (XRF), time-of-flight secondary ion mass spectrometry (TOF–SIMS), polarimetry, and terahertz time-domain spectroscopy (THz-TDS) to determine the integrity of the weld and chemical changes in the welded areas. Our data shows no significant changes in glass chemistry and structure on average over nano- to micro-scales occurred from the welding process within the limits of the characterization tools. Our results demonstrate successful welding of glass plates without significant changes in the glass chemistry, structure, or properties in the laser-modified region or strains in the bulk glass.

Matthies, Kathleen [ORNL] (ORCID:0009000213135441)↗
DOE OSTI2020

Ultrafast terahertz spectroscopy provides insight into charge transfer efficiency and dynamics in artificial photosynthesis

Terahertz (THz) spectroscopy provides a noncontact method to measure the ultrafast dynamics and photoconductivity of mobile carriers in semiconducting materials. This has proven useful in studying artificial photosynthesis devices which use semiconductor photoelectrodes. In this work, we present a brief introduction to optical-pump THz-probe (OPTP) spectroscopy, a technique that provides unique and useful insight into interfacial electron transfer (from the surface-attached dye to the conduction band of the semiconductor) in dye-sensitized photoelectrochemical cells. Compared with more familiar methods like visible transient absorption spectroscopy, OPTP spectroscopy stands out in offering both sub-picosecond time resolution as well as sensitivity to mobile carriers (electrons and holes) in the semiconductor portion of artificial photosynthesis devices. The mobile carriers are crucial to device performance as only they pass to the other half cell to complete the reaction. In order to highlight these advantages and illustrate the types of questions OPTP spectroscopy can address, we discuss three case studies. In the first, OPTP spectroscopy is used to measure the injection rates from a set of six different dyes, revealing the effect of the energetics and lifetimes of the dye excited states on interfacial electron transfer. The subsequent case studies investigate the influence of varying the moieties which bind to the surface (anchors), as well as the moieties that connect the chromophore with these anchors (linkers). OPTP spectroscopy was used to measure the interfacial electron transfer rate as these moieties were varied.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Electronic Melting of Silicon in Nanostructures using X-ray Forbidden Bragg Reflections

Abstract We carried out a short beamtime at the Pohang Accelerator Laboratory x-ray Free Electron Laser to perform a pump-probe (PP) laser excitation diffraction experiment on the silicon (222) forbidden Bragg peak. To limit the x-ray penetration, we used a “device layer” silicon film wafer bonded to a silicon substrate. The sample, specially fabricated by MEMC Electronic Materials, had a Si(100) substrate bonded to a 170 nm Si(100) film rotated at 45° for crystallographic isolation. A second sample was reactive-ion-etched down to 52 nm thickness. In the silicon lattice, the covalent bonds are seen exclusively at the 222 reflection. Upon laser excitation, these electrons are expected to be excited to the valence band on femtosecond electronic time scales. The Si(222) reflection is therefore expected to be extinguished on this fast time scale, while the electron–phonon coupled acoustic response is determined by the lattice dynamics. The latter is determined by the speed of sound over the device thickness, which is in the mid-picosecond range.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Observation of Fundamental Mechanisms in Compression-Induced Phase Transformations Using Ultrafast X-ray Diffraction

As theoretically hypothesized for several decades in group IV transition metals, we have discovered a dynamically stabilized body-centered cubic (bcc) intermediate state in Zr under uniaxial loading at sub-nanosecond timescales. Under ultrafast shock wave compression, rather than the transformation from α-Zr to the more disordered hex-3 equilibrium ω-Zr phase, in its place we find the formation of a previously unobserved nonequilibrium bcc metastable intermediate. We probe the compression-induced phase transition pathway in zirconium using time-resolved sub-picosecond x-ray diffraction analysis at the Linac Coherent Light Source. We also present molecular dynamics simulations using a potential derived from first-principles methods which independently predict this intermediate phase under ultrafast shock conditions. In contrast with experiments on longer timescale (> 10 ns) where the phase diagram alone is an adequate predictor of the crystalline structure of a material, our recent study highlights the importance of metastability and time dependence in the kinetics of phase transformations.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Self-organization of photoionized plasmas via kinetic instabilities

Abstract Self-organization in an unmagnetized collisionless plasma (in this paper) refers to formation of transient coherent structures such as collective oscillations (electrostatic waves) or magnetic fields resulting from so-called kinetic effects in the plasma. This topical review provides a comprehensive analysis of the self-organization of strong-field photoionized, non-equilibrium plasmas through kinetic instabilities. The authors propose and demonstrate a novel experimental platform that enables the formation of dense plasmas with known highly anisotropic and non-thermal electron velocity distribution functions on a timescale on the order of an inverse electron plasma frequency. We then show that such plasmas are highly susceptible to a hierarchy of kinetic instabilities, including two-stream, current filamentation and Weibel, that convert a fraction of the electron kinetic energy into electric and/or magnetic energy stored in self-organized structures. The electrostatic waves so produced are measured using a collective light (Thomson) scattering technique with femtosecond resolution as the kinetic instabilities aided by collisions eventually thermalize the plasma electrons. In addition, we describe a novel experimental technique that has made it possible to map the temporal evolution of the wavenumber spectrum of the thermal Weibel instability with picosecond resolution, which leads to the formation of quasi-static coherent magnetic fields with different topologies in photoionized plasmas. Finally, the paper summarizes the important results and discusses future directions on this topic.

Zhang, Chaojie (ORCID:0000000180353014)↗
DOE OSTI2022

Transient nature of fast relaxation in metallic glass

Metallic glasses exhibit fast mechanical relaxations at temperatures well below the glass transition, one of which shows little variation with temperature known as nearly constant loss (NCL). Despite the important implications of this phenomenon to deformation, the origin of the relaxation is unclear. Through molecular dynamics simulations of a model metallic glass, Cu 64.5 Zr 35.5 , we implement molecular dynamics dynamical mechanical spectroscopy (MD-DMS) with system stress decomposed into atomic-level stresses to identify the group of atoms responsible for NCL. This work demonstrates that NCL relaxation is due to transient groups of atoms that revert to the typical atomic-level viscoelastic behavior over picosecond timescales. They are homogenously distributed throughout the glass and have no outstanding features, rather than having defect-like local structure as previously reported.

36 MATERIALS SCIENCE↗