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David A. Reis

Publications and source records attributed to David A. Reis.

At least 19 recordsLinked to original sources

Nonresonant optomechanical control of structural phases

Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties.

physics.optics

Emergent Antiphase Stacking in a Transient Charge Density Wave

Photoexcitation can induce novel states in materials that are inaccessible in equilibrium, a recent example being the light-induced charge density wave (CDW) observed in $\text{LaTe}_3$. Here, we investigate this transient CDW using infrared-pump x-ray-probe scattering at a free-electron laser, with high momentum and time resolution. We find that the transient CDW Bragg peak is broad in reciprocal space, indicating a highly disordered state. The ordering wavevector of the transient state is different from the equilibrium orders that develop in this class of materials - the transient peak appears near (2/7, 0, 0) reciprocal lattice units, whereas the equilibrium $a$ order and $c$ order occur at $\approx (5/7, 0, 0)$ and $(0, 0, 2/7)$, respectively. The transient CDW is therefore distinct from the equilibrium $a$ order, differing in the relative phase of the CDW displacement between the two equivalent nearly-square Te-Te nets in the conventional unit cell. Our work highlights how photoexcitation can access states with no equilibrium analog, and how x-ray scattering can provide microscopic insight into such elusive phases.

cond-mat.str-el

A textured polar phase in strained SrTiO3

Quantum materials can harbour hidden phases whose microscopic structures differ from conventional ordered states while reproducing their macroscopic signatures, making them easy to miss. Strontium titanate is a longstanding puzzle of this kind: on cooling it shows every hallmark of an incipient ferroelectric, yet never orders, and is usually described as a quantum paraelectric in which fluctuations suppress ferroelectricity. Here we combine uniaxial strain, single-cycle terahertz excitation and femtosecond x-ray scattering to measure the polar collective modes of strontium titanate as a function of momentum and strain. Under modest tensile strain, we observe a new vibrational mode that emerges not at the Brillouin zone centre, as a ferroelectric transition would require, but at finite wavevector, identifying the ordered state as a polar texture on nanometre length scales rather than a uniform ferroelectric. Unstrained quantum paraelectric strontium titanate is then naturally understood as the disordered precursor of this textured phase, offering a resolution to a decades-old puzzle and illustrating how finite-momentum collective excitations can unmask hidden phases in quantum materials.

cond-mat.mtrl-sci

Initial Performance of the E320 Tracker

Our recent study discussed the prospects for measuring single positrons produced in electron-laser collisions via the nonlinear Breit-Wheeler deep-tunneling process in the SLAC Experiment 320 at the FACET-II RF LINAC. In this work, we demonstrate how a tracking detector, that is a scaled-down version of the one discussed in the prospective simulation study, enables the measurement. This prototype detector, installed in Aug 2024, is built out of five layers of single ALPIDE chips. The data are taken from several standalone runs completed in Nov 2024 and Feb 2025. We use positrons generated through conversion of Bremsstrahlung photons as a proxy to the nonlinear Breit-Wheeler process. These positrons are produced by the beam electrons in a thin Beryllium foil close to the experiment's interaction point. The tracking approach used in this initial work is based on a Hough-Transform seeding algorithm followed by a straight line fit confined to the detector volume. Even with this relatively simple approach, we are able to measure a signal rate of $(1.20\pm0.06_{stat.}\pm0.56_{syst.})\times10^{-1}$ positrons per shot. This signal rate is comparable to the nonlinear Breit-Wheeler rate expected in the main experiment. Notably, the measurement is achieved under an extreme, unprecedented background hit density of ~1.7/mm$^2$, unlike the main experiment, where at least a twice lower density is expected. This large background is mostly due to secondary particles produced when the large flux of Bremsstrahlung photons interacts with the material of the beamline elements. When the foil is retracted, the false-positive signal rate is shown to be four orders of magnitude smaller than the signal rate. We further show that the high spatial tracking resolution of ~5 micron allows to characterize the positrons' spectra. The results are compared to simulations, which are found to be compatible with the data.

hep-ex

Phonon-driven decoherence of high-harmonic generation in the solid-state

High-harmonic generation in solids has emerged as a powerful probe of ultrafast electron dynamics and lattice motion, and recent theoretical work has suggested that thermally driven lattice fluctuations can act as an effective source of decoherence in the harmonic-generation process. However, a direct experimental link between high-harmonic emission and temperature-driven incoherent phonons has remained unclear. Here, we investigate the temperature dependence of high-harmonic generation in ultrapure silicon using reflection-geometry measurements over a wide temperature range. We observe that the harmonic yield increases significantly with decreasing temperature. To interpret these results, we introduce a one-dimensional atomic-chain model in which finite temperature is represented by random lattice displacements that mimic incoherent phonon fluctuations. The simulations reproduce the magnitude of temperature-dependent change of the harmonic signal and support a picture in which thermally induced lattice disorder enhances electron-hole decoherence, thereby reducing high-harmonic emission. Our results establish incoherent phonons as an important source of decoherence in solid-state high-harmonic generation.

cond-mat.mes-hall

Prospects for the production and detection of Breit-Wheeler tunneling positrons in Experiment 320 at the FACET-II accelerator

The SLAC Experiment 320 collides 10 TW-class laser pulses with the high-quality, 10 GeV electron beam from the FACET-II RF LINAC. This setup is expected to produce a sizable number of $e^+e^-$ pairs via nonlinear Breit-Wheeler mechanism in the strong-field tunneling regime, with an estimated yield of ~0.01-0.1 pairs per collision. This small signal rate typically comes along with large backgrounds originating, e.g., from dumping the high-charge primary beam, secondaries induced by the beam halo, as well as photons and low-energy electrons produced in the electron-laser collision itself. These backgrounds may reach densities of O(100) charged particles per cm^2 (and even more neutral particles) at the surface of the sensing elements, making it a tremendous challenge for an unambiguous detection of single particles. In this work, we demonstrate how detectors and methods adapted from high-energy physics experiments, can enable this measurement. The solution presented is based on a highly granular, multi-layer, radiation-hard pixel detector paired with powerful particle-tracking algorithms. Using a detailed simulation of the existing experimental setup, we show how the false-positive rate due to background processes can be reduced by more than an order of magnitude relative to the expected signal after full reconstruction. Furthermore, we show that the high spatial tracking resolution achievable (<10 microns) allows for positron momentum measurements with a resolution of <2%, enabling spectral characterization of the nonlinear Breit-Wheeler process. Based on our extensive simulation, with a conservatively large background assumption, we show that it is possible to measure single Breit-Wheeler positrons in the coming data taking campaign of E320. That would be the first statistically significant observation and characterization of this elusive process in the (deep) tunneling regime.

hep-ex

Terahertz-induced tunnel ionization drives coherent Raman-active phonon in Bismuth

Driving coherent lattice motion with THz pulses has emerged as a novel pathway for achieving dynamic stabilization of exotic phases that are inaccessible in equilibrium quantum materials. In this work, we present a previously unexplored mechanism for THz excitation of Raman-active phonons. We show that intense THz pulses centered at 1 THz can excite the Raman-active $A_{1g}$ phonon mode at 2.9 THz in a bismuth film. We rule out the possibilities of the phonon being excited through conventional anharmonic coupling to other modes or via a THz sum frequency process. Instead, we demonstrate that the THz-driven tunnel ionization provides a plausible means of creating a displacive driving force to initiate the phonon oscillations. Our work highlights a new mechanism for exciting coherent phonons, offering potential for dynamic control over the electronic and structural properties of semimetals and narrow-band semiconductors on ultrafast timescales.

cond-mat.mes-hall

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics

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.

cond-mat.mtrl-sci

Nanoscale Ultrafast Lattice Modulation with Hard X-ray Free Electron Laser

Understanding and controlling microscopic dynamics across spatial and temporal scales has driven major progress in science and technology over the past several decades. While ultrafast laser-based techniques have enabled probing nanoscale dynamics at their intrinsic temporal scales down to femto- and attoseconds, the long wavelengths of optical lasers have prevented the interrogation and manipulation of such dynamics with nanoscale spatial specificity. With advances in hard X-ray free electron lasers (FELs), significant progress has been made developing X-ray transient grating (XTG) spectroscopy, aiming at the coherent control of elementary excitations with nanoscale X-ray standing waves. So far, XTGs have been probed only at optical wavelengths, thus intrinsically limiting the achievable periodicities to several hundreds of nm. By achieving sub-femtosecond synchronization of two hard X-ray pulses at a controlled crossing angle, we demonstrate the generation of an XTG with spatial periods of 10 nm. The XTG excitation drives a thermal grating that drives coherent monochromatic longitudinal acoustic phonons in the cubic perovskite, SrTiO3 (STO). With a third X-ray pulse with the same photon energy, time-and-momentum resolved measurement of the XTG-induced scattering intensity modulation provides evidence of ballistic thermal transport at nanometer scale in STO. These results highlight the great potential of XTG for studying high-wave-vector excitations and nanoscale transport in condensed matter, and establish XTG as a powerful platform for the coherent control and study of nanoscale dynamics.

physics.optics

A High-Flux Electron Detector System to Measure Non-linear Compton Scattering at LUXE

Recently, advancements in high-intensity laser technology have enabled the exploration of non-perturbative Quantum Electrodynamics (QED) in strong-field regimes. Notable aspects include non-linear Compton scattering and Breit-Wheeler pair production, observable when colliding high-intensity laser pulses and relativistic electron beams. The LUXE experiment at DESY and the E-320 experiment at SLAC aim to study these phenomena by measuring the created high-flux Compton electrons and photons. We propose a novel detector system featuring a segmented gas-filled Cherenkov detector with a scintillator screen and camera setup, designed to efficiently detect high-flux Compton electrons. Preliminary results from E-320 measurement campaigns demonstrate methods for reconstructing electron energy spectra, aiming to reveal crucial features of non-perturbative QED.

physics.ins-det

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic lengthscales. Our results provide direct evidence that ultrafast excitation of LaTe$_3$ leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

cond-mat.mtrl-sci

Ultrafast measurements under anisotropic strain reveal near equivalence of competing charge orders in TbTe$_3$

We report ultrafast reflectivity measurements of the dynamics of the order parameter of the charge density wave (CDW) in TbTe$_3$ under anisotropic strain. We observe an increase in the frequency of the amplitude mode with increasing tensile strain along the $a$-axis (which drives the lattice into $a>c$, with $a$ and $c$ the lattice constants), and similar behavior for tensile strain along $c$ ($c>a$). This suggests that both strains stabilize the corresponding CDW order and further support the near equivalence of the CDW phases oriented in $a$- and $c$-axis, in spite of the orthorhombic space group. The results were analyzed within the time-dependent Ginzburg-Landau framework, which agrees well with the reflectivity dynamics.

cond-mat.str-el

Ultrafast lattice disordering can be accelerated by electronic collisional forces

In the prevalent picture of ultrafast structural phase transitions, the atomic motion occurs in a slowly varying potential energy surface determined adiabatically by the fast electrons. However, this ignores non-conservative forces caused by electron-lattice collisions, which can significantly influence atomic motion. Most ultrafast techniques only probe the average structure and are less sensitive to random displacements, and therefore do not detect the role played by non-conservative forces in phase transitions. Here we show that the lattice dynamics of the prototypical insulator-to-metal transition of VO2 cannot be described by a potential energy alone. We use the sample temperature to control the preexisting lattice disorder before ultrafast photoexcitation across the phase transition and our ultrafast diffuse scattering experiments show that the fluctuations characteristic of the rutile metal develop equally fast (120 fs) at initial temperatures of 100 K and 300 K. This indicates that additional non-conservative forces are responsible for the increased lattice disorder. These results highlight the need for more sophisticated descriptions of ultrafast phenomena beyond the Born-Oppenheimer approximation as well as ultrafast probes of spatial fluctuations beyond the average unit cell measured by diffraction.

cond-mat.str-el

Hard X-ray Generation and Detection of Nanometer-Scale Localized Coherent Acoustic Wave Packets in SrTiO$_3$ and KTaO$_3$

We demonstrate that the absorption of femtosecond x-ray pulses can excite quasi-spherical high-wavevector coherent acoustic phonon wavepackets using an all x-ray pump and probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with strain pulses 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 strain wavepacket and the energy absorption efficiency, which 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, even though there are no nanoscale structures or light-intensity patterns that would ordinarily be required to generate acoustic waves of wavelengths much shorter than the penetration depth. Whereas in GaAs and GaP we do not observe a signal above background. The results provide crucial information on x-ray matter interactions, which sheds light on the mechanism of x-ray energy deposition, and the study of high wavevector acoustic phonons and thermal transport at the nanoscale.

cond-mat.mtrl-sci

Ultrafast measurements of mode-specific deformation potentials of Bi$_2$Te$_3$ and Bi$_2$Se$_3$

Quantifying electron-phonon interactions for the surface states of topological materials can provide key insights into surface-state transport, topological superconductivity, and potentially how to manipulate the surface state using a structural degree of freedom. We perform time-resolved x-ray diffraction (XRD) and angle-resolved photoemission (ARPES) measurements on Bi$_2$Te$_3$ and Bi$_2$Se$_3$, following the excitation of coherent A$_{1g}$ optical phonons. We extract and compare the deformation potentials coupling the surface electronic states to local A$_{1g}$-like displacements in these two materials using the experimentally determined atomic displacements from XRD and electron band shifts from ARPES.We find the coupling in Bi$_2$Te$_3$ and Bi$_2$Se$_3$ to be similar and in general in agreement with expectations from density functional theory. We establish a methodology that quantifies the mode-specific electron-phonon coupling experimentally, allowing detailed comparison to theory. Our results shed light on fundamental processes in topological insulators involving electron-phonon coupling.

cond-mat.mtrl-sci

Determination of nonthermal bonding origin of a novel photoexcited lattice instability in SnSe

Interatomic forces that bind materials are largely determined by an often complex interplay between the electronic band-structure and the atomic arrangements to form its equilibrium structure and dynamics. As these forces also determine the phonon dispersion, lattice dynamics measurements are often crucial tools for understanding how materials transform between different structures. This is the case for the mono-chalcogenides which feature a number of lattice instabilities associated with their network of resonant bonds and a large tunability in their functional properties. SnSe hosts a novel lattice instability upon above-bandgap photoexcitation that is distinct from the distortions associated with its high temperature phase transition, demonstrating that photoexcitation can alter the interatomic forces significantly different than thermal excitation. Here we report decisive time-resolved X-ray scattering-based measurements of the nonequlibrium lattice dynamics in SnSe. By fitting interatomic force models to the excited-state dispersion, we determine this instability as being primarily due to changes in the fourth-nearest neighbor bonds that connect bilayers, with relatively little change to the intralayer resonant bonds. In addition to providing critical insight into the nonthermal bonding origin of the instability in SnSe, such measurements will be crucial for understanding and controlling materials properties under non-equilibrium conditions.

cond-mat.mtrl-sci

Ultrafast x-ray scattering reveals composite amplitude collective mode in the Weyl charge density wave material (TaSe$_4$)$_2$I

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe$_4$)$_2$I following photoexcitation with femtosecond infrared laser pulses. From the time-dependent diffraction signal at the CDW sidebands we identify an amplitude mode derived primarily from the transverse acoustic component of the CDW static distortion. The dynamics of this acoustic amplitude mode are described well by a model of a displacive excitation, which we interpret as mediated through a coupling to the optical phonon component associated with the tetramerization of the Ta chains.

cond-mat.mtrl-sci