arXiv subjects

Ryan A. Duncan

Publications and source records attributed to Ryan A. Duncan.

12 recordsLinked to original sources

arXiv2026

Dynamically suppressed lattice rotations in SrTiO$_3$ as a basis for photo-induced ferroelectricity

Photo-induced ferroelectricity in the quantum paraelectric SrTiO$_3$ involves the dynamical interplay between a coherently driven Ti-O stretching vibration and multiple structural degrees of freedom, including antiferrodistortive rotations, strain, and the polar mode instability. In the high-temperature cubic phase, in the absence of average antiferrodistortion, time-resolved X-ray diffuse scattering has evidenced a correlation between a photo-induced reduction in antiferrodistortive fluctuations and the emergence of ferroelectric order. Here, we complement these measurements with time-resolved elastic X-ray diffraction in the low-temperature tetragonal phase, in which antiferrodistortive fluctuations are small but a finite average rotation has set in. In this phase, we observe a long-lived reduction of the equilibrium antiferrodistortive rotation angle. A unified theory of the nonlinear lattice dynamics based on first-principles calculations describes the dynamics in both high-temperature cubic and low-temperature tetragonal phases, providing a basis for light-induced ferroelectricity in SrTiO$_3$.

cond-mat.mtrl-sci↗

arXiv2026

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↗

arXiv2025

Dimensionality reduction of optically generated vortex strings in a charge density wave

In phase transitions, mesoscale structures such as topological defects, vortex strings, and domain walls control the path towards equilibrium, and thus the functional properties of many active devices. In photoinduced phase transitions driven by femtosecond laser excitation, the temporal (pulse duration) and spatial (penetration depth) structure of the optical excitation present opportunities for control and creating structures with unique topologies. By performing time-resolved optical pump, x-ray probe experiments on the CDW system Pd-intercalated ErTe$_{3}$, we gain access to the nanoscale dynamics of the mesoscale topological features (vortex strings) produced after a quench, which have a different apparent dimensionality than the topological defects predicted from the bulk system. We show that these vortex strings persist for much longer than the electronic recovery time. The critical exponent obtained from power-law scaling of the intensity as a function of wavevector shows a reduction in the effective dimensionality of the topological defects in the system, corroborated by time-dependent Ginzburg-Landau simulations. Our results demonstrate a novel pathway to use light to control the dimensionality and orientation of topological defects in quantum materials, which could be used to stabilize competing quantum states.

cond-mat.mes-hall↗

arXiv2024

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↗

arXiv2024

Observation of polarization density waves in SrTiO3

The nature of the "failed" ferroelectric transition in SrTiO3 has been a long-standing puzzle in condensed matter physics. A compelling explanation is the competition between ferroelectricity and an instability with a mesoscopic modulation of the polarization. These polarization density waves, which should become especially strong near the quantum critical point, break local inversion symmetry and are difficult to probe with conventional x-ray scattering methods. Here we combine a femtosecond x-ray free electron laser (XFEL) with THz coherent control methods to probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization on nanometer lengthscales in SrTiO3. We find polar-acoustic collective modes that are soft particularly at the tens of nanometer lengthscale. These precursor collective excitations provide evidence for the conjectured mesoscopic modulated phase in SrTiO3.

cond-mat.mtrl-sci↗

arXiv2024

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↗

arXiv2022

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↗

arXiv2022

Observation of the massive Lee-Fukuyama phason in a charge density wave insulator

The lowest-lying fundamental excitation of an incommensurate charge density wave (CDW) material is widely believed to be a massless phason -- a collective modulation of the phase of the CDW order parameter. However, as first pointed out by Lee and Fukuyama, long-range Coulomb interactions should push the phason energy up to the plasma energy of the CDW condensate, resulting in a massive phason and a fully gapped spectrum. Whether such behavior occurs in a CDW system has been unresolved for more than four decades. Using time-domain THz emission spectroscopy, we investigate this issue in the material (TaSe$_4$)$_2$I, a classical example of a quasi-one-dimensional CDW insulator. Upon transient photoexcitation at low temperatures, we find the material strikingly emits coherent, narrow-band THz radiation. The frequency, polarization and temperature-dependence of the emitted radiation imply the existence of a phason that acquires mass by coupling to long-range Coulomb interaction. Our observations constitute the first direct evidence of the massive "Lee-Fukuyama" phason and highlight the potential applicability of fundamental collective modes of correlated materials as compact and robust sources of THz radiation.

cond-mat.str-el↗

arXiv2020

Thermal transport in nanoporous holey silicon membranes investigated with optically-induced transient thermal gratings

In this study, we use the transient thermal grating optical technique \textemdash a non-contact, laser-based thermal metrology technique with intrinsically high accuracy \textemdash to investigate room-temperature phonon-mediated thermal transport in two nanoporous holey silicon membranes with limiting dimensions of 100 nm and 250 nm respectively. We compare the experimental results to ab initio calculations of phonon-mediated thermal transport according to the phonon Boltzmann transport equation (BTE) using two different computational techniques. We find that the calculations conducted within the Casimir framework, i.e. based on the BTE with the bulk phonon dispersion and diffuse scattering from surfaces, are in quantitative agreement with the experimental data, and thus conclude that this framework is adequate for describing phonon-mediated thermal transport through holey silicon membranes with feature sizes on the order of 100 nm.

cond-mat.mes-hall↗

arXiv2019

Observation of second sound in graphite at temperatures above 100 K

Wavelike thermal transport in solids, referred to as second sound, has until now been an exotic phenomenon limited to a handful of materials at low temperatures. This has restricted interest in its occurrence and in its potential applications. Through time-resolved optical measurements of thermal transport on 5-20 μm length scales in graphite, we have made direct observations of second sound at temperatures above 100 K. The results are in qualitative agreement with ab initio calculations that predict wavelike phonon hydrodynamics on ~ 1-μm length scale up to almost room temperature. The results suggest an important role of second sound in microscale transient heat transport in two-dimensional and layered materials in a wide temperature range.

cond-mat.mes-hall↗

arXiv2017

Unifying first principle theoretical predictions and experimental measurements of size effects on thermal transport in SiGe alloys

In this work, we demonstrate the correspondence between first principle calculations and experimental measurements of size effects on thermal transport in SiGe alloys. Transient thermal grating (TTG) is used to measure the effective thermal conductivity. The virtual crystal approximation under the density functional theory (DFT) framework combined with impurity scattering is used to determine the phonon properties for the exact alloy composition of the measured samples. With these properties, classical size effects are calculated for the experimental geometry of reflection mode TTG using the recently-developed variational solution to the phonon Boltzmann transport equation (BTE), which is verified against established Monte Carlo simulations. We find agreement between theoretical predictions and experimental measurements in the reduction of thermal conductivity (as much as $\sim$ 25\% of the bulk value) across grating periods spanning one order of magnitude. This work provides a framework for the tabletop study of size effects on thermal transport.

cond-mat.mes-hall↗

arXiv2016

Thermal transport in suspended silicon membranes measured by laser-induced transient gratings

Studying thermal transport at the nanoscale poses formidable experimental challenges due both to the physics of the measurement process and to the issues of accuracy and reproducibility. The laser-induced transient thermal grating (TTG) technique permits non-contact measurements on nanostructured samples without a need for metal heaters or any other extraneous structures, offering the advantage of inherently high absolute accuracy. We present a review of recent studies of thermal transport in nanoscale silicon membranes using the TTG technique. An overview of the methodology, including an analysis of measurements errors, is followed by a discussion of new findings obtained from measurements on both solid and nanopatterned membranes. The most important results have been a direct observation of non-diffusive phonon-mediated transport at room temperature and measurements of thickness-dependent thermal conductivity of suspended membranes across a wide thickness range, showing good agreement with first-principles-based theory assuming diffuse scattering at the boundaries. Measurements on a membrane with a periodic pattern of nanosized holes indicated fully diffusive transport and yielded thermal diffusivity values in agreement with Monte Carlo simulations. Based on the results obtained to-date, we conclude that room-temperature thermal transport in membranebased silicon nanostructures is now reasonably well understood.

cond-mat.mes-hall↗