arXiv subjects

K. A. Nelson

Publications and source records attributed to K. A. Nelson.

15 recordsLinked to original sources

arXiv2026

Time-domain extreme ultraviolet diffuse scattering spectroscopy of nanoscale surface phonons

We report the observation of dynamic fringe patterns in the diffuse scattering of extreme ultraviolet light from surfaces, following femtosecond optical excitation. At each point on the detector, the diffuse scattering intensity exhibits oscillations at well-defined frequencies that correspond to surface phonons with wave vectors determined by the scattering geometry, indicating that the optical excitation generates coherent surface phonons propagating in all directions and spanning a wavelength range from 60 to 300 nm. This phenomenon is observed on a variety of samples, including single-layer and multilayer metal films, as well as bulk semiconductors. The measured surface phonon dispersions show good agreement with theoretical calculations. By comparing signal amplitudes from samples with different surface morphologies, we find that the excitation mechanism is linked to the natural surface roughness of the samples. However, the signal is still detectable on extremely smooth surfaces with sub-nanometer roughness. Our findings demonstrate a simple and effective method for optically exciting coherent surface phonons with nanoscale wavelengths on a wide range of solid samples and establish a foundation for surface phonon spectroscopy in a wave vector range well beyond the limit of conventional surface Brillouin scattering.

cond-mat.mtrl-sci↗

arXiv2022

Reanalysis of experimental determinations of polariton-polariton interactions in microcavities

The polariton-polariton interaction strength is an important parameter for all kinds of applications using the nonlinear properties of polaritons, such as optical switching and single-photon blockade devices. In this paper, we review and compare the results of a series of experiments on polariton-polariton interactions in GaAs/Al$_x$Ga$_{-1x}$As microcavity polariton structures, and present new theoretical analysis of these experiments. We show that not just the energy shift of the spectral lines, but also the results of measurements sensitive to the polariton scattering rate are important for the calibration of the interaction parameter at low excitation density. We find that when adjustments are made to correct for new understanding of the experiments, the value of the interaction parameter at low density is lower than previous reported, but still significantly higher than theoretically predicted.

cond-mat.quant-gas↗

arXiv2022

Extreme ultraviolet transient gratings: A tool for nanoscale photoacoustics

Collective lattice dynamics determine essential aspects of condensed matter, such as elastic and thermal properties. These exhibit strong dependence on the length-scale, reflecting the marked wavevector dependence of lattice excitations. The extreme ultraviolet transient grating (EUV TG) approach has demonstrated the potential of accessing a wavevector range corresponding to the 10s of nm length-scale, representing a spatial scale of the highest relevance for fundamental physics and forefront technology, previously inaccessible by optical TG and other inelastic scattering methods. In this manuscript we report on the capabilities of this technique in the context of probing thermoelastic properties of matter, both in the bulk and at the surface, as well as discussing future developments and practical considerations.

cond-mat.mtrl-sci↗

arXiv2022

Direct Observation of Coherent Longitudinal and Shear Acoustic Phonons in TaAs Using Ultrafast X-ray Diffraction

Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast Suppression of the Ferroelectric Instability in KTaO$_3$

We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \kto. % We use ultrafast near-UV (central wavelength 266\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\,Å\, and $< 10$~fs pulse duration). We observe changes in the diffuse intensity that we conclude are associated with a hardening of the soft transverse optical and transverse acoustic phonon branches along $Γ$ to $X$ and $Γ$ to $M$. Using ground- and excited-state interatomic force constants from density functional theory (DFT) and assuming the phonon populations can be described by a time-dependent temperature, we fit the quasi-equilibrium thermal diffuse intensity to the experimental time-dependent intensity. We obtain the instantaneous lattice temperature and density of photoexcited charge carriers as a function of time delay. The DFT calculations demonstrate that photoexcitation transfers charge from oxygen $2p$ derived $π$-bonding orbitals to Ta $5d$ derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

cond-mat.mtrl-sci↗

arXiv2020

Nanoscale transient magnetization gratings excited and probed by femtosecond extreme ultraviolet pulses

We utilize coherent femtosecond extreme ultraviolet (EUV) pulses derived from a free electron laser (FEL) to generate transient periodic magnetization patterns with periods as short as 44 nm. Combining spatially periodic excitation with resonant probing at the dichroic M-edge of cobalt allows us to create and probe transient gratings of electronic and magnetic excitations in a CoGd alloy. In a demagnetized sample, we observe an electronic excitation with 50 fs rise time close to the FEL pulse duration and ~0.5 ps decay time within the range for the electron-phonon relaxation in metals. When the experiment is performed on a sample magnetized to saturation in an external field, we observe a magnetization grating, which appears on a sub-picosecond time scale as the sample is demagnetized at the maxima of the EUV intensity and then decays on the time scale of tens of picoseconds via thermal diffusion. The described approach opens prospects for studying dynamics of ultrafast magnetic phenomena on nanometer length scales.

cond-mat.mes-hall↗

arXiv2019

Effect of optically-induced potential on the energy of trapped exciton-polaritons below the condensation threshold

Exciton-polaritons (polaritons herein) offer a unique nonlinear platform for studies of collective macroscopic quantum phenomena in a solid state system. Shaping of polariton flow and polariton confinement via potential landscapes created by nonresonant optical pumping has gained considerable attention due to the degree of flexibility and control offered by optically-induced potentials. Recently, large density-dependent energy shifts (blueshifts) exhibited by optically trapped polaritons at low densities, below the bosonic condensation threshold, were interpreted as an evidence of strong polariton-polariton interactions [Nat. Phys. 13, 870 (2017)]. In this work, we further investigate the origins of these blueshifts in optically-induced circular traps and present evidence of significant blueshift of the polariton energy due to reshaping of the optically-induced potential with laser pump power. Our work demonstrates strong influence of the effective potential formed by an optically-injected excitonic reservoir on the energy blueshifts observed below and up to the polariton condensation threshold and suggests that the observed blueshifts arise due to interaction of polaritons with the excitonic reservoir, rather than due to polariton-polariton interaction.

cond-mat.quant-gas↗

arXiv2018

Single-bubble and multi-bubble cavitation in water triggered by laser-driven focusing shock waves

In this study a single laser pulse spatially shaped into a ring is focused into a thin water layer, creating an annular cavitation bubble and cylindrical shock waves: an outer shock that diverges away from the excitation laser ring and an inner shock that focuses towards the center. A few nanoseconds after the converging shock reaches the focus and diverges away from the center, a single bubble nucleates at the center. The inner diverging shock then reaches the surface of the annular laser-induced bubble and reflects at the boundary, initiating nucleation of a tertiary bubble cloud. In the present experiments, we have performed time-resolved imaging of shock propagation and bubble wall motion. Our experimental observations of single-bubble cavitation and collapse and appearance of ring-shaped bubble clouds are consistent with our numerical simulations that solve a one dimensional Euler equation in cylindrical coordinates. The numerical results agree qualitatively with the experimental observations of the appearance and growth of bubble clouds at the smallest laser excitation rings. Our technique of shock-driven bubble cavitation opens novel perspectives for the investigation of shock-induced single-bubble or multi-bubble cavitation phenomena in thin liquids.

cond-mat.soft↗

arXiv2017

Contact-based and spheroidal vibrational modes of a hexagonal monolayer of microspheres on a substrate

We study acoustic modes of a close-packed hexagonal lattice of spheres adhered to a substrate, propagating along a high-symmetry direction. The model, accounting for both normal and shear coupling between the spheres and between the spheres and the substrate, yields three contact-based vibrational modes involving both translational and rotational motion of the spheres. Furthermore, we study the effect of sphere-substrate and sphere-sphere contacts on spheroidal vibrational modes of the spheres within a perturbative approach. The sphere-substrate interaction results in a frequency upshift for the modes having a non-zero displacement at the contact point with the substrate. Sphere-sphere interactions result in dispersion of spheroidal modes turning them into propagating waves, albeit with a small group velocity. Analytical dispersion relations for both contact-based and spheroidal modes are presented and compared with results obtained for a square lattice.

physics.class-ph↗

arXiv2016

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO$_3$

The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply sub-picosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO$_3$ ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond timescales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables direct comparison with first-principles-based molecular dynamics simulations, with good agreement obtained.

cond-mat.mtrl-sci↗

arXiv2016

Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide

Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.

cond-mat.str-el↗

arXiv2015

What is the Brillouin Zone of an Anisotropic Photonic Crystal?

The concept of the Brillouin zone (BZ) in relation to a photonic crystal fabricated in an optically anisotropic material is explored both experimentally and theoretically. In experiment, we used femtosecond laser pulses to excite THz polaritons and image their propagation in lithium niobate and lithium tantalate photonic crystal (PhC) slabs. We directly measured the dispersion relation inside PhCs and observed that the lowest bandgap expected to form at the BZ boundary forms inside the BZ in the anisotropic lithium niobate PhC. Our analysis shows that in an anisotropic material the BZ - defined as the Wigner-Seitz cell in the reciprocal lattice - is no longer bounded by Bragg planes and thus does not conform to the original definition of the BZ by Brillouin. We construct an alternative Brillouin zone defined by Bragg planes and show its utility in identifying features of the dispersion bands. We show that for an anisotropic 2D PhC without dispersion, the Bragg plane BZ can be constructed by applying the Wigner-Seitz method to a stretched or compressed reciprocal lattice. We also show that in the presence of the dispersion in the underlying material or in a slab waveguide, the Bragg planes are generally represented by curved surfaces rather than planes. The concept of constructing a BZ with Bragg planes should prove useful in understanding the formation of dispersion bands in anisotropic PhCs and in selectively tailoring their optical properties.

physics.optics↗

arXiv2014

Lattice swelling and modulus change in a helium-implanted tungsten alloy: X-ray micro-diffraction, surface acoustic wave measurements, and multiscale modelling

Using X-ray micro-diffraction and surface acoustic wave spectroscopy, we measure lattice swelling and elastic modulus changes in a W-1%Re alloy after implantation with 3110 appm of helium. A fraction of a percent observed lattice expansion gives rise to an order of magnitude larger reduction in the surface acoustic wave velocity. A multiscale elasticity, molecular dynamics, and density functional theory model is applied to the interpretation of observations. The measured lattice swelling is consistent with the relaxation volume of self-interstitial and helium-filled vacancy defects that dominate the helium-implanted material microstructure. Molecular dynamics simulations confirm the elasticity model for swelling. Elastic properties of the implanted surface layer also change due to defects. The reduction of surface acoustic wave velocity predicted by density functional theory calculations agrees remarkably well with experimental observations.

cond-mat.mtrl-sci↗

arXiv2013

Detection of shorter-than-skin-depth acoustic pulses in a metal film via transient reflectivity

The detection of ultrashort laser-generated acoustic pulses at a metal surface and the reconstruction of the acoustic strain profile are investigated. A 2 ps-long acoustic pulse generated in an SrRuO$_{3}$ layer propagates through an adjacent gold layer and is detected at its surface by a reflected probe pulse. We show that the intricate shape of the transient reflectivity waveform and the ability to resolve acoustic pulses shorter than the optical skin depth are controlled by a single parameter, which is determined by the ratio of the real and imaginary parts of the photoelastic constant of the material. We also demonstrate a Fourier transform-based algorithm that can be used to extract acoustic strain profiles from transient reflectivity measurements.

cond-mat.mtrl-sci↗

arXiv2013

Interaction of a Contact Resonance of Microspheres with Surface Acoustic Waves

We study the interaction of surface acoustic waves (SAWs) with the contact-based, axial vibrational resonance of 1 μm silica microspheres forming a two-dimensional granular crystal adhered to a substrate. The laser-induced transient grating technique is used to excite SAWs and measure their dispersion. The measured dispersion curves exhibit "avoided crossing" behavior due to the hybridization of the SAWs with the microsphere resonance. We compare the measured dispersion curves with those predicted by our analytical model, and find excellent agreement. The approach presented can be used to study the contact mechanics and adhesion of micro- and nanoparticles as well as the dynamics of microscale granular crystals.

cond-mat.mes-hall↗