arXiv subjects

Keith A. Nelson

Publications and source records attributed to Keith A. Nelson.

At least 55 records · Page 3Linked to original sources

arXiv2020

Room Temperature Terahertz Electroabsorption Modulation by Excitons in Monolayer Transition Metal Dichalcogenides

The interaction between off-resonant laser pulses and excitons in monolayer transition metal dichalcogenides is attracting increasing interest as a route for the valley-selective coherent control of the exciton properties. Here, we extend the classification of the known off-resonant phenomena by unveiling the impact of a strong THz field on the excitonic resonances of monolayer MoS$_2$. We observe that the THz pump pulse causes a selective modification of the coherence lifetime of the excitons, while keeping their oscillator strength and peak energy unchanged. We rationalize these results theoretically by invoking a hitherto unobserved manifestation of the Franz-Keldysh effect on an exciton resonance. As the modulation depth of the optical absorption reaches values as large as 0.05 dB/nm at room temperature, our findings open the way to the use of semiconducting transition metal dichalcogenides as compact and efficient platforms for high-speed electroabsorption devices.

cond-mat.mes-hall↗

arXiv2020

Pressure-Thresholded Response in Cylindrically Shocked Cyclotrimethylene Trinitramine (RDX)

We demonstrate a strongly thresholded response in cyclotrimethylene trinitramine (RDX) when it is cylindrically shocked using a novel waveguide geometry. Using ultrafast single-shot multi-frame imaging, we demonstrate that <100-μm diameter single crystals of RDX embedded in a polymer host deform along preferential planes for >100 ns after the shock first arrives in the crystal. We use in-situ imaging and time-resolved photoemission to demonstrate that short-lived chemistry occurs with complex deformation pathways. Using scanning electron microscopy and ultrasmall-angle X-ray scattering, we demonstrate that the shock-induced dynamics leave behind porous crystals, with pore shapes and sizes that change significantly with shock energy. A threshold pressure of ~ 12 GPa at the center of convergence separated the single-mode planar crystal deformations from the chemistry-coupled multi-plane dynamics at higher pressures. Our observations indicate preferential directions for deformation for our cylindrically shocked system, despite the applied stress along many different crystallographic planes.

cond-mat.mtrl-sci↗

arXiv2019

Laser-Driven High-Velocity Microparticle Launcher In Atmosphere And Under Vacuum

This paper presents a novel approach to launch single microparticles at high velocities under low vacuum conditions. In an all-optical table-top method, microparticles with sizes ranging from a few microns to tens of microns are accelerated to supersonic velocities depending on the particle mass. The acceleration is performed through a laser ablation process and the particles are monitored in free space using an ultra-high-speed multi-frame camera with nanosecond time resolution. Under low vacuum, we evaluate the current platform performance by measuring particle velocities for a range of particle types and sizes, and demonstrate blast wave suppression and drag reduction under vacuum. Showing an impact on polyethylene, we demonstrate the capability of the experimental setup to study materials behavior under high-velocity impact. The present method is relevant to space applications, particularly to rendezvous missions where velocities range from tens of m/s to a few km/s, as well as to a wide range of terrestrial applications including impact bonding and impact-induced erosion.

astro-ph.IM↗

arXiv2019

Terahertz generation by beamlet superposition

We analytically show how a superposition of beamlets produces terahertz radiation with greater spatial homogeneity and efficiency compared to tilted-pulse-fronts generated by diffraction gratings. The advantages are particularly notable for large pump bandwiths and beam sizes, alluding to better performance in the presence of cascading effects and higher energy pumping. A theory of terahertz generation using a superposition of beamlets is developed. It is shown how such an arrangement produces a distortion free tilted-pulse-front. Closed form expressions for terahertz spectra and transients in three spatial dimensions are derived. Conditions for obtaining performance parity and bounds for optimal parameters are furnished.

physics.optics↗

arXiv2019

Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films

Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $\mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2\ \mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase.

cond-mat.str-el↗

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↗

arXiv2018

Terahertz-Field-Induced Ferroelectricity in Quantum Paraelectric SrTiO$_3$

"Hidden phases" are metastable collective states of matter that are typically not accessible on equilibrium phase diagrams. These phases can host exotic properties in otherwise conventional materials and hence may enable novel functionality and applications, but their discovery and access are still in early stages. Using intense terahertz electric field excitation, we show that an ultrafast phase transition into a hidden ferroelectric phase can be dynamically induced in the quantum paraelectric SrTiO$_3$. The induced lowering in crystal symmetry yields dramatic changes in the phonon excitation spectra. Our results demonstrate collective coherent control over material structure, in which a single-cycle field drives ions along the microscopic pathway leading directly to their locations in a new crystalline phase on an ultrafast timescale.

cond-mat.mtrl-sci↗

arXiv2018

Time-domain Brillouin Scattering as a Local Temperature Probe in Liquids

We present results of time-domain Brillouin scattering (TDBS) to determine the local temperature of liquids in contact to an optical transducer. TDBS is based on an ultrafast pump-probe technique to determine the light scattering frequency shift caused by the propagation of coherent acoustic waves in a sample. Since the temperature influences the Brillouin scattering frequency shift, the TDBS signal probes the local temperature of the liquid. Results for the extracted Brillouin scattering frequencies recorded at different liquid temperatures and at different laser powers - i.e. different steady state background temperatures- are shown to demonstrate the usefulness of TDBS as a temperature probe. This TDBS experimental scheme is a first step towards the investigation of ultrathin liquids measured by GHz ultrasonic probing.

cond-mat.soft↗

arXiv2018

Terahertz-frequency magnon-phonon-polaritons in the strong coupling regime

Strong coupling between light and matter occurs when the two interact strongly enough to form new hybrid modes called polaritons. Here we report on the strong coupling of both the electric and magnetic degrees of freedom to an ultrafast terahertz (THz) frequency electromagnetic wave. In our system, optical phonons in a slab of ferroelectric lithium niobate (LiNbO$_3$) are strongly coupled to a THz electric field to form phonon-polaritons, which are simultaneously strongly coupled to magnons in an adjacent slab of canted antiferromagnetic erbium orthoferrite (ErFeO$_3$) via the THz magnetic field. The strong coupling leads to the formation of new magnon-phonon-polariton modes, which we experimentally observe in the wavevector-frequency dispersion curve as an avoided crossing and in the time-domain as a normal-mode beating. Our simple yet versatile on-chip waveguide platform provides a promising avenue by which to explore both ultrafast THz spintronics applications and the quantum nature of the interaction.

physics.optics↗

arXiv2017

Real-time observation of a coherent lattice transformation into a high-symmetry phase

Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. Direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations, and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This precludes conventional ultrafast spectroscopy in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we were able to observe the photoinduced phase transition from the semimetallic, low-symmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities was predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10 mJ/cm2 in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for tens of picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration.

cond-mat.mtrl-sci↗

arXiv2017

Development of Single-Shot Multi-Frame Imaging of Cylindrical Shock Waves in a Multi-Layered Assembly

We demonstrate single-shot multi-frame imaging of quasi-2D cylindrically converging shock waves as they propagate through a multi-layer target sample assembly. We visualize the shock with sequences of up to 16 images, using a Fabry-Perot cavity to generate a pulse train that can be used in various imaging configurations. We employ multi-frame shadowgraph and dark-field imaging to measure the amplitude and phase of the light transmitted through the shocked target. Single-shot multi-frame imaging tracks geometric distortion and additional features in our images that were not previously resolvable in this experimental geometry. Analysis of our images, in combination with simulations, shows that the additional image features are formed by a coupled wave structure resulting from interface effects in our targets. This technique presents a new capability for tabletop imaging of shock waves that can be easily extended to experiments at large-scale facilities.

physics.app-ph↗

arXiv2017

Time-domain Brillouin scattering for the determination of laser-induced temperature gradients in liquids

We present an optical technique based on ultrafast photoacoustics to precisely determine the local temperature distribution profile in liquid samples in contact with a laser heated optical transducer. This ultrafast pump-probe experiment uses time-domain Brillouin scattering (TDBS) to locally determine the light scattering frequency shift. As the temperature influences the Brillouin scattering frequency, the TDBS signal probes the local laser-induced temperature distribution in the liquid. We demonstrate the relevance and the sensitivity of this technique for the measurement of the absolute laser-induced temperature gradient of a glass forming liquid prototype, glycerol, at different laser pump powers - i.e. different steady state background temperatures. Complementarily, our experiments illustrate how this TDBS technique can be applied to measure thermal diffusion in complex multilayer systems in contact to a surrounding liquid.

cond-mat.mtrl-sci↗

arXiv2017

Nondiffusive thermal transport from micro/nanoscale sources producing nonthermal phonon populations exceeds Fourier heat conduction

We study nondiffusive thermal transport by phonons at small distances within the framework of the Boltzmann transport equation (BTE) and demonstrate that the transport is significantly affected by the distribution of phonons emitted by the source. We discuss analytical solutions of the steady-state BTE for a source with a sinusoidal spatial profile, as well as for a three- dimensional Gaussian hot spot, and provide numerical results for single crystal silicon at room temperature. If a micro/nanoscale heat source produces a thermal phonon distribution, it gets hotter than predicted by the heat diffusion equation; however, if the source predominantly produces low-frequency acoustic phonons with long mean free paths, it may get significantly cooler than predicted by the heat equation, yielding an enhanced heat transport.

cond-mat.mes-hall↗

arXiv2017

Observation of Bulk Fermi Arc and Polarization Half Charge from Paired Exceptional Points

The ideas of topology have found tremendous success in Hermitian physical systems, but even richer properties exist in the more general non-Hermitian framework. Here, we theoretically propose and experimentally demonstrate a new topologically-protected bulk Fermi arc which---unlike the well-known surface Fermi arcs arising from Weyl points in Hermitian systems---develops from non-Hermitian radiative losses in photonic crystal slabs. Moreover, we discover half-integer topological charges in the polarization of far-field radiation around the Fermi arc. We show that both phenomena are direct consequences of the non-Hermitian topological properties of exceptional points, where resonances coincide in their frequencies and linewidths. Our work connects the fields of topological photonics, non-Hermitian physics and singular optics, and paves the way for future exploration of non-Hermitian topological systems.

physics.optics↗

arXiv2017

Machine Learning to Analyze Images of Shocked Materials for Precise and Accurate Measurements

A supervised machine learning algorithm, called locally adaptive discriminant analysis (LADA), has been developed to locate boundaries between identifiable image features that have varying intensities. LADA is an adaptation of image segmentation, which includes techniques that find the positions of image features (classes) using statistical intensity distributions for each class in the image. In order to place a pixel in the proper class, LADA considers the intensity at that pixel and the distribution of intensities in local (nearby) pixels. This paper presents the use of LADA to provide, with statistical uncertainties, the positions and shapes of features within ultrafast images of shock waves. We demonstrate the ability to locate image features including crystals, density changes associated with shock waves, and material jetting caused by shock waves. This algorithm can analyze images that exhibit a wide range of physical phenomena because it does not rely on comparison to a model. LADA enables analysis of images from shock physics with statistical rigor independent of underlying models or simulations

physics.app-ph↗

arXiv2017

Rapid and Precise Determination of Zero-Field Splittings by Terahertz Time-Domain Electron Paramagnetic Resonance Spectroscopy

Zero-field splitting (ZFS) parameters are fundamentally tied to the geometries of metal ion complexes. Despite their critical importance for understanding the magnetism and spectroscopy of metal complexes, they are not routinely available through general laboratory-based techniques, and are often inferred from magnetism data. Here we demonstrate a simple tabletop experimental approach that enables direct and reliable determination of ZFS parameters in the terahertz (THz) regime. We report time-domain measurements of electron paramagnetic resonance (EPR) signals associated with THz-frequency ZFSs in molecular complexes containing high-spin transition-metal ions. We measure the temporal profiles of the free-induction decays of spin resonances in the complexes at zero and nonzero external magnetic fields, and we derive the EPR spectra via numerical Fourier transformation of the time-domain signals. In most cases, absolute values of the ZFS parameters are extracted from the measured zero-field EPR frequencies, and the signs can be determined by zero-field measurements at two different temperatures. Field-dependent EPR measurements further allow refined determination of the ZFS parameters and access to the g-factor. The results show good agreement with those obtained by other methods. The simplicity of the method portends wide applicability in chemistry, biology and material science.

physics.chem-ph↗

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↗

arXiv2017

Direct Test of Supercooled Liquid Scaling Relations

Diverse material classes exhibit practically identical behavior when made viscous upon cooling toward the glass transition, suggesting a common theoretical basis. The first-principles scaling laws that have been proposed to describe the evolution with temperature have yet to be appropriately tested due to the extraordinary range of time scales involved. We used seven different measurement methods to determine the structural relaxation kinetics of a prototype molecular glass former over a temporal range of 13 decades and over a temperature range spanning liquid to glassy states. For the material studied, our results comprise a comprehensive validation of the two scaling relations that are central to the fundamental question of whether supercooled liquid dynamics can be described universally. The ultrabroadband mechanical measurements demonstrated have fundamental and practical applications in polymer science, geophysics, multifunctional materials, and other areas.

cond-mat.soft↗