arXiv subjects

Keith A. Nelson

Publications and source records attributed to Keith A. Nelson.

At least 91 records · Page 5Linked to original sources

arXiv2014

Reconstructing phonon mean free path contributions to thermal conductivity using nanoscale membranes

Knowledge of the mean free path distribution of heat-carrying phonons is key to understanding phonon-mediated thermal transport. We demonstrate that thermal conductivity measurements of thin membranes spanning a wide thickness range can be used to characterize how bulk thermal conductivity is distributed over phonon mean free paths. A non-contact transient thermal grating technique was used to measure the thermal conductivity of suspended Si membranes ranging from 15 to 1500 nm in thickness. A decrease in the thermal conductivity from 74% to 13% of the bulk value is observed over this thickness range, which is attributed to diffuse phonon boundary scattering. Due to the well-defined relation between the membrane thickness and phonon mean free path suppression, combined with the range and accuracy of the measurements, we can reconstruct the bulk thermal conductivity accumulation vs. phonon mean free path, and compare with theoretical models.

cond-mat.mes-hall↗

arXiv2014

Nonlinear Acoustics at GHz Frequencies in a Viscoelastic Fragile Glass Former

Using a picosecond pump-probe ultrasonic technique, we study the propagation of high-amplitude, laser-generated longitudinal coherent acoustic pulses in the viscoelastic fragile glass former DC704. We observe an increase of almost ten percent in acoustic pulse propagation speed of its leading shock front at the highest optical pump fluence which is a result of the supersonic nature of nonlinear propagation in the viscous medium. From our measurement we deduce the nonlinear acoustic parameter of the glass former in the GHz frequency range across the glass transition temperature.

cond-mat.mtrl-sci↗

arXiv2013

Coherent exciton dynamics in supramolecular light-harvesting nanotubes revealed by ultrafast quantum process tomography

Long-lived exciton coherences have been recently observed in photosynthetic complexes via ultrafast spectroscopy, opening exciting possibilities for the study and design of coherent exciton transport. Yet, ambiguity in the spectroscopic signals has led to arguments for interpreting them in terms of the exciton dynamics, demanding more stringent tests. We propose a novel strategy, Quantum Process Tomography (QPT) for ultrafast spectroscopy, to reconstruct the evolving quantum state of excitons in double-walled supramolecular light-harvesting nanotubes at room temperature. The protocol calls for eight transient grating experiments with varied pulse spectra. Our analysis reveals unidirectional energy transfer from the outer to the inner wall excitons, absence of nonsecular processes, and an unexpected coherence between those two states lasting about 150 femtoseconds, indicating weak electronic coupling between the walls. Our work constitutes the first experimental QPT in a 'warm' and complex system, and provides an elegant scheme to maximize information from ultrafast spectroscopy experiments.

quant-ph↗

arXiv2012

Femtosecond nonlinear ultrasonics in gold probed with ultrashort surface plasmons

Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for unambiguous characterization of arbitrary ultrafast acoustic transients. The giant acoustic pulses experience substantial nonlinear reshaping already after a propagation distance of 100 nm in a crystalline gold layer. Excellent agreement with the Korteveg-de Vries model points to future quantitative nonlinear femtosecond THz-ultrasonics at the nano-scale in metals at room temperature.

physics.optics↗

arXiv2012

Lifetime of sub-THz coherent acoustic phonons in a GaAs-AlAs superlattice

We measure the lifetime of the zone-center 340 GHz longitudinal phonon mode in a GaAs-AlAs superlattice excited and probed with femtosecond laser pulses. By comparing measurements conducted at room temperature and liquid nitrogen temperature we separate the intrinsic (phonon-phonon scattering) and extrinsic contributions to phonon relaxation. The estimated room temperature intrinsic lifetime of 0.95 ns is compared to available calculations and experimental data for bulk GaAs. We conclude that ~0.3 THz phonons are in the transition zone between Akhiezer and Landau-Rumer regimes of phonon-phonon relaxation at room temperature.

cond-mat.mes-hall↗

arXiv2012

Nonlinear terahertz metamaterials via field-enhanced carrier dynamics in GaAs

We demonstrate nonlinear metamaterial split ring resonators (SRRs) on GaAs at terahertz frequencies. For SRRs on doped GaAs films, incident terahertz radiation with peak fields of ~20 - 160 kV/cm drives intervalley scattering. This reduces the carrier mobility and enhances the SRR LC response due to a conductivity decrease in the doped thin film. Above ~160 kV/cm, electric field enhancement within the SRR gaps leads to efficient impact ionization, increasing the carrier density and the conductivity which, in turn, suppresses the SRR resonance. We demonstrate an increase of up to 10 orders of magnitude in the carrier density in the SRR gaps on semi-insulating GaAs substrate. Furthermore, we show that the effective permittivity can be swept from negative to positive values with increasing terahertz field strength in the impact ionization regime, enabling new possibilities for nonlinear metamaterials.

physics.optics↗

arXiv2012

Direct Measurement of Room Temperature Non-diffusive Thermal Transport Over Micron Distances in a Silicon Membrane

The "textbook" phonon mean free path (MFP) of heat carrying phonons in silicon at room temperature is ~40 nm. However, a large contribution to the thermal conductivity comes from low-frequency phonons with much longer MFPs. We present a simple experiment demonstrating that room temperature thermal transport in Si significantly deviates from the diffusion model already at micron distances. Absorption of crossed laser pulses in a freestanding silicon membrane sets up a sinusoidal temperature profile that is monitored via diffraction of a probe laser beam. By changing the period of the thermal grating we vary the heat transport distance within the range ~1-10 μm. At small distances, we observe a reduction in the effective thermal conductivity indicating a transition from the diffusive to the ballistic transport regime for the low-frequency part of the phonon spectrum.

cond-mat.mtrl-sci↗

arXiv2011

Phase-controlled, heterodyne laser-induced transient grating measurements of thermal transport properties in opaque material

The methodology for a heterodyned laser-induced transient thermal grating technique for non-contact, non-destructive measurements of thermal transport in opaque material is presented. Phase-controlled heterodyne detection allows us to isolate pure phase or amplitude transient grating signal contributions by varying the relative phase between reference and probe beams. The phase grating signal includes components associated with both transient reflectivity and surface displacement whereas the amplitude grating contribution is governed by transient reflectivity alone. By analyzing the latter with the two-dimensional thermal diffusion model, we extract the in-plane thermal diffusivity of the sample. Measurements on a 5 μm thick single crystal PbTe film yielded excellent agreement with the model over a range of grating periods from 1.6 to 2.8 μm. The measured thermal diffusivity of 1.3 \times 10-6 m2/s was found to be slightly lower than the bulk value.

cond-mat.other↗

arXiv2011

Onset of non-diffusive phonon transport in transient thermal grating decay

The relaxation of a spatially sinusoidal temperature perturbation in a dielectric crystal at a temperature comparable to or higher than the Debye temperature is investigated theoretically. We assume that most phonons contributing to the specific heat have mean free path (MFP) much shorter than the thermal transport distance and can be described by the thermal diffusion model. Low-frequency phonons that may have MFP comparable to or longer than the grating period are described by the Boltzmann transport equation. These low-frequency phonons are assumed to interact with the thermal reservoir of high frequency phonons but not with each other. Within the single mode relaxation time approximation, an analytical expression for the thermal grating relaxation rate is obtained. We show that the contribution of "ballistic" phonons with long MFP to the effective thermal conductivity governing the grating decay is suppressed compared to their contribution to thermal transport at long distances. The reduction in the effective thermal conductivity in Si at room temperature is found to be significant at grating periods as large as 10 microns.

cond-mat.mtrl-sci↗

arXiv2011

Molecular Orientation by Intense Single Cycle THz Pulses

Intense single-cycle THz pulses resonantly interacting with molecular rotations are shown to induce significant field-free orientation under ambient conditions. We calculate and measure the angular distribution associated with THz-driven rotational motion and correlate the THz-induced orientation and alignment in an OCS gas sample.

physics.chem-ph↗

arXiv2011

$α$-Scale Decoupling of the Mechanical Relaxation and Diverging Shear Wave Propagation Lengthscale in Triphenylphosphite

We have performed depolarized Impulsive Stimulated Scattering experiments to observe shear acoustic phonons in supercooled triphenylphosphite (TPP) from $\sim$10 - 500 MHz. These measurements, in tandem with previously performed longitudinal and shear measurements, permit further analyses of the relaxation dynamics of TPP within the framework of the mode coupling theory (MCT). Our results provide evidence of $α$ coupling between the shear and longitudinal degrees of freedom up to a decoupling temperature $T_c$ = 231 K. A lower bound length scale of shear wave propagation in liquids verified the exponent predicted by theory in the vicinity of the decoupling temperature.

cond-mat.dis-nn↗

arXiv2011

Direct Visualization of Laser-Driven Focusing Shock Waves

Cylindrically or spherically focusing shock waves have been of keen interest for the past several decades. In addition to fundamental study of materials under extreme conditions, cavitation, and sonoluminescence, focusing shock waves enable myriad applications including hypervelocity launchers, synthesis of new materials, production of high-temperature and high-density plasma fields, and a variety of medical therapies. Applications in controlled thermonuclear fusion and in the study of the conditions reached in laser fusion are also of current interest. Here we report on a method for direct real-time visualization and measurement of laser-driven shock generation, propagation, and 2D focusing in a sample. The 2D focusing of the shock front is the consequence of spatial shaping of the laser shock generation pulse into a ring pattern. A substantial increase of the pressure at the convergence of the acoustic shock front is observed experimentally and simulated numerically. Single-shot acquisitions using a streak camera reveal that at the convergence of the shock wave in liquid water the supersonic speed reaches Mach 6, corresponding to the multiple gigapascal pressure range 30 GPa.

cond-mat.mtrl-sci↗

arXiv2011

Nonlinear THz Conductivity Dynamics in CVD-Grown Graphene

We report strong THz-induced transparency in CVD-grown graphene where 92%-96% of the peak-field is transmitted compared to 74% at lower field strength. Time-resolved THz-pump/THz-probe studies reveal that the absorption recovers in 2-3 ps. The induced transparency is believed to arise from nonlinear pumping of carriers in graphene which suppresses the mobility and consequently the conductivity in a spectral region where the light-matter interaction is particularly strong.

cond-mat.mtrl-sci↗

arXiv2009

Terahertz Kerr effect

We have observed optical birefringence in liquids induced by single-cycle THz pulses with field strengths exceeding 100 kV/cm. The induced change in polarization is proportional to the square of the THz electric field. The time-dependent THz Kerr signal is composed of a fast electronic response that follows the individual cycles of the electric field and a slow exponential response associated with molecular orientation.

cond-mat.other↗

arXiv2009

Observation of Nonequilibrium Carrier Distribution in Ge, Si and GaAs by Terahertz-pump--Terahertz-probe Measurements

We compare the observed strong saturation of the free carrier absorption in n-type semiconductors at 300 K in the terahertz frequency range when single-cycle pulses with intensities up to 150 MW/cm2 are used. In the case of germanium, a small increase of the absorption occurs at intermediate THz pulse energies. The recovery of the free carrier absorption was monitored by time-resolved THz-pump/THz-probe measurements. At short probe delay times, the frequency response of germanium cannot be fitted by the Drude model. We attribute these unique phenomena of Ge to dynamical overpopulation of the high mobility gamma conduction band valley.

cond-mat.mtrl-sci↗

arXiv2009

THz-pump -- THz-probe spectroscopy of semiconductors at high field strengths

Pumping n-type GaAs and InSb with ultrafast THz pulses having intensities higher than 150 MW/cm2 shows strong free carrier absorption saturation at temperatures of 300 K and 200 K respectively. If the energy imparted to the carriers exceeds the bandgap, impact ionization processes can occur. The dynamics of carrier cooling in GaAs and impact ionization in InSb were monitored using THz-pump/THz probe spectroscopy which provides both sub-bandgap excitation and probing, eliminating any direct optical electron-hole generation that complicates the evaluation of results in optical pump/THz probe experiments.

cond-mat.mtrl-sci↗

arXiv2008

Impact ionization in InSb probed by THz-pump THz-probe spectroscopy

Picosecond carrier dynamics in indium antimonide (InSb) following excitation by below-bandgap broadband far infrared radiation were investigated at 200 K and 80 K. Using a novel THz-pump/THz-probe scheme with pump THz fields of 100 kV/cm and an intensity of 100 MW/cm^2, we observed carrier heating and impact ionization. The number of carriers produced exceeds 10^16 cm-3, corresponding to a change in carrier density Delta N/N of 700% at 80K. The onset of a well defined absorption peak at 1.2 THz is an indication of changes in LO and LA phonon populations due to cooling of the hot electrons.

cond-mat.mtrl-sci↗

arXiv2008

Nanoconcentration of Terahertz Radiation in Plasmonic Waveguides

Recent years have seen an explosive research and development of nanoplasmonics in the visible and near-infrared (near-ir) frequency regions. One of the most fundamental effects in nanoplasmonics is nano-concentration of optical energy. Plasmonic nanofocusing has been predicted and experimentally achieved. It will be very beneficial for the fundamental science, engineering, environmental, and defense applications to be able to nano-concentrate terahertz radiation (frequency 1 - 10 THz or vacuum wavelength 300 - 30 microns). This will allow for the nanoscale spatial resolution for THz imaging and introduce the THz spectroscopy on the nanoscale, taking full advantage of the rich THz spectra and submicron to nanoscale structures of many engineering, physical, and biological objects of wide interest: electronic components (integrated circuits, etc.), bacteria, their spores, viruses, macromolecules, carbon clusters and nanotubes, etc. In this Letter we establish the principal limits for the nanoconcentration of the THz radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration We predict that the adiabatic compression of THz radiation from the initial spot size of light wavelength to the final size of R = 100 - 250 nm can be achieved with the THz radiation intensity increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for the THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses will allow the observation of nonlinear THz effects and a carrying out a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative.

physics.optics↗