arXiv subjects

Keith A. Nelson

Publications and source records attributed to Keith A. Nelson.

At least 73 records · Page 4Linked to original sources

arXiv2016

Supersonic Impact of Metallic Micro-particles

Understanding material behavior under high velocity impact is the key to addressing a variety of fundamental questions in areas ranging from asteroid strikes and geological cratering to impact-induced phase transformations, spallation, wear, and ballistic penetration. Recently, adhesion has emerged in this spectrum since it has been found that micrometer-sized metallic particles can bond to metallic substrates under supersonic-impact conditions. However, the mechanistic aspects of impact-induced adhesion are still unresolved. Here we study supersonic impact of individual metallic microparticles on substrates with micro-scale and nanosecond-level resolution. This permits the first direct observation of a material-dependent threshold velocity, above which the particle undergoes impact-induced material ejection and adheres to the substrate. Our finite element simulations reveal that prevailing theories of impact-induced shear localization and melting cannot account for the material ejection. Rather, it originates from the propagation of a pressure wave induced upon impact. The experiments and simulations together establish that the critical adhesion velocity for supersonic microparticles is proportional to the bulk speed of sound.

cond-mat.mtrl-sci↗

arXiv2016

Bose-Einstein Condensation of Long-Lifetime Polaritons in Thermal Equilibrium

Exciton-polaritons in semiconductor microcavities have been used to demonstrate quantum effects such as Bose-Einstein condensation, superfluity, and quantized vortices. However, in these experiments, the polaritons have not reached thermal equilibrium when they undergo the transition to a coherent state. This has prevented the verification of one of the canonical predictions for condensation, namely the phase diagram. In this work, we have created a polariton gas in a semiconductor microcavity in which the quasiparticles have a lifetime much longer than their thermalization time. This allows them to reach thermal equilibrium in a laser-generated confining trap. Their energy distributions are well fit by equilibrium Bose-Einstein distributions over a broad range of densities and temperatures from very low densities all the way up to the threshold for Bose-Einstein condensation. The good fits of the Bose-Einstein distribution over a broad range of density and temperature imply that the particles obey the predicted power law for the phase boundary of Bose-Einstein condensation.

cond-mat.quant-gas↗

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↗

arXiv2016

Terahertz-driven Luminescence and Colossal Stark Effect in CdSe:CdS Colloidal Quantum Dots

Unique optical properties of colloidal semiconductor quantum dots (QDs), arising from quantum mechanical confinement of charge within these structures, present a versatile testbed for the study of how high electric fields affect the electronic structure of nanostructured solids. Earlier studies of quasi-DC electric field modulation of QD properties have been limited by the electrostatic breakdown processes under the high externally applied electric fields, which have restricted the range of modulation of QD properties. In contrast, in the present work we drive CdSe:CdS core:shell QD films with high-field THz-frequency electromagnetic pulses whose duration is only a few picoseconds. Surprisingly, in response to the THz excitation we observe QD luminescence even in the absence of an external charge source. Our experiments show that QD luminescence is associated with a remarkably high and rapid modulation of the QD band-gap, which is changing by more than 0.5 eV (corresponding to 25% of the unperturbed bandgap energy) within the picosecond timeframe of THz field profile. We show that these colossal energy shifts can be consistently explained by the quantum confined Stark effect. Our work demonstrates a route to extreme modulation of material properties without configurational changes in material sets or geometries. Additionally, we expect that this platform can be adapted to a novel compact THz detection scheme where conversion of THz fields (with meV-scale photon energies) to the visible/near-IR band (with eV-scale photon energies) can be achieved at room temperature with high bandwidth and sensitivity.

physics.optics↗

arXiv2016

Two-dimensional terahertz magnetic resonance spectroscopy of collective spin waves

Nonlinear manipulation of nuclear and electron spins is the basis for all advanced methods in magnetic resonance including multidimensional nuclear magnetic and electron spin resonance spectroscopies, magnetic resonance imaging, and in recent years, quantum control over individual spins. The methodology is facilitated by the ease with which the regime of strong coupling can be reached between radiofrequency or microwave magnetic fields and nuclear or electron spins respectively, typified by sequences of magnetic pulses that control the magnetic moment directions. The capabilities meet a bottleneck, however, for far-infrared magnetic resonances characteristic of correlated electron materials, molecular magnets, and proteins that contain high-spin transition metal ions. Here we report the development of two-dimensional terahertz magnetic resonance spectroscopy and its use for direct observation of the nonlinear responses of collective spin waves (magnons). The spectra show magnon spin echoes and 2-quantum signals that reveal pairwise correlations between magnons at the Brillouin zone center. They also show resonance-enhanced second-harmonic and difference-frequency signals. Our methods are readily generalizable to multidimensional magnetic resonance spectroscopy and nonlinear coherent control of terahertz-frequency spin systems in molecular complexes, biomolecules, and materials.

cond-mat.mtrl-sci↗

arXiv2016

Nonlinear two-dimensional terahertz photon echo and rotational spectroscopy in the gas phase

Ultrafast two-dimensional spectroscopy utilizes correlated multiple light-matter interactions for retrieving dynamic features that may otherwise be hidden under the linear spectrum. Its extension to the terahertz regime of the electromagnetic spectrum, where a rich variety of material degrees of freedom reside, remains an experimental challenge. Here we report ultrafast two-dimensional terahertz spectroscopy of gas-phase molecular rotors at room temperature. Using time-delayed terahertz pulse pairs, we observe photon echoes and other nonlinear signals resulting from molecular dipole orientation induced by three terahertz field-dipole interactions. The nonlinear time-domain orientation signals are mapped into the frequency domain in two-dimensional rotational spectra which reveal J-state-resolved nonlinear rotational dynamics. The approach enables direct observation of correlated rotational transitions and may reveal rotational coupling and relaxation pathways in the ground electronic and vibrational state.

physics.atom-ph↗

arXiv2016

Variational Approach to Solving the Spectral Boltzmann Transport Equation in Transient Thermal Grating for Thin Films

The phonon Boltzmann transport equation (BTE) is widely utilized to study non-diffusive thermal transport. We find a solution of the BTE in the thin film transient thermal grating (TTG) experimental geometry by using a recently developed variational approach with a trial solution supplied by the Fourier heat conduction equation. We obtain an analytical expression for the thermal decay rate that shows excellent agreement with Monte Carlo simulations. We also obtain a closed form expression for the effective thermal conductivity that demonstrates the full material property and heat transfer geometry dependence, and recovers the limits of the one-dimensional TTG expression for very thick films and the Fuchs-Sondheimer expression for very large grating spacings. The results demonstrate the utility of the variational technique for analyzing non-diffusive phonon-mediated heat transport for nanostructures in multi-dimensional transport geometries, and will assist the probing of the mean free path (MFP) distribution of materials via transient grating experiments.

cond-mat.mes-hall↗

arXiv2016

How two-dimensional brick layer J-aggregates differ from linear ones: excitonic properties and line broadening mechanisms

We study the excitonic coupling and homogeneous spectral line width of brick layer J-aggregate films. We begin by analysing the structural information revealed by the two-exciton states probed in two-dimensional spectra. Our first main result is that the relation between the excitonic couplings and the spectral shift in a two-dimensional structure is different (larger shift for the same nearest neighbour coupling) from that in a one-dimensional structure, which leads to an estimation of dipolar coupling in two-dimensional lattices. We next investigate the mechanisms of homogeneous broadening - population relaxation and pure dephasing - and evaluate their relative importance in linear and two-dimensional aggregates. Our second main result is that pure dephasing dominates the line width in two-dimensional systems up to a crossover temperature, which explains the linear temperature dependence of the homogeneous line width. This is directly related to the decreased density of states at the band edge when compared with linear aggregates, thus reducing the contribution of population relaxation to dephasing. Pump-probe experiments are suggested to directly measure the lifetime of the bright state and can therefore support the proposed model.

physics.chem-ph↗

arXiv2016

Nonlinear acousto-magneto-plasmonics

We review the recent progress in experimental and theoretical research of interactions between the acoustic, magnetic and plasmonic transients in hybrid metal-ferromagnet multilayer structures excited by ultrashort laser pulses. The main focus is on understanding the nonlinear aspects of the acoustic dynamics in materials as well as the peculiarities in the nonlinear optical and magneto-optical response. For example, the nonlinear optical detection is illustrated in details by probing the static magneto-optical second harmonic generation in gold-cobalt-silver trilayer structures in Kretschmann geometry. Furthermore, we show experimentally how the nonlinear reshaping of giant ultrashort acoustic pulses propagating in gold can be quantified by time-resolved plasmonic interferometry and how these ultrashort optical pulses dynamically modulate the optical nonlinearities. The effective medium approximation for the optical properties of hybrid multilayers facilitates the understanding of novel optical detection techniques. In the discussion we highlight recent works on the nonlinear magneto-elastic interactions, and strain-induced effects in semiconductor quantum dots.

cond-mat.mes-hall↗

arXiv2016

Monte Carlo Study of Non-diffusive Relaxation of A Transient Thermal Grating in Thin Membranes

The impact of boundary scattering on non-diffusive thermal relaxation of a transient grating in thin membranes is rigorously analyzed using the multidimensional phonon Boltzmann equation. The gray Boltzmann simulation results indicate that approximating models derived from previously reported one-dimensional relaxation model and Fuchs-Sondheimer model fail to describe the thermal relaxation of membranes with thickness comparable with phonon mean free path. Effective thermal conductivities from spectral Boltzmann simulations completely free of any fitting parameters are shown to agree reasonably well with experimental results. These findings are important for improving our fundamental understanding of non-diffusive thermal transport in membranes and other nanostructures.

cond-mat.mes-hall↗

arXiv2016

Stable Switching among High-Order Modes in Polariton Condensates

We report multistate optical switching among high-order bouncing-ball modes ("ripples") and whispering-gallerying modes ("petals") of exciton-polariton condensates in a laser-generated annular trap. By tailoring the diameter and power of the annular trap, the polariton condensate can be switched among different trapped modes, accompanied by redistribution of spatial densities and superlinear increase in the emission intensities, implying that polariton condensates in this geometry could be exploited for a multistate switch. A model based on non-Hermitian modes of the generalized Gross-Pitaevskii equation reveals that this mode switching arises from competition between pump-induced gain and in-plane polariton loss. The parameters for reproducible switching among trapped modes have been measured experimentally, giving us a phase diagram for mode switching. Taken together, the experimental result and theoretical modeling advances our fundamental understanding of the spontaneous emergence of coherence and move us toward its practical exploitation.

cond-mat.mes-hall↗

arXiv2015

THz generation using a reflective stair-step echelon

We present a novel method for THz generation in lithium niobate using a reflective stair-step echelon structure. The echelon produces a discretely tilted pulse front with less angular dispersion compared to a high groove-density grating. The THz output was characterized using both a 1-lens and 3-lens imaging system to set the tilt angle at room and cryogenic temperatures. Using broadband 800 nm pulses with a pulse energy of 0.95 mJ and a pulse duration of 70 fs (24 nm FWHM bandwidth, 39 fs transform limited width), we produced THz pulses with field strengths as high as 500 kV/cm and pulse energies as high as 3.1 $μ$J. The highest conversion efficiency we obtained was 0.33%. In addition, we find that the echelon is easily implemented into an experimental setup for quick alignment and optimization.

physics.optics↗

arXiv2015

Cooperative photoinduced metastable phase control in strained manganite films

A major challenge in condensed matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic-lattice coupling that, in turn, stabilize the metallic phase. These results reveal that strain engineering can tune emergent functionality towards proximal macroscopic states to enable dynamic ultrafast optical phase switching and control.

cond-mat.str-el↗

arXiv2015

A Variational Approach to Extracting the Phonon Mean Free Path Distribution from the Spectral Boltzmann Transport Equation

The phonon Boltzmann transport equation (BTE) is a powerful tool for studying non-diffusive thermal transport. Here, we develop a new universal variational approach to solving the BTE that enables extraction of phonon mean free path (MFP) distributions from experiments exploring non-diffusive transport. By utilizing the known Fourier solution as a trial function, we present a direct approach to calculating the effective thermal conductivity from the BTE. We demonstrate this technique on the transient thermal grating (TTG) experiment, which is a useful tool for studying non-diffusive thermal transport and probing the mean free path (MFP) distribution of materials. We obtain a closed form expression for a suppression function that is materials dependent, successfully addressing the non-universality of the suppression function used in the past, while providing a general approach to studying thermal properties in the non-diffusive regime.

cond-mat.mes-hall↗

arXiv2015

Transient terahertz photoconductivity measurements of minority-carrier lifetime in tin sulfide thin films: Advanced metrology for an early-stage photovoltaic material

Materials research with a focus on enhancing the minority-carrier lifetime of the light-absorbing semiconductor is key to advancing solar energy technology for both early-stage and mature material platforms alike. Tin sulfide (SnS) is an absorber material with several clear advantages for manufacturing and deployment, but the record power conversion efficiency remains below 5%. We report measurements of bulk and interface minority-carrier recombination rates in SnS thin films using optical-pump, terahertz (THz)-probe transient photoconductivity (TPC) measurements. Post-growth thermal annealing in H_2S gas increases the minority-carrier lifetime, and oxidation of the surface reduces the surface recombination velocity. However, the minority-carrier lifetime remains below 100 ps for all tested combinations of growth technique and post-growth processing. Significant improvement in SnS solar cell performance will hinge on finding and mitigating as-yet-unknown recombination-active defects. We describe in detail our methodology for TPC experiments, and we share our data analysis routines as freely-available software.

cond-mat.mtrl-sci↗

arXiv2015

Polaritons are Not Weakly Interacting: Direct Measurement of the Polariton-Polariton Interaction Strength

Exciton-polaritons in a microcavity are composite two-dimensional bosonic quasiparticles, arising from the strong coupling between confined light modes in a resonant planar optical cavity and excitonic transitions, typically using excitons in semiconductor quantum wells (QWs) placed at the antinodes of the same cavity. Quantum phenomena such as Bose-Einstein condensation (BEC), quantized vortices, and macroscopic quantum states have been reported at temperatures from tens of Kelvin up to room temperatures, and polaritonic devices such as spin switches \cite{Amo2010} and optical transistors have also been reported. Many of these effects of exciton-polaritons depend crucially on the polariton-polariton interaction strength. Despite the importance of this parameter, it has been difficult to make an accurate experimental measurement, mostly because of the difficulty of determining the absolute densities of polaritons and bare excitons. Here we report the direct measurement of the polariton-polariton interaction strength in a very high-Q microcavity structure. By allowing polaritons to propagate over 40 $μ$m to the center of a laser-generated annular trap, we are able to separate the polariton-polariton interactions from polariton-exciton interactions. The interaction strength is deduced from the energy renormalization of the polariton dispersion as the polariton density is increased, using the polariton condensation as a benchmark for the density. We find that the interaction strength is about two orders of magnitude larger than previous theoretical estimates, putting polaritons squarely into the strongly-interacting regime. When there is a condensate, we see a sharp transition to a different dependence of the renormalization on the density, which is evidence of many-body effects.

cond-mat.quant-gas↗

arXiv2015

Non-Contact Measurement of Thermal Diffusivity in Ion-Implanted Nuclear Materials

Knowledge of mechanical and physical property evolution due to irradiation damage is essential for the development of future fission and fusion reactors. Ion-irradiation provides an excellent proxy for studying irradiation damage, allowing high damage doses without sample activation. Limited ion-penetration-depth means that only few-micron-thick damaged layers are produced. Substantial effort has been devoted to probing the mechanical properties of these thin implanted layers. Yet, whilst key to reactor design, their thermal transport properties remain largely unexplored due to a lack of suitable measurement techniques. Here we demonstrate non-contact thermal diffusivity measurements in ion-implanted tungsten for nuclear fusion armour. Alloying with transmutation elements and the interaction of retained gas with implantation-induced defects both lead to dramatic reductions in thermal diffusivity. These changes are well captured by our modelling approaches. Our observations have important implications for the design of future fusion power plants.

cond-mat.mtrl-sci↗

arXiv2015

From populations to coherences and back again: a new insight about rotating dipoles

The process in which light is absorbed by an ensemble of molecules obeys the fundamental law of conservation of energy - the energy removed from the light resides in the molecular degrees of freedom. In the process of coherent emission from excited molecules known as free-induction decay (FID), spectroscopic measurements of the emitted radiation are often conducted in order to gain insight into molecular structure and behavior. However, the direct influence of the FID emission on its molecular source is not measured directly. In this work we present experimental evidence from the molecular rotor perspective of the consequences of terahertz-frequency FID emission from rotationally excited molecules. We show that when gas phase molecules transiently orient under field-free conditions, the energy radiated via FID is manifest as an abrupt reduction in excited rotational populations. The connection between coherent FID emission and stored energy leaves a particularly distinct signature in our measurements, but the results are generalizable throughout coherent spectroscopy and coherent control.

physics.atom-ph↗