Showing papers by "Keith A. Nelson published in 2016"

Cooperative photoinduced metastable phase control in strained manganite films

Abstract: Strain engineering can ‘hide’ the ordinal ferrometallic state in manganite films, pushing the system to a metastable state, which can then be controlled through photoexcitation.

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

Abstract: Ultrafast 2D spectroscopy uses 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. We report a demonstration of ultrafast 2D 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 multiple terahertz field−dipole interactions. The nonlinear time domain orientation signals are mapped into the frequency domain in 2D rotational spectra that 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.

Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3

Abstract: 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 subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 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 time scales. 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 a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.

Dynamics of supersonic microparticle impact on elastomers revealed by real-time multi-frame imaging.

Abstract: Understanding high–velocity microparticle impact is essential for many fields, from space exploration to medicine and biology. Investigations of microscale impact have hitherto been limited to post–mortem analysis of impacted specimens, which does not provide direct information on the impact dynamics. Here we report real–time multi–frame imaging studies of the impact of 7 μm diameter glass spheres traveling at 700–900 m/s on elastomer polymers. With a poly(urethane urea) (PUU) sample, we observe a hyperelastic impact phenomenon not seen on the macroscale: a microsphere undergoes a full conformal penetration into the specimen followed by a rebound which leaves the specimen unscathed. The results challenge the established interpretation of the behaviour of elastomers under high–velocity impact.

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

Abstract: 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 SnSthin films using optical-pump, terahertz-probe transient photoconductivity (TPC) measurements. Post-growth thermal annealing in H2S 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 SnSsolar 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 in the form freely available software.

Photo-excited charge carriers suppress sub-terahertz phonon mode in silicon at room temperature

Abstract: There is a growing interest in the mode-by-mode understanding of electron and phonon transport for improving energy conversion technologies, such as thermoelectrics and photovoltaics. Whereas remarkable progress has been made in probing phonon–phonon interactions, it has been a challenge to directly measure electron–phonon interactions at the single-mode level, especially their effect on phonon transport above cryogenic temperatures. Here we use three-pulse photoacoustic spectroscopy to investigate the damping of a single sub-terahertz coherent phonon mode by free charge carriers in silicon at room temperature. Building on conventional pump–probe photoacoustic spectroscopy, we introduce an additional laser pulse to optically generate charge carriers, and carefully design temporal sequence of the three pulses to unambiguously quantify the scattering rate of a single-phonon mode due to the electron–phonon interaction. Our results confirm predictions from first-principles simulations and indicate the importance of the often-neglected effect of electron–phonon interaction on phonon transport in doped semiconductors.

THz generation using a reflective stair-step echelon

Abstract: 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 μJ. 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.

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

Abstract: 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-princ...

Nonlinear acousto-magneto-plasmonics

Abstract: 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.

Monte Carlo study of non-diffusive relaxation of a transient thermal grating in thin membranes

Abstract: 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 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.

Increase in elastic anisotropy of single crystal tungsten upon He-ion implantation measured with laser-generated surface acoustic waves

Abstract: We report the experimental observation of an increase in the elastic anisotropy of tungsten upon He-ion implantation, probed optically using transient grating spectroscopy. Surface acoustic wave (SAW) velocity measurements were performed on a (110) oriented tungsten single crystal as a function of in-plane propagation direction for unimplanted and implanted samples. Our measurements allow us to finely resolve the remarkably small elastic anisotropy of the samples investigated. SAW velocity calculations are used to interpret the experimental data and to extract the Zener anisotropy parameter η and the elastic constant C44. Upon ion implantation, we observe an increase in the quantity (η−1) by a factor of 2.6. The surprising increase in elastic anisotropy agrees with previous theoretical predictions based on ab initio calculations of the effect of self-interstitial atoms and He-filled vacancy defects on the elastic properties of tungsten.

Photo-excited charge carriers suppress sub-terahertz phonon mode in silicon at room temperature

Abstract: There is a growing interest in the mode-by-mode understanding of electron and phonon transport for improving energy conversion technologies, such as thermoelectrics and photovoltaics. Whereas remarkable progress has been made in probing phonon–phonon interactions, it has been a challenge to directly measure electron–phonon interactions at the single-mode level, especially their effect on phonon transport above cryogenic temperatures. Here we use three-pulse photoacoustic spectroscopy to investigate the damping of a single sub-terahertz coherent phonon mode by free charge carriers in silicon at room temperature. Building on conventional pump–probe photoacoustic spectroscopy, we introduce an additional laser pulse to optically generate charge carriers, and carefully design temporal sequence of the three pulses to unambiguously quantify the scattering rate of a single-phonon mode due to the electron–phonon interaction. Our results confirm predictions from first-principles simulations and indicate the importance of the often-neglected effect of electron–phonon interaction on phonon transport in doped semiconductors.

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

Abstract: 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.

Interferometric analysis of laser-driven cylindrically focusing shock waves in a thin liquid layer.

Abstract: Shock waves in condensed matter are of great importance for many areas of science and technology ranging from inertially confined fusion to planetary science and medicine. In laboratory studies of shock waves, there is a need in developing diagnostic techniques capable of measuring parameters of materials under shock with high spatial resolution. Here, time-resolved interferometric imaging is used to study laser-driven focusing shock waves in a thin liquid layer in an all-optical experiment. Shock waves are generated in a 10 µm-thick layer of water by focusing intense picosecond laser pulses into a ring of 95 µm radius. Using a Mach-Zehnder interferometer and time-delayed femtosecond laser pulses, we obtain a series of images tracing the shock wave as it converges at the center of the ring before reemerging as a diverging shock, resulting in the formation of a cavitation bubble. Through quantitative analysis of the interferograms, density profiles of shocked samples are extracted. The experimental geometry used in our study opens prospects for spatially resolved spectroscopic studies of materials under shock compression.

Variational approach to extracting the phonon mean free path distribution from the spectral Boltzmann transport equation

Abstract: The phonon Boltzmann transport equation (BTE) is a powerful tool for studying nondiffusive 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 nondiffusive transport. By utilizing the known Fourier heat conduction 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 experiment, which is a useful tool for studying nondiffusive thermal transport and probing the MFP distribution of materials. We obtain a closed form expression for a suppression function that is materials dependent, successfully addressing the nonuniversality of the suppression function used in the past, while providing a general approach to studying thermal properties in the nondiffusive regime.

The impact of sodium contamination in tin sulfide thin-film solar cells

Abstract: Through empirical observations, sodium (Na) has been identified as a benign contaminant in some thin-film solar cells. Here, we intentionally contaminate thermally evaporated tin sulfide (SnS) thin-films with sodium and measure the SnS absorber properties and solar cell characteristics. The carrier concentration increases from 2 × 1016 cm−3 to 4.3 × 1017 cm−3 in Na-doped SnS thin-films, when using a 13 nm NaCl seed layer, which is detrimental for SnS photovoltaic applications but could make Na-doped SnS an attractive candidate in thermoelectrics. The observed trend in carrier concentration is in good agreement with density functional theory calculations, which predict an acceptor-type NaSn defect with low formation energy.

Resonant attenuation of surface acoustic waves by a disordered monolayer of microspheres

Abstract: Attenuation of surface acoustic waves (SAWs) by a disordered monolayer of polystyrene microspheres is investigated. Surface acoustic wave packets are generated by a pair of crossed laser pulses in a glass substrate coated with a thin aluminum film and detected via the diffraction of a probe laser beam. When a 170 μm-wide strip of micron-sized spheres is placed on the substrate between the excitation and detection spots, strong resonant attenuation of SAWs near 240 MHz is observed. The attenuation is caused by the interaction of SAWs with a contact resonance of the microspheres, as confirmed by acoustic dispersion measurements on the microsphere-coated area. Frequency-selective attenuation of SAWs by such a locally resonant metamaterial may lead to reconfigurable SAW devices and sensors, which can be easily manufactured via self-assembly techniques.

Variational approach to solving the spectral Boltzmann transport equation in transient thermal grating for thin films

Abstract: 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 distribution of materials via transient grating experiments

Variational approach to extracting the phonon mean free path distribution from the spectral Boltzmann transport equation

Abstract: The phonon Boltzmann transport equation (BTE) is a powerful tool for studying nondiffusive 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 nondiffusive transport. By utilizing the known Fourier heat conduction 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 experiment, which is a useful tool for studying nondiffusive thermal transport and probing the MFP distribution of materials. We obtain a closed form expression for a suppression function that is materials dependent, successfully addressing the nonuniversality of the suppression function used in the past, while providing a general approach to studying thermal properties in the nondiffusive regime.

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

Abstract: 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.

Supersonic Impact of Metallic Micro-particles

Abstract: 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.

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

Abstract: 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...

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

Abstract: 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.

Systems, Methods, and Apparatus for Radiation Detection

Abstract: A radiation detection technique employs field enhancing structures and electroluminescent materials to converts incident Terahertz (THz) radiation into visible light and/or infrared light. In this technique, the field-enhancing structures, such as split ring resonators or micro-slits, enhances the electric field of incoming THz light within a local area, where the electroluminescent material is applied. The enhanced electric field then induces the electroluminescent material to emit visible and/or infrared light via electroluminescent process. A detector such as avalanche photodiode can detect and measure the emitted light. This technique allows cost-effective detection of THz radiation at room temperatures.

What is the Brillouin zone of an anisotropic photonic crystal

Abstract: The authors discuss the concept of the Brillouin zone, central to many fields of condensed matter physics. They challenge the universality of defining the Brillouin zone as a Wigner-Seitz cell of the reciprocal lattice. Experimental measurements of terahertz phonon-polariton dispersion in a photonic crystal fabricated in a thin slab of an anisotropic material (lithium niobate) demonstrate that the lowest band gap does not form at the boundary of the conventionally defined Brillouin zone, in contrast to a similar photonic crystal fabricated in a nearly isotropic lithium tantalate. The analysis motivated by this unexpected experimental result shows that in an anisotropic photonic crystal the Wigner-Seitz cell of the reciprocal lattice is no longer bounded by Bragg planes and, consequently, does not conform to the original definition of the Brillouin zone. The authors construct an alternative Brillouin zone bounded by the Bragg planes and show its utility in analyzing the dispersion bands of anisotropic photonic crystals.