Influence of two photon absorption induced free carriers on coherent polariton and phonon generation in ZnTe crystals

Combination of femtosecond Kerr, two photon absorption, and impulsive stimulated Raman scattering (ISRS) experiments have been carried out to investigate the effect of pulse energy and crystal temperature on the generation of coherent polaritons and phonons in 〈110〉 cut ZnTe single crystals of three different resistivities. We demonstrate that the effect of two photon induced free carriers on the creation of both the polaritons and phonons is largest at 4 K where the free carrier lifetime is enhanced. The temperature dependant ISRS on high and low purity ZnTe crystals allows us to unambiguously assign the phonon mode at 3.5 THz to the longitudinal acoustic mode at X-point in the Brillouin zone, LA(X).

Phonon anomalies and structural transition in spin ice Dy2Ti2O7: a simultaneous pressure-dependent and temperature-dependent Raman study

We revisit the assignment of Raman phonons of rare-earth titanates by performing Raman measurements on single crystals of O18 isotope-rich spin ice Dy2Ti2O718 and nonmagnetic Lu2Ti2O718 pyrochlores and compare the results with their O16 counterparts. We show that the low-wavenumber Raman modes below 250 cm-1 are not due to oxygen vibrations. A mode near 200 cm-1, commonly assigned as F2g phonon, which shows highly anomalous temperature dependence, is now assigned to a disorder-induced Raman active mode involving Ti4+ vibrations. Moreover, we address here the origin of the new Raman mode, observed below TC similar to 110 K in Dy2Ti2O7, through a simultaneous pressure-dependent and temperature-dependent Raman study. Our study confirms the new mode to be a phonon mode. We find that dTC/dP = + 5.9 K/GPa. Temperature dependence of other phonons has also been studied at various pressures up to similar to 8 GPa. We find that pressure suppresses the anomalous temperature dependence. The role of the inherent vacant sites present in the pyrochlore structure in the anomalous temperature dependence is also discussed. Copyright (c) 2012 John Wiley & Sons, Ltd.

Raman & Infrared Study of Bi Filled Co4Sb12

CoSb3 skutterudites are established thermoelectric materials in the 500-800K temperature range. Undoped and Bi filled CoSb3 samples were synthesized by induction melting-annealing process and phase confirmation done by X-Ray diffraction. The role of bismuth as a filler in CoSb3 was investigated by Raman and far infrared reflectance study. It was found that bismuth strengthens Sb vibrations, and can potentially scatter Sb related acoustic phonons effectively. As a result substantial reduction in thermal conductivity may be possible with proper control of Bi filling.

Acoustic and optical phonon dynamics from femtosecond time-resolved optical spectroscopy of the superconducting iron pnictide Ca(Fe0.944Co0.056)(2)As-2

We report the temperature evolution of coherently excited acoustic and optical phonon dynamics in the superconducting iron pnictide single crystal Ca(Fe0.944Co0.056)(2)As-2 across the spin density wave transition at T-SDW similar to 85 K and the superconducting transition at T-SC similar to 20 K. The strain pulse propagation model applied to the generation of the acoustic phonons yields the temperature dependence of the optical constants, and longitudinal and transverse sound velocities in the temperature range from 3.1 K to 300 K. The frequency and dephasing times of the phonons show anomalous temperature dependence below T-SC indicating a coupling of these low-energy excitations with the Cooper-pair quasiparticles. A maximum in the amplitude of the acoustic modes at T similar to 170 is seen, attributed to spin fluctuations and strong spin-lattice coupling before T-SDW. Copyright (c) EPLA, 2012

A physics-based flexural phonon-dependent thermal conductivity model for single layer graphene

In this paper, we address a physics-based closed-form analytical model of flexural phonon-dependent diffusive thermal conductivity (kappa) of suspended rectangular single layer graphene sheet. A quadratic dependence of the out-of-plane phonon frequency, generally called flexural phonons, on the phonon wave vector has been taken into account to analyze the behavior of kappa at lower temperatures. Such a dependence has further been used for the determination of second-order three-phonon Umklapp and isotopic scatterings. We find that these behaviors in our model are best explained through the upper limit of Debye cut-off frequency in the second-order three-phonon Umklapp scattering of the long phonon waves that actually remove the thermal conductivity singularity by contributing a constant scattering rate at low frequencies and note that the out-of-plane Gruneisen parameter for these modes need not be too high. Using this, we clearly demonstrate that. follows a T-1.5 and T-2 law at lower and higher temperatures in the absence of isotopes, respectively. However in their presence, the behavior of kappa sharply deviates from the T-2 law at higher temperatures. The present geometry-dependent model of kappa is found to possess an excellent match with various experimental data over a wide range of temperatures which can be put forward for efficient electro-thermal analyses of encased/supported graphene.

Sharp raman anomalies and broken adiabaticity at a pressure induced transition from band to topological insulator in Sb2Se3

The nontrivial electronic topology of a topological insulator is thus far known to display signatures in a robust metallic state at the surface. Here, we establish vibrational anomalies in Raman spectra of the bulk that signify changes in electronic topology: an E-g(2) phonon softens unusually and its linewidth exhibits an asymmetric peak at the pressure induced electronic topological transition (ETT) in Sb2Se3 crystal. Our first-principles calculations confirm the electronic transition from band to topological insulating state with reversal of parity of electronic bands passing through a metallic state at the ETT, but do not capture the phonon anomalies which involve breakdown of adiabatic approximation due to strongly coupled dynamics of phonons and electrons. Treating this within a four-band model of topological insulators, we elucidate how nonadiabatic renormalization of phonons constitutes readily measurable bulk signatures of an ETT, which will facilitate efforts to develop topological insulators by modifying a band insulator. DOI: 10.1103/PhysRevLett.110.107401

Thermoelectric properties of PbTe with encapsulated bismuth secondary phase

Lead Telluride (PbTe) with bismuth secondary phase embedded in the bulk has been prepared by matrix encapsulation technique. X-Ray Diffraction results indicated crystalline PbTe, while Rietveld analysis showed that Bi did not substitute at either Pb or Te site, which was further confirmed by Raman and X-Ray Photoelectron Spectroscopy. Scanning Electron Microscopy showed the expected presence of a secondary phase, while Energy Dispersive Spectroscopy results showed a slight deficiency of tellurium in the PbTe matrix, which might have occurred during synthesis due to higher vapor pressure of Te. Transmission Electron Microscopy results did not show any nanometer sized Bi phase. Seebeck coefficient (S) and electrical conductivity (sigma) were measured from room temperature to 725 K. A decrease in S and sigma with increasing Bi content showed an increased scattering of electrons from PbTe-Bi interfaces, along with a possible electron acceptor role of Bi secondary phase. An overall decrease in the power factor was thus observed. Thermal conductivity, measured from 400K to 725K, was smaller at starting temperature with increasing Bi concentration, and almost comparable to that of PbTe at higher temperatures, indicating a more important role of electrons as compared to phonons at PbTe-Bi interfaces. Still, a reasonable zT of 0.8 at 725K was achieved for undoped PbTe, but no improvement was found for bismuth added samples with micrometer inclusions. (C) 2013 American Institute of Physics. http://dx.doi.org/10.1063/1.4796148]

Physics-Based Solution for Electrical Resistance of Graphene Under Self-Heating Effect

In this brief, we present a physics-based solution for the temperature-dependent electrical resistance of a suspended metallic single-layer graphene (SLG) sheet under Joule self-heating. The effect of in-plane and flexural phonons on the electron scattering rates for a doped SLG layer has been considered, which particularly demonstrates the variation of the electrical resistance with increasing temperature at different current levels using the solution of the self-heating equation. The present solution agrees well with the available experimental data done with back-gate electrostatic method over a wide range of temperatures.

An unusual temperature induced isostructural phase transition in a scheelite, Li0.5Ce0.5MoO4

High resolution synchrotron X-ray diffraction, dielectric and Raman scattering study of a scheelite compound Li0.5Ce0.5MoO4 (LCM) revealed that it transforms to a self similar structure above 400 degrees C. The thermally induced isostructural phase transition (IPT), a phenomenon which has rarely been reported in the literature, is preceded by partial softening of the zone centre phonons followed by their hardening above the IPT transition temperature. The high temperature isostructural phase, which exhibits expanded lattice parameters and cell volume, nucleates and grows in the low temperature matrix over a very wide temperature range. Both the phases show nearly identical thermal expansion suggesting similarities in symmetry, unaltered coordination environments around the atoms across the transition.

Thermoelectric performance of a single-layer graphene sheet for energy harvesting

We investigate the thermoelectric (TE) figure-of-merit of a single-layer graphene (SLG) sheet by a physics-based analytical technique. We first develop analytical models of electrical and thermal resistances and the Seebeck coefficient of SLG by considering electron interactions with the in-plane and flexural phonons. Using those models, we show that both the figure-of-merit and the TE efficiency can be substantially increased with the addition of isotope doping as it significantly reduces the phonon-dominated thermal conductivity. In addition, we report that the TE open circuit output voltage and output power depends weakly on the SLG sheet dimensions and sheet concentration in the strongly diffusive regime. Proposed models agree well with the available experimental data and demonstrate the immense potential of graphene for waste-heat recovery application.

Modeling of temperature and field-dependent electron mobility in a single-layer graphene sheet

In this paper, we address a physics-based analytical model of electric-field-dependent electron mobility (mu) in a single-layer graphene sheet using the formulation of Landauer and Mc Kelvey's carrier flux approach under finite temperature and quasi-ballistic regime. The energy-dependent, near-elastic scattering rate of in-plane and out-of-plane (flexural) phonons with the electrons are considered to estimate mu over a wide range of temperature. We also demonstrate the variation of mu with carrier concentration as well as the longitudinal electric field. We find that at high electric field (>10(6) Vm(-1)), the mobility falls sharply, exhibiting the scattering between the electrons and flexural phonons. We also note here that under quasi-ballistic transport, the mobility tends to a constant value at low temperature, rather than in between T-2 and T-1 in strongly diffusive regime. Our analytical results agree well with the available experimental data, while the methodologies are put forward to estimate the other carrier-transmission-dependent transport properties.

Solution of Time Dependent Joule Heat Equation for a Graphene Sheet Under Thomson Effect

We address a physics-based solution of joule heating phenomenon in a single-layer graphene (SLG) sheet under the presence of Thomson effect. We demonstrate that the temperature in an isotopically pure (containing only C-12) SLG sheet attains its saturation level quicker than when doped with its isotopes (C-13). From the solution of the joule heating equation, we find that the thermal time constant of the SLG sheet is in the order of tenths of a nanosecond for SLG dimensions of a few micrometers. These results have been formulated using the electron interactions with the inplane and flexural phonons to demonstrate a field-dependent Landauer transmission coefficient. We further develop an analytical model of the SLG specific heat using the quadratic (out of plane) phonon band structure over the room temperature. Additionally, we show that a cooling effect in the SLG sheet can be substantially enhanced with the addition of C-13. The methodologies as discussed in this paper can be put forward to analyze the graphene heat spreader theory.

Thermoelectric Properties of Two-Phase PbTe with Indium Inclusions

The thermoelectric figure of merit (zT) can be increased by introduction of additional interfaces in the bulk to reduce the thermal conductivity. In this work, PbTe with a dispersed indium (In) phase was synthesized by a matrix encapsulation technique for different In concentrations. x-Ray diffraction analysis showed single-phase PbTe with In secondary phase. Rietveld analysis did not show In substitution at either the Pb or Te site, and this was further confirmed by room-temperature Raman data. Low-magnification (similar to 1500x) scanning electron microscopy images showed micrometer-sized In dispersed throughout the PbTe matrix, while at high magnification (150,000x) an agglomeration of PbTe particles in the hot-pressed samples could be seen. The electrical resistivity (rho) and Seebeck coefficient (S) were measured from 300 K to 723 K. Negative Seebeck values showed all the samples to be n-type. A systematic increase in resistivity and higher Seebeck coefficient values with increasing In content indicated the role of PbTe-In interfaces in the scattering of electrons. This was further confirmed by the thermal conductivity (kappa), measured from 423 K to 723 K, where a greater reduction in the electronic as compared with the lattice contribution was found for In-added samples. It was found that, despite the high lattice mismatch at the PbTe-In interface, phonons were not scattered as effectively as electrons. The highest zT obtained was 0.78 at 723 K for the sample with the lowest In content.

Molecular Dynamics Study of Phonon Screening in Graphene

Phonon interaction with electrons or phonons or with structural defects result in a phonon mode conversion. The mode conversion is governed by the frequency wave-vector dispersion relation. The control over phonon mode or the screening of phonon in graphene is studied using the propagation of amplitude modulated phonon wave-packet. Control over phonon properties like frequency and velocity opens up several wave guiding, energy transport and thermo-electric applications of graphene. One way to achieve this control is with the introduction of nano-structured scattering in the phonon path. Atomistic model of thermal energy transport is developed which is applicable to devices consisting of source, channel and drain parts. Longitudinal acoustic phonon mode is excited from one end of the device. Molecular dynamics based time integration is adopted for the propagation of excited phonon to the other end of the device. The amount of energy transfer is estimated from the relative change of kinetic energy. Increase in the phonon frequency decreases the kinetic energy transmission linearly in the frequency band of interest. Further reduction in transmission is observed with the tuning of channel height of the device by increasing the boundary scattering. Phonon mode selective transmission control have potential application in thermal insulation or thermo-electric application or photo-thermal amplification.

Study Of Lattice Dynamics In Yttrium Doped NdMnO3 Using Raman Spectroscopy

A systematic study of Raman spectra on Yttrium doped NdMnO3 polycrystalline samples was undertaken to understand the lattice dynamics in this compound. Raman active phonons were analyzed and the observed peak were assigned to elucidate various phonon modes in the range (200 - 800) cm(-1). It was observed that at 325 cm(-1) phonon frequency shifts upward as much as upto 4 % with increase in Yttrium content. Lattice distortions manifest themselves by frequency shifts in both bending and tilt modes of MnO6 octahedra, resulting in increase of Raman band line-widths.