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© 2018 Author(s). The thermal conductivity of self-assembled nanocomposite oxide films consisting of cobalt ferrite (CFO) spinel pillars grown within a single-crystal bismuth ferrite (BFO) perovskite matrix is described as a function of the volume fraction of the spinel. Single phase BFO and CFO had cross-plane thermal conductivities of 1.32 W m-1 K-1 and 3.94 W m-1 K-1, respectively, and the thermal conductivity of the nanocomposites increased with the CFO volume fraction within this range. A small increase (∼5%) in thermal conductivity for the pure CFO phase in the AC-demagnetized state was observed, suggesting possible magnon contributions. Steady state gray-medium based variance-reduced Monte Carlo simulations show consistent trends with experimental data on the dependence of thermal conductivity with the CFO volume fraction.

Wavelike thermal transport in solids, referred to as second sound, is an exotic phenomenon previously limited to a handful of materials at low temperatures. The rare occurrence of this effect restricted its scientific and practical importance. We directly observed second sound in graphite at temperatures above 100 kelvins by using time-resolved optical measurements of thermal transport on the micrometer-length scale. Our experimental results are in qualitative agreement with ab initio calculations that predict wavelike phonon hydrodynamics. We believe that these results potentially indicate an important role of second sound in microscale transient heat transport in two-dimensional and layered materials in a wide temperature range., United States. Office of Naval Research (Grant N00014-16-1-2436), National Science Foundation (U.S.) (Grant EFMA-1542864), United States. Department of Energy. Office of Science. Energy Frontier Research Center (Award DE-SC0001299), United States. Department of Energy. Office of Basic Energy Sciences (Award DE-SC0001299)

Advances in developing ultrafast coherent sources operating at extreme ultraviolet (EUV) and x-ray wavelengths allow the extension of nonlinear optical techniques to shorter wavelengths. Here, we describe EUV transient grating spectroscopy, in which two crossed femtosecond EUV pulses produce spatially periodic nanoscale excitations in the sample and their dynamics is probed via diffraction of a third time-delayed EUV pulse. The use of radiation with wavelengths down to 13.3 nm allowed us to produce transient gratings with periods as short as 28 nm and observe thermal and coherent phonon dynamics in crystalline silicon and amorphous silicon nitride. This approach allows measurements of thermal transport on the ~10-nm scale, where the two samples show different heat transport regimes, and can be applied to study other phenomena showing nontrivial behaviors at the nanoscale, such as structural relaxations in complex liquids and ultrafast magnetic dynamics., United States. Department of Energy. Office of Basic Energy Sciences (Award DE-SC0001299), United States. Department of Energy. Office of Science. Energy Frontier Research Center (Award DE-SC001912)

We demonstrate the agreement between first-principles calculations and experimental measurements of size effects in thermal transport in SiGe alloys without fitting parameters. Transient thermal grating (TTG) is used to measure the effect of the grating period on the temperature decay. The virtual crystal approximation under the density-functional-theory 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, 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 fourfold of the bulk value) across grating periods spanning one order of magnitude. This paper provides a framework for the study of size effects in thermal transport in opaque materials.

We demonstrate the agreement between first-principles calculations and experimental measurements of size effects in thermal transport in SiGe alloys without fitting parameters. Transient thermal grating (TTG) is used to measure the effect of the grating period on the temperature decay. The virtual crystal approximation under the density-functional-theory 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, 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 fourfold of the bulk value) across grating periods spanning one order of magnitude. This paper provides a framework for the study of size effects in thermal transport in opaque materials., Solid-State Solar-Thermal Energy Conversion Center (Award DE-SC0001299), Solid-State Solar-Thermal Energy Conversion Center (Award DE-FG02-09ER46577)

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.

The role of the ferroelectric polarization state and crystal structure in determining the room-temperature thermal conductivity of epitaxial BiFeO₃ thin films is investigated. The ferroelectric domain configuration is varied by changing the oxygen partial pressure during growth, as well as by polarizing the samples by the application of an in situ electric field during the thermal conductivity measurement. However, little or no dependence of thermal conductivity on the ferroelectric domain structure is observed. In contrast, the thermal conductivity significantly depends on the morphotropic phase structure, being about 2/3 as large in tetragonal-like compared to rhombohedral-like BiFeO₃ film. The substantial structural dependence of thermal conductivity found here may provide a route to reversible manipulation of thermal properties., Solid-State Solar-Thermal Energy Conversion Center (Award DE-SC0001299), Solid-State Solar-Thermal Energy Conversion Center (Award DE-FG02-09ER46577)

It has been well known that the phonon drag effect—an extra electrical current induced by phonon heat flow via electron–phonon interaction—can lead to unusually high Seebeck coefficient at low temperatures. However, its use for improving thermoelectric performance has been controversial. Here, using first principles calculations we examine the phonon drag with detailed mode-specific contributions and reveal that even in heavily doped silicon at room temperature, phonon drag can still be significant, which challenges the previous belief that phonon drag vanishes in heavily doped samples. A phonon filter is designed to spectrally decouple the phonon drag from the heat conduction. Our simulation explores the coupled electron phonon transport and uncovers the possibility of optimizing the phonon drag for better thermoelectrics., United States. Department of Energy. Office of Science. Solid-State Solar Thermal Energy Conversion Center (Award DE- SC0001299/DE-FG02-09ER46577), United States. Air Force. Office of Scientific Research. Multidisciplinary University Research Initiative (AFOSR MURI FA9550-10-1-0533)

The impact of boundary scattering on non-diffusive thermal relaxation of a transient grating in thin membranes is rigorously analyzed using the multidimensional phononBoltzmann 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., United States. Dept. of Energy. Office of Science (Solid-State Solar-Thermal Energy Conversion Center Award DE-SC0001299/DE-FG02-09ER46577)

Although the thermoelectric figure of merit zT above 300 K has seen significant improvement recently, the progress at lower temperatures has been slow, mainly limited by the relatively low Seebeck coefficient and high thermal conductivity. Here we report, for the first time to our knowledge, success in first-principles computation of the phonon drag effect-a coupling phenomenon between electrons and nonequilibrium phonons-in heavily doped region and its optimization to enhance the Seebeck coefficient while reducing the phonon thermal conductivity by nanostructuring. Our simulation quantitatively identifies the major phonons contributing to the phonon drag, which are spectrally distinct from those carrying heat, and further reveals that although the phonon drag is reduced in heavily doped samples, a significant contribution to Seebeck coefficient still exists. An ideal phonon filter is proposed to enhance zT of silicon at room temperature by a factor of 20 to ∼0.25, and the enhancement can reach 70 times at 100 K. This work opens up a new venue toward better thermoelectrics by harnessing nonequilibrium phonons., United States. Air Force Office of Scientific Research (Multidisciplinary Research Program of the University Research Initiative, AFOSR MURI FA9550-10-1-0533), United States. Dept. of Energy (S3TEC Energy Frontier Research Center, Award DE-SC0001299/DE-FG02-09ER46577)

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., United States. Dept. of Energy. Office of Science (Solid-State Solar-Thermal Energy Conversion Center Award DE-SC0001299/DE-FG02-09ER46577)

The impact of boundary scattering on non-diffusive thermal relaxation of a transient grating in thin membranes is rigorously analyzed using the multidimensional phononBoltzmann 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., United States. Dept. of Energy. Office of Science (Solid-State Solar-Thermal Energy Conversion Center Award DE-SC0001299/DE-FG02-09ER46577)

Heat conduction in semiconductors and dielectrics depends upon their phonon mean free paths that describe the average travelling distance between two consecutive phonon scattering events. Nondiffusive phonon transport is being exploited to extract phonon mean free path distributions. Here, we describe an implementation of a nanoscale thermal conductivity spectroscopy technique that allows for the study of mean free path distributions in optically absorbing materials with relatively simple fabrication and a straightforward analysis scheme. We pattern 1D metallic grating of various line widths but fixed gap size on sample surfaces. The metal lines serve as both heaters and thermometers in time-domain thermoreflectance measurements and simultaneously act as wire-grid polarizers that protect the underlying substrate from direct optical excitation and heating. We demonstrate the viability of this technique by studying length-dependent thermal conductivities of silicon at various temperatures. The thermal conductivities measured with different metal line widths are analyzed using suppression functions calculated from the Boltzmann transport equation to extract the phonon mean free path distributions with no calibration required. This table-top ultrafast thermal transport spectroscopy technique enables the study of mean free path spectra in a wide range of technologically important materials., United States. Dept. of Energy. Office of Science (Solid-State Solar-Thermal Energy Conversion Center Award DE-SC0001299/DE-FG02-09ER46577)

The electron-phonon interaction is well known to create major resistance to electron transport in metals and semiconductors, whereas fewer studies are directed to its effect on phonon transport, especially in semiconductors. We calculate the phonon lifetimes due to scattering with electrons (or holes), combine them with the intrinsic lifetimes due to the anharmonic phonon-phonon interaction, all from first principles, and evaluate the effect of the electron-phonon interaction on the lattice thermal conductivity of silicon. Unexpectedly, we find a significant reduction of the lattice thermal conductivity at room temperature as the carrier concentration goes above 10[superscript 19] cm[superscript −3] (the reduction reaches up to 45% in p-type silicon at around 10[superscript 21] cm[superscript −3]), a range of great technological relevance to thermoelectric materials.