Importance of frequency-dependent grain boundary scattering in nanocrystalline silicon and silicon-germanium thermoelectrics

Nanocrystalline silicon and silicon-germanium alloys are promising thermoelectric materials that have achieved substantially improved figure of merits compared to their bulk counterparts. This enhancement is typically attributed to a reduction in lattice thermal conductivity by phonon scattering at grain boundaries. However, further improvements are difficult to achieve because grain boundary scattering is poorly understood, with recent experimental observations suggesting that the phonon transmissivity may depend on phonon frequency rather than being constant as in the commonly used gray model. Here, we examine the impact of frequency-dependent grain boundary scattering in nanocrystalline silicon and silicon-germanium alloys in a realistic 3D geometry using frequency-dependent variance-reduced Monte Carlo simulations. We find that the grain boundary may not be as effective as predicted by the gray model in scattering certain phonons, with a substantial amount of heat being carried by low frequency phonons with mean free paths longer than the grain size. Our result will help guide the design of more efficient thermoelectrics

Cross-plane heat conduction in thin solid films

Cross-plane heat transport in thin films with thickness comparable to the phonon mean free paths is of both fundamental and practical interest. However, physical insight is difficult to obtain for the cross-plane geometry due to the challenge of solving the Boltzmann equation in a finite domain. Here, we present a semi-analytical series expansion method to solve the transient, frequency-dependent Boltzmann transport equation that is valid from the diffusive to ballistic transport regimes and rigorously includes frequency-dependence of phonon properties. Further, our method is more than three orders of magnitude faster than prior numerical methods and provides a simple analytical expression for the thermal conductivity as a function of film thickness. Our result enables a more accurate understanding of heat conduction in thin films

Length Dependent Thermal Conductivity Measurements Yield Phonon Mean Free Path Spectra in Nanostructures

Thermal conductivity measurements over variable lengths on nanostructures such as nanowires provide important information about the mean free paths (MFPs) of the phonons responsible for heat conduction. However, nearly all of these measurements have been interpreted using an average MFP even though phonons in many crystals possess a broad MFP spectrum. Here, we present a reconstruction method to obtain MFP spectra of nanostructures from variable-length thermal conductivity measurements. Using this method, we investigate recently reported length-dependent thermal conductivity measurements on SiGe alloy nanowires and suspended graphene ribbons. We find that the recent measurements on graphene imply that 70 % of the heat in graphene is carried by phonons with MFPs longer than 1 micron

Analytical Green’s function of the multidimensional frequency-dependent phonon Boltzmann equation

Thermal phonon transport at length scales comparable to mean free paths is governed by the Boltzmann equation, which is challenging to solve due to its high dimensionality. Here, we present an analytical Green's function for the frequency-dependent, multidimensional Boltzmann equation under the relaxation-time approximation. The new analytical solution is valid from diffusive to ballistic transport regimes and rigorously includes frequency dependence of phonon properties. We demonstrate that our result enables simple closed-form solutions for a number of multidimensional problems for which the only prior solution methods have been computationally expensive numerical simulations

Quasiballistic Heat Conduction in Transient Grating Spectroscopy

Transient grating (TG) spectroscopy is an important experimental technique to measure mean free path (MFP) spectra using observations of quasiballistic heat conduction. To obtain MFP spectra, the measurements must be interpreted within the framework of the frequency-dependent Boltzmann transport equation (BTE), but previous solutions have restricted validity due to simplifying assumptions. Here, we analyze heat conduction in TG using a new analytical solution of the frequency-dependent BTE that accurately describes thermal transport from the diffusive to ballistic regimes. We demonstrate that our result enables a more accurate measurement of MFP spectra and thus will lead to an improved understanding of heat conduction in solids

Semi-analytical solution to the frequency-dependent Boltzmann transport equation for cross-plane heat conduction in thin films

Cross-plane heat transport in thin films with thicknesses comparable to the phonon mean free paths is of both fundamental and practical interest for applications such as light-emitting diodes and quantum well lasers. However, physical insight is difficult to obtain for the cross-plane geometry due to the challenge of solving the Boltzmann equation in a finite domain. Here, we present a semi-analytical series expansion method to solve the transient, frequency-dependent Boltzmann transport equation that is valid from the diffusive to ballistic transport regimes and rigorously includes the frequency-dependence of phonon properties. Further, our method is more than three orders of magnitude faster than prior numerical methods and provides a simple analytical expression for the thermal conductivity as a function of film thickness. Our result enables a straightforward physical understanding of cross-plane heat conduction in thin films

Fresnel transmission coefficients for thermal phonons at solid interfaces

Interfaces play an essential role in phonon-mediated heat conduction in solids, impacting applications ranging from thermoelectric waste heat recovery to heat dissipation in electronics. From a microscopic perspective, interfacial phonon transport is described by transmission and reflection coefficients, analogous to the well-known Fresnel coefficients for light. However, these coefficients have never been directly measured, and thermal transport processes at interfaces remain poorly understood despite considerable effort. Here, we report the first measurements of the Fresnel transmission coefficients for thermal phonons at a metal-semiconductor interface using ab-initio phonon transport modeling and a thermal characterization technique, time-domain thermoreflectance. Our measurements show that interfaces act as thermal phonon filters that transmit primarily low frequency phonons, leading to these phonons being the dominant energy carriers across the interface despite the larger density of states of high frequency phonons. Our work realizes the long-standing goal of directly measuring thermal phonon transmission coefficients and demonstrates a general route to study microscopic processes governing interfacial heat conduction

Quasiballistc Heat Conduction in Transient Grating Spectroscopy

Transient grating (TG) spectroscopy is an important experimental technique to measure mean free path (MFP) spectra using observations of quasiballistic heat conduction. To obtain MFP spectra, the measurements must be interpreted within the framework of the frequency-dependent Boltzmann transport equation (BTE), but previous solutions have restricted validity due to simplifying assumptions. Here, we analyze heat conduction in TG using a new analytical solution of the frequency-dependent BTE that accurately describes thermal transport from the diffusive to ballistic regimes. We demonstrate that our result enables a more accurate measurement of MFP spectra and thus will lead to an improved understanding of heat conduction in solids