Studies of non-diffusive heat conduction through spatially periodic and time-harmonic thermal excitations

Studies of non-diffusive heat conduction provide insight into the fundamentals of heat transport in condensed matter. The mean free paths (MFPs) of phonons that are most important for conducting heat are well represented by a material's thermal conductivity accumulation function. Determining thermal conductivity accumulation functions experimentally by studying conduction in non-diffusive regimes is a recent area of study called phonon MFP spectroscopy. In this thesis, we investigate nondiffusive transport both experimentally and theoretically to advance methods for determining thermal conductivity accumulation functions in materials. We explore both spatially periodic and time-harmonic thermal excitations as a means for probing the non-diffusive transport regime, where the Fourier heat diffusion law breaks down. Boltzmann transport equation calculations of one-dimensional (1D) spatially sinusoidal thermal excitations are performed for gray-medium and fully spectral cases. We compare our calculations to simplified transport models and demonstrate that a model based on integrating gray-medium solutions can reasonably model materials with a narrow range of dominant heat-carrying phonon MFPs. We also consider the inverse problem of determining thermal conductivity accumulation functions from experimental measurements of thermal-length-scale-dependent effective thermal conductivity. Based on experimental measurements of Si membranes of varying thickness, we reproduce the thermal conductivity accumulation function for bulk Si. To investigate materials with short phonon MFPs, we developed an experimental approach based on microfabricating 1D wire grid polarizers on the surface of a material under study. This work finds that the dominant thermal length scales in polycrystalline Bi 2Te3 are smaller than 100 nm. We also determine that even small amounts of direct sample optical excitation, which occurs when light transmits through the grating and directly excites electron-hole pairs in the substrate, can appreciably influence the measured results, suggesting that an alternate approach that prevents all direct optical excitation is preferable. To study thermal length scales smaller than 100 nm without the need for microfabrication, we develop a method for extracting high frequency response information 3 from transient optical measurements. For a periodic heat flux input, the thermal penetration depth in a semi-infinite sample depends on the excitation frequency, with higher frequencies leading to shallower thermal penetration depths. Prior work using frequencies as high as 200 MHz observed apparent non-diffusive behavior. Our method allows for frequencies of at least 1 GHz, but we do not observe any deviation from the heat diffusion equation, suggesting that prior observations attributed to non-diffusive effects were likely the result of transport phenomena in the metal transducer. Thesis Supervisor: Gang Chen Title: Carl Richard Soderberg Professor of Power Engineering

[1]  Humphrey J. Maris,et al.  Improved apparatus for picosecond pump‐and‐probe optical measurements , 1996 .

[2]  Gang Chen,et al.  Thermal Conductivity of Nanostructured Thermoelectric Materials , 2006 .

[3]  D. Balageas,et al.  Micron‐scale thermal characterizations of interfaces parallel or perpendicular to the surface , 1995 .

[4]  O. Matsuda,et al.  A method for the frequency control in time-resolved two-dimensional gigahertz surface acoustic wave imaging , 2014 .

[5]  A. Majumdar,et al.  Thermometry and Thermal Transport in Micro/Nanoscale Solid-State Devices and Structures , 2002 .

[6]  D. Cahill,et al.  Thermal Conductance of metal-metal interfaces , 2005 .

[7]  A. Majumdar Microscale Heat Conduction in Dielectric Thin Films , 1993 .

[8]  J. Chyi,et al.  Broadband terahertz ultrasonic transducer based on a laser-driven piezoelectric semiconductor superlattice. , 2012, Ultrasonics.

[9]  J. Rogers,et al.  Optical Generation and Characterization of Acoustic Waves in Thin Films: Fundamentals and Applications , 2000 .

[10]  Fujimoto,et al.  Femtosecond electronic heat-transport dynamics in thin gold films. , 1987, Physical review letters.

[11]  M. Dresselhaus,et al.  High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys , 2008, Science.

[12]  H. Maris,et al.  Electron diffusion in metals studied by picosecond ultrasonics. , 1994, Physical review. B, Condensed matter.

[13]  Qing Li,et al.  Quasi-ballistic thermal transport from nanoscale interfaces observed using ultrafast coherent soft x-ray beams , 2011, OPTO.

[14]  K. Nelson,et al.  Reconstructing phonon mean-free-path contributions to thermal conductivity using nanoscale membranes , 2014, 1408.6747.

[15]  Junichiro Shiomi,et al.  Phonon conduction in PbSe, PbTe, and PbTe 1 − x Se x from first-principles calculations , 2012 .

[16]  David Broido,et al.  Intrinsic phonon relaxation times from first-principles studies of the thermal conductivities of Si and Ge , 2010 .

[17]  K. Nelson,et al.  Lifetime of sub-THz coherent acoustic phonons in a GaAs-AlAs superlattice , 2012, 1210.1254.

[18]  Gang Chen,et al.  Nonlocal and Nonequilibrium Heat Conduction in the Vicinity of Nanoparticles , 1996 .

[19]  B. C. Daly,et al.  Picosecond ultrasonic measurements of attenuation of longitudinal acoustic phonons in silicon , 2009 .

[20]  R. Peierls,et al.  Zur kinetischen Theorie der Wärmeleitung in Kristallen , 1929 .

[21]  Gang Chen,et al.  Spectral Phonon Transport Properties of Silicon Based on Molecular Dynamics Simulations and Lattice Dynamics , 2008 .

[22]  Mika Prunnila,et al.  Reduction of the thermal conductivity in free-standing silicon nano-membranes investigated by non-invasive Raman thermometry , 2014, APL Materials.

[23]  Gang Chen,et al.  Disparate quasiballistic heat conduction regimes from periodic heat sources on a substrate , 2014 .

[24]  D. Cahill,et al.  Indirect heating of Pt by short-pulse laser irradiation of Au in a nanoscale Pt/Au bilayer , 2014 .

[25]  D. Cahill Analysis of heat flow in layered structures for time-domain thermoreflectance , 2004 .

[26]  Xuan Zheng,et al.  Two-tint pump-probe measurements using a femtosecond laser oscillator and sharp-edged optical filters. , 2008, The Review of scientific instruments.

[27]  Eberhard Burkel,et al.  Inelastic Scattering of X-Rays with Very High Energy Resolution , 1991 .

[28]  A. Rosencwaig,et al.  Detection of thermal waves through optical reflectance , 1985 .

[29]  Gang Chen,et al.  Heat Transfer in Thermoelectric Materials and Devices , 2013 .

[30]  David G. Cahill,et al.  Frequency dependence of the thermal conductivity of semiconductor alloys , 2007 .

[31]  Erik H. Anderson,et al.  A New Regime of Nanoscale Thermal Transport: Collective Diffusion Counteracts Dissipation Inefficiency , 2014 .

[32]  D. Pohl,et al.  Laser-Induced Dynamic Gratings , 1986 .

[33]  Gang Chen Nanoscale energy transport and conversion : a parallel treatment of electrons, molecules, phonons, and photons , 2005 .

[34]  K. Nelson,et al.  Non-diffusive relaxation of a transient thermal grating analyzed with the Boltzmann transport equation , 2013 .

[35]  E. H. Sondheimer,et al.  The mean free path of electrons in metals , 1952 .

[36]  A. Minnich,et al.  Phonon black-body radiation limit for heat dissipation in electronics. , 2015, Nature materials.

[37]  W. Press Numerical recipes in Fortran 77 : the art of scientific computing : volume 1 of fortran numerical recipes , 1996 .

[38]  J. Callaway Model for Lattice Thermal Conductivity at Low Temperatures , 1959 .

[39]  A. Minnich Exploring electron and phonon transport at the nanoscale for thermoelectric energy conversion , 2011 .

[40]  Oliver B. Wright,et al.  Ultrafast acoustic phonon generation in gold , 1996 .

[41]  K. Nelson,et al.  Examining thermal transport through a frequency-domain representation of time-domain thermoreflectance data. , 2014, The Review of scientific instruments.

[42]  A. Minnich Towards a microscopic understanding of phonon heat conduction , 2014, 1405.0532.

[43]  Radial Quasiballistic Transport in Time-Domain Thermoreflectance Studied Using Monte Carlo Simulations , 2014, 1402.1114.

[44]  D. Cahill,et al.  Anisotropic failure of Fourier theory in time-domain thermoreflectance experiments , 2014, Nature Communications.

[45]  J. C. Jaeger,et al.  Conduction of Heat in Solids , 1952 .

[46]  Gang Chen,et al.  Studies on surface preparation and smoothness of nanostructured Bi2Te3-based alloys by electrochemical and mechanical methods , 2011 .

[47]  P. Raad,et al.  Minimizing the uncertainties associated with the measurement of thermal properties by the Transient thermo-reflectance method , 2005, IEEE Transactions on Components and Packaging Technologies.

[48]  Gang Chen,et al.  Pulse accumulation, radial heat conduction, and anisotropic thermal conductivity in pump-probe transient thermoreflectance. , 2008, The Review of scientific instruments.

[49]  J. Malen,et al.  Instrumentation of broadband frequency domain thermoreflectance for measuring thermal conductivity accumulation functions. , 2013, The Review of scientific instruments.

[50]  Gang Chen,et al.  Direct measurement of room-temperature nondiffusive thermal transport over micron distances in a silicon membrane. , 2012, Physical review letters.

[51]  Changhu Xing,et al.  Parametric Study of the Frequency-Domain Thermoreflectance Technique , 2012 .

[52]  K. Nelson,et al.  Optical heterodyne detection of laser-induced gratings. , 1998, Optics letters.

[53]  M. Wagner,et al.  Single-beam thermowave analysis of semiconductors , 1991 .

[54]  Klaus Fuchs,et al.  The conductivity of thin metallic films according to the electron theory of metals , 1938, Mathematical Proceedings of the Cambridge Philosophical Society.

[55]  K. Nelson,et al.  Elastic modulus and in-plane thermal diffusivity measurements in thin polyimide films using symmetry-selective real-time impulsive stimulated thermal scattering , 1994 .

[56]  Stephen P. Boyd,et al.  Graph Implementations for Nonsmooth Convex Programs , 2008, Recent Advances in Learning and Control.

[57]  Fischer,et al.  Phonon radiative heat transfer and surface scattering. , 1988, Physical review. B, Condensed matter.

[58]  Phase-controlled, heterodyne laser-induced transient grating measurements of thermal transport properties in opaque material , 2011, 1109.6685.

[59]  A. Minnich,et al.  Determining phonon mean free paths from observations of quasiballistic thermal transport. , 2012, Physical review letters.

[60]  Kenneth E. Goodson,et al.  Phonon scattering in silicon films with thickness of order 100 nm , 1999 .

[61]  Qing Hao,et al.  Frequency-dependent Monte Carlo simulations of phonon transport in two-dimensional porous silicon with aligned pores , 2009 .

[62]  G. J. Snyder,et al.  Heavily Doped p‐Type PbSe with High Thermoelectric Performance: An Alternative for PbTe , 2011, Advanced materials.

[63]  G. Eesley,et al.  Transient thermoreflectance from thin metal films , 1986, Annual Meeting Optical Society of America.

[64]  D. Cahill,et al.  Two-channel model for nonequilibrium thermal transport in pump-probe experiments , 2013 .

[65]  Gang Chen,et al.  Heat transport in silicon from first-principles calculations , 2011, 1107.5288.

[66]  A. Schmidt Optical characterization of thermal transport from the nanoscale to the macroscale , 2008 .

[67]  Cristina H Amon,et al.  Broadband phonon mean free path contributions to thermal conductivity measured using frequency domain thermoreflectance , 2013, Nature Communications.

[68]  M. G. Holland Phonon Scattering in Semiconductors From Thermal Conductivity Studies , 1964 .

[69]  M. Dresselhaus,et al.  Thermal conductivity spectroscopy technique to measure phonon mean free paths. , 2011, Physical review letters.

[70]  C. Dames,et al.  Mean free path spectra as a tool to understand thermal conductivity in bulk and nanostructures , 2013 .

[71]  Onset of nondiffusive phonon transport in transient thermal grating decay , 2011, 1108.3770.

[72]  David J. Singh,et al.  Giant anharmonic phonon scattering in PbTe. , 2011, Nature materials.

[73]  A. Minnich,et al.  Length Dependent Thermal Conductivity Measurements Yield Phonon Mean Free Path Spectra in Nanostructures , 2014, Scientific Reports.

[74]  Bekir Sami Yilbas,et al.  Quasiballistic heat transfer studied using the frequency-dependent Boltzmann transport equation , 2011 .

[75]  D. Maillet,et al.  Thermal Quadrupoles: Solving the Heat Equation through Integral Transforms , 2000 .

[76]  A. Bell On the production and reproduction of sound by light , 1880, American Journal of Science.