Monte Carlo based statistical approach to solve Boltzmann Transport Equation (BTE) has become a norm to investigate heat transport in semiconductors at sub-micron regime, owing mainly to its ability to characterize realistically sized device geometries qualitatively. One of the primary issues with this technique is that the approach predominantly uses empirically fitted phonon dispersion relations as input to determine the properties of phonons so as to predict the thermal conductivity of specified material geometry. The empirically fitted dispersion relations assume harmonic approximation thereby failing to account for thermal expansion, interaction of lattice waves, effect of strain on spring stiffness, and accurate phonon-phonon interaction. To circumvent this problem, in this work, a coupled molecular mechanics-Monte Carlo (MM-MC) platform has been developed and used to solve the phonon Boltzmann Transport Equation (BTE) for the calculation of thermal conductivity of several novel and emerging nanostructures. The use of the quasi-anharmonic MM approach (as implemented in the open source NEMO 3-D software toolkit) not only allows one to capture the true atomicity of the underlying lattice but also enables the simulation of realistically-sized structures containing millions of atoms. As compared to the approach using an empirically fitted phonon dispersion relation, here, a 17% increase in the thermal conductivity for a silicon nanowire due to the incorporation of atomistic corrections in the LA (longitudinal acoustic) branch alone has been reported. The atomistically derived thermal conductivity as calculated from the MM-MC framework is then used in the modular design and analysis of (i) a silicon nanowire based thermoelectric cooler (TEC) unit, and (ii) a GaN/InN based nanostructured light emitting device (LED). It is demonstrated that the use of empirically fitted phonon bandstructure parameters overestimates the temperature difference between the hot and the cold sides and the overall cooling efficiency of the system, thereby, demanding the use of the BTE derived thermal conductivity in the calculation of thermal conductivity. In case of the light-emitting device, the microscopically derived material parameters, as compared to their bulk and fitted counterparts, yielded [approximately] 3% correction (increase) in optical efficiency. A non-deterministic approach adopted in this work, therefore, provides satisfactory results in what concerns phonons transport in both ballistic and diffusive regimes to understand and/predict the heat transport phenomena in nanostructures.

"Managing thermal energy generation and transfer within the nanoscale devices (transistors) of modern microelectronics is important as it limits speed, carrier mobility, and affects reliability. Application of Fourier’s Law of Heat Conduction to the small length and times scales associated with transistor geometries and switching frequencies doesn’t give accurate results due to the breakdown of the continuum assumption and the assumption of local thermodynamic equilibrium. Heat conduction at these length and time scales occurs via phonon transport, including both classical and quantum effects. Traditional methods for phonon transport modeling are lacking in the combination of computational efficiency, physical accuracy, and flexibility. The Statistical Phonon Transport Model (SPTM) is an engineering design tool for predicting non-equilibrium phonon transport. The goal of this work has been to enhance the models and computational algorithms of the SPTM to elevate it to have a high combination of accuracy and flexibility. Four physical models of the SPTM were enhanced. The lattice dynamics calculation of phonon dispersion relations was extended to use first and second nearest neighbor interactions, based on published interatomic force constants computed with first principles Density Functional Theory (DFT). The computation of three phonon scattering partners (that explicitly conserve energy and momentum) with the inclusion of the three optical phonon branches was applied using scattering rates computed from Fermi’s Golden Rule. The prediction of phonon drift was extended to three dimensions within the framework of the previously established methods of the SPTM. Joule heating as a result of electron-phonon scattering in nanoscale electronic devices was represented using a modal specific phonon source that can be varied in space and time. Results indicate the use of first and second nearest neighbor lattice dynamics better predicted dispersion when compared to experimental results and resulted in a higher fidelity representation of phonon group velocities and three phonon scattering partners in an anisotropic manner. Three phonon scattering improvements resulted in enhanced fidelity in the prediction of phonon modal decay rates across the wavevector space and thus better representation of non-equilibrium behavior. Comparisons to the range of phonon transport modeling approaches from literature verify that the SPTM has higher phonon fidelity than Boltzmann Transport Equation and Monte Carlo and higher length scale and time scale fidelity than Direct Atomic Simulation. Additional application of the SPTM to both a 1-d silicon nanowire transistor and a 3-d FinFET array transistor in a transient manner illustrate the design capabilities. Thus, the SPTM has been elevated to fill the gap between lower phonon fidelity Monte Carol (MC) models and high fidelity, inflexible direct quantum simulations (or Direct Atomic Simulations (DAS)) within the field of phonon transport modeling for nanoscale electronic devices. The SPTM has produced high fidelity device level non-equilibrium phonon information in a 3-d, transient manner where Joule heating occurs. This information is required due to the fact that effective lattice temperatures are not adequate to describe the local thermal conditions. Knowledge of local phonon distributions, which can’t be determined from application of Fourier’s law, is important because of effects on electron mobility, device speed, leakage, and reliability."--Abstract.

With novel electronic and optical properties, two-dimensional (2D) materials and their heterogeneous integration have enabled promising electronic and photonic applications. However, significant thermal challenges arise due to numerous van der Waals (vdW) interfaces limiting dissipation of heat generated in the device, induces significant temperature rise, and creates large thermal mismatch, resulting in the degradation of device performance and even failure of the device. The highly localized heat generation during device operation thus becomes a major bottleneck of 2D nanodevice performance. Nevertheless, classical descriptions of heat transfer, i.e., Fourier's Law, become invalid from the microscopic view. Furthermore, it remains challenging to measure heat transport precisely. Advances in the characterization and understanding of heat transfer at the nanoscale are thus needed for practical thermal management of nanoelectronics. Recent theoretical and experimental progress promises more effective nanoelectronics thermal management. On the one hand, atomistic simulation provides great opportunities to investigate fundamental thermal transport processes under ideal conditions by tracking the motion of all atoms. Raman spectroscopy, on the other hand, has been widely applied to detect lattice or molecule vibration on small scales owing to its superior spatial resolution. In this thesis, we leverage the power of atomistic simulation and Raman spectroscopy to understand and characterize thermophysical and thermal transport properties for engineering thermal transport in 2D vdW nanoelectronics. The thesis presents a method of characterizing thermal expansion coefficients for 2D transitional metal dichalcogenide monolayers experimentally and theoretically, and an atomistic simulation framework to predict thermal transport properties, which is used to study vdW binding effects on anisotropic heat transfer and phonon transport through an MoS2-amorphous silica heterostructure toward optimal 2D device heat dissipation. With combined efforts of experiments and simulation, this thesis opens up new avenues to understand, characterize, and engineer thermal transport in 2D vdW nanoelectronics.

The inability to remove heat efficiently is currently one of the stumbling blocks toward further miniaturization and advancement of electronic, optoelectronic, and micro-electro-mechanical devices. In order to formulate better heat removal strategies and designs, it is first necessary to understand the fundamental mechanisms of heat transport in semiconductor thin films. Modeling techniques, based on first principles, can play the crucial role of filling gaps in our understanding by revealing information that experiments are incapable of. Heat conduction in crystalline semiconductor films occurs by lattice vibrations that result in the propagation of quanta of energy called phonons. If the mean free path of the traveling phonons is larger than the film thickness, thermodynamic equilibrium ceases to exist, and thus, the Fourier law of heat conduction is invalid. In this scenario, bulk thermal conductivity values, which are experimentally determined by inversion of the Fourier law itself, cannot be used for analysis. The Boltzmann Transport Equation (BTE) is a powerful tool to treat non-equilibrium heat transport in thin films. The BTE describes the evolution of the number density (or energy) distribution for phonons as a result of transport (or drift) and inter-phonon collisions. Drift causes the phonon energy distribution to deviate from equilibrium, while collisions tend to restore equilibrium. Prior to solution of the BTE, it is necessary to compute the lifetimes (or scattering rates) for phonons of all wave-vector and polarization. The lifetime of a phonon is the net result of its collisions with other phonons, which in turn is governed by the conservation of energy and momentum during the underlying collision processes. This research project contributed to the state-of-the-art in two ways: (1) by developing and demonstrating a calibration-free simple methodology to compute intrinsic phonon scattering (Normal and Umklapp processes) time scales with the inclusion of optical phonons, and (2) by developing a suite of numerical algorithms for solution of the BTE for phonons. The suite of numerical algorithms includes Monte Carlo techniques and deterministic techniques based on the Discrete Ordinates Method and the Ballistic-Diffusive approximation of the BTE. These methods were applied to calculation of thermal conductivity of silicon thin films, and to simulate heat conduction in multi-dimensional structures. In addition, thermal transport in silicon nanowires was investigated using two different first principles methods. One was to apply the Green-Kubo formulation to an equilibrium system. The other was to use Non-Equilibrium Molecular Dynamics (NEMD). Results of MD simulations showed that the nanowire cross-sectional shape and size significantly affects the thermal conductivity, as has been found experimentally. In summary, the project clarified the role of various phonon modes - in particular, optical phonon - in non-equilibrium transport in silicon. It laid the foundation for the solution of the BTE in complex three-dimensional structures using deterministic techniques, paving the way for the development of robust numerical tools that could be coupled to existing device simulation tools to enable coupled electro-thermal modeling of practical electronic/optoelectronic devices. Finally, it shed light on why the thermal conductivity of silicon nanowires is so sensitive to its cross-sectional shape.

Heat conduction in semiconductors and dielectrics involves cumulative contributions from phonons with different frequencies and mean free paths (MFPs). Knowing the phonon MFP distribution allows us to gain insight into the fundamental microscopic transport physics and has important implications for many energy applications. The key metric that quantifies the relative contributions of different phonon MFPs to thermal conductivity is termed thermal conductivity accumulation function. In this thesis, we advance a thermal conductivity spectroscopy technique based upon experimental observation of non-diffusive thermal transport using wire grid linear polarizer in conjunction with time-domain thermoreflectance (TDTR) pump-and-probe measurement setup. Consistent algorithm based on solution from the phonon Boltzmann transport equation (BTE) is also developed to approximately extract the thermal conductivity accumulation functions in materials studied. The heat flux suppression function appropriate for the experimental sample geometry relates the measured apparent thermal conductivities to the material's phonon MFP distributions. We develop a multi-dimensional thermal transport model based on the gray phonon BTE to find the suppression function relevant to our spectroscopy experiment. The simulation results reveal that the suppression function depends upon both the heater size and the heater array period. We also find that the suppression function depends significantly on the location of the temperature measurement. Residual suppression effect is observed for finite filling fractions (ratio of heater size to heater array period) due to the transport coupling in the underlying substrate induced by the neighboring heaters. Prior phonon MFP spectroscopy techniques suffer from one or several of the following limitations: (1) diffraction limited to micrometer lengthscales by focusing optics, (2) applying only to transparent materials, or (3) involving complex micro-fabrications. We explore an alternate approach here using wire grid linear polarizer in combination with TDTR measurement. The wire grid polarizer is designed with sub-wavelength gaps between neighboring heaters to prevent direct photo-excitation in the substrate while simultaneously functioning as heaters and thermometers during the measurement. The spectroscopy technique is demonstrated in crystalline silicon by studying length-dependent thermal transport across a range of lengthscales and temperatures. We utilize the calculated heat flux suppression functions and the measured size-dependent effective thermal conductivities to reconstruct the phonon MFPs in silicon and achieve reasonably good agreement with calculation results from first principle density function theory. Knowledge of phonon MFP distributions in thermoelectric materials will help design nanostructures to further reduce lattice thermal conductivity to achieve better thermoelectric performance in the next-generation thermoelectric devices. We apply the developed wire grid polarizer spectroscopy technique to study phonon MFP distributions in two thermoelectric materials: Nb0.95 Ti0.05FeSb and boron-doped nanocrystalline Si80Ge20B. We find that the dominant phonon MFPs that contribute to thermal conductivity in those two materials are in the a few tens to a few hundreds of nanometers. The measurement results also shed light on why nanostructuring is an effective approach to scattering phonons and improve the thermoelectric behavior.

Advanced materials with extreme thermal conductivity are critically important for various technological applications including energy conversion, storage, and thermal management. Low thermal conductivity is needed for thermal insulation and thermoelectric energy harvesting, while high thermal conductivity is desirable for efficient heat spreading in electronics. However, practical application deployments are usually limited by the materials availability in nature. Moreover, understanding the fundamental origins for extreme thermal conductivity still remains challenging. My PhD research focuses on finding new thermal materials and unveiling fundamental phonon transport mechanisms in extreme thermal conductivity matters to push the frontier of thermal science. My dissertation is composed of three topics. The first topic is focused on developing and investigating a new group of ultrahigh conductivity materials. High-quality boron phosphide (BP) and boron arsenide (BAs) crystal are synthesized and measured with thermal conductivities of 460 and 1300 W/mK, respectively. In particular, our result shows that BAs is the best thermal conductor among common bulk metals and semiconductors. To better understand the fundamental origin of such an ultrahigh thermal conductivity, advanced phonon spectroscopy and temperature dependent characterizations are performed. Our measurements, in conjunction with atomistic theory, reveal that, unlike the commonly accepted rule for most materials near room temperature, high-order anharmonicity through the four-phonon process is significant in BA because of its unique band structure. Our result underscores the promise of using BP and BAs for thermal management and develops microscopic understanding of the phonon transport mechanisms. The second topic of my thesis is to investigate phonon transport in ultralow thermal conductivity material with a focus on tin selenide (SnSe). SnSe is a recently discovered material for high performance thermoelectricity. However, the thermal properties of intrinsic SnSe remain elusive in literature. To understand the dominant phonon transport mechanisms for the extremely low thermal conductivity of SnSe, temperature-dependent sound velocity, lattice expansion, and Gr neisen parameter was measured. The measurement result shows that high-order anharmonicity introduces strong phonon renormalization and the ultralow thermal conductivity. The third topic of the thesis is to investigate in-situ dynamic tuning of thermal conductivity in layered materials. A novel device platform based on lithium ion battery is developed to characterize the interactions between ions and phonons of layered materials. We observe a highly reversible modulation and anisotropy of thermal conductivity from phonon scattering introduced by ionic intercalation in the interspacing layers. This study provides a unique approach to explore the fundamental energy transport involving lattices and ions and open up new opportunities in thermal engineering.

With the advancement of nanofabrication techniques, the sizes of semiconductor electronic and optoelectronic devices keep decreasing while the operating speeds keep increasing. High-speed operation leads to more heat generation and puts more thermal stress on the devices. Since the heat conduction in semiconductors is dominated by the lattice (i.e., phonons), understanding phonon transport in nanostructures is essential to addressing and alleviating the thermal-stress problem in these modern devices. In addition to the increased thermal stress, the advanced techniques that have allowed for the shrinking of the devices routinely rely on heterostructuring, doping, alloying, and the growth of intentionally strained layers to achieve the desired electronic and optical properties. These introduce impediments to phonon transport such as boundaries, interfaces, point defects (alloy atoms or dopants), and strain. Phonon transport is strongly affected by this nanoscale disorder. This dissertation examines how different types of disorder interact with phonons and degrade phonon transport. First, we study thermal transport in graphene nanoribbons (GNRs). GNRs are quasi-one-dimensional (quasi-1D) systems where the edges (boundaries) play an important role in reducing thermal conductivity. Additionally, the thermal transport in GNRs is anisotropic and depend on the GNR's chirality (GNR orientation and edge termination). We use phonon Monte Carlo (PMC) with full phonon dispersions to describe two highly-symmetric types of GNRs: the armchair GNR (AGNR) and the zigzag GNR (ZGNR). PMC tracks phonon in real space and we can explicitly include non-trivial edge structures. Moreover, the relatively low computational burden of PMC allows us to simulate samples up to 100 $\mu$m in length and predict an upper limit for thermal conductivity in graphene. We then investigate the thermal conductivity in III-V superlattices (SLs). SLs consist of alternating thin layers of different materials and III-V SLs are widely used in nanoscale thermoelectric and optoelectronic devices. The key feature in SLs is that it contains many interfaces, which dictates thermal transport. As III-V SLs are often fabricated using well-controlled techniques and have high-quality interfaces, we develop a model with only one free parameter---the effective rms roughness of the interfaces---to describe its twofold influence: reducing the in-plane layer thermal conductivity and introducing thermal boundary resistance (TBR) in the cross-plane direction. Both the calculated in-plane and cross-plane thermal conductivity of SLs agree with a number of different experiments. Finally, we study thermal conductivity of ternary III-V alloys. In modern optoelectronic devices, ternary III-V alloys are used more often than binary compounds because one can use composition engineering to achieve different effective masses, electron/hole barrier heights, and strain levels. Ternary alloys are usually treated under the virtual crystal approximation (VCA) where cation atoms are assumed to be randomly distributed and possess an averaged mass. This assumption is challenged by a discrepancy between different experiments, as well as the discrepancy between experiments and calculations. We use molecular dynamics (MD) to study the ternary alloy system as both atom masses and atom locations are explicitly tracked in MD. We discover that the thermal conductivity is determined by a competition between mass-difference scattering and the short-range ordering of the cations.

There have been few books devoted to the study of phonons, a major area of condensed matter physics. The Physics of Phonons is a comprehensive theoretical discussion of the most important topics, including some topics not previously presented in book form. Although primarily theoretical in approach, the author refers to experimental results wherever possible, ensuring an ideal book for both experimental and theoretical researchers. The author begins with an introduction to crystal symmetry and continues with a discussion of lattice dynamics in the harmonic approximation, including the traditional phenomenological approach and the more recent ab initio approach, detailed for the first time in this book. A discussion of anharmonicity is followed by the theory of lattice thermal conductivity, presented at a level far beyond that available in any other book. The chapter on phonon interactions is likewise more comprehensive than any similar discussion elsewhere. The sections on phonons in superlattices, impure and mixed crystals, quasicrystals, phonon spectroscopy, Kapitza resistance, and quantum evaporation also contain material appearing in book form for the first time. The book is complemented by numerous diagrams that aid understanding and is comprehensively referenced for further study. With its unprecedented wide coverage of the field, The Physics of Phonons will be indispensable to all postgraduates, advanced undergraduates, and researchers working on condensed matter physics.

Through analyses, experimental results, and worked-out numerical examples, Microscale and Nanoscale Heat Transfer: Fundamentals and Engineering Applications explores the methods and observations of thermophysical phenomena in size-affected domains. Compiling the most relevant findings from the literature, along with results from their own re