Thermal transport properties are critical for applications ranging from thermal management to energy conversion. Passive thermal management has been an area of study for over a century and has only grown as technology has advanced because it requires no additional energy to remove heat. Changing the nanostructure of the materials involved in passive heat transfer methods, either by geometric changes or stoichiometric changes, can greatly improve the effectiveness of this heat transfer method. In order to explore this further, this work employs LAMMPS molecular dynamics (MD) simulation software to calculate the lattice thermal conductivity (λp) of a nanoparticle (NP) and material used indifferent passive heat transfer methods after either modifying their geometry or stoichiometry. The NPs this work will simulate are single-wall carbon nanotubes (SWCNTs), which have been well known for high λp, and their applications in improving thermal conductivity in matrix materials. The material this work will simulate is magnesium silicide (Mg2Si), a thermoelectric material. Thermoelectric materials, in general, become more efficient in converting heat into electrical power as their λp decreases. λp will be calculated for SWC-NTs of varying lengths, diameters, and at varying equilibration temperatures (Teq). λp will be calculated for samples of pure Mg2Si and Mg2Si with off-stoichiometry over a range of Teq values. Two methods will be used to induce the off-stoichiometry: atomic silicon (Si) substitutionals, and Si NPs. A range of stoichiometric ratios will be applied to the material by both methods, and then λp will be calculated for each of these cases. This is done so as to observe which method of stoichiometric change, given the same stoichiometric ratio, decreases λp greater, and, therefore, causes Mg2Si to be a better thermoelectric material. It is expected that increases in length will increase the λp of the SWCNT, while increases in diameter and Teq will decrease λp. It is expected that increases in atomic percent (a/o) Si and Teq will decrease λp regardless of the method of stoichiometric change, and that the Si NP method will decrease λp more than the atomic Si substitutional method.

Nanotechnology has made it possible to create materials with unique properties. This development offers new opportunities and overcomes challenges for many thermal transport applications. Yet, it requires a more fundamental scientific understanding of nanoscale transport. This thesis emphasizes how simulation, mathematical, and numerical methods can lead to more grounded studies of nanoscale thermal transport for biological and physical applications. For instance, magnetic fluid hyperthermia (MFH), an emerging cancer treatment, is a noninvasive method to selectively destroy a tumor by heating a ferrofluid-impregnated malignant tissue with minimal damage to the surrounding healthy tissue. We model the problem by considering an idealized spherical tumor that is surrounded by healthy tissue. The dispersed magnetic nanoparticles in the tumor are excited by an AC magnetic field to generate heat. The temperature distribution during MFH is investigated through a bioheat transfer relation which indicates that the P\'eclet, Joule, and Fourier numbers are the more influential parameters that determine the heating during such a thermotherapy. Thus, we show that a fundamental parametric investigation of the heating of soft materials can provide pathways for optimal MFH design. Since ferrofluid materials themselves play a key role in heating, we examine six materials that are being considered as candidates for MFH use. These are simulated to investigate the heating of ferrofluid-loaded tumors. We show that iron-platinum, magnetite, and maghemite are viable MFH candidates since they are able to provide the desired heating of a tumor which will destroy it while keeping the surrounding healthy tissues at a relatively safe temperature. Recent advances in the synthesis and nanofabrication of electron devices have lead to diminishing feature sizes. This has in turn increased the power dissipation per unit area that is required to cool the devices, leading to a serious thermal management challenge. The phonon thermal conductivity is an important material property because of its role in thermal energy transport in semiconductors. A higher thermal conductivity material is capable of removing more heat since higher frequency phonons are able to travel through it. In this thesis, the effects of surface stress on the lattice thermal conductivity are presented for a silicon nanowire. Based on a continuum approach, a phonon dispersion relation is derived for a nanowire that is under surface stress and the phonon relaxation time is employed to subsequently determine its thermal conductivity. The surface stress is found to significantly influence the phonon dispersion and thus the Debye temperature. Consequently, the phonon thermal conductivity decreases with increasing surface stress. Different magnitudes of surface stress could arise from various material coatings and through different nanofabrication processes, effects of which are generally unclear and not considered. Our results show how such variations in surface stress can be gainfully used in phonon engineering and to manipulate the thermal conductivity of a nanomaterial. The thermal transport during thermoelectric cooling is also an important property since thermoelectric devices are compact, reliable, easy to control, use no refrigerants and require lower maintenance than do more traditional refrigeration devices. We focus on the Thomson effect that occurs when there is a current flow in the presence of a temperature gradient in the material, and investigate its influence on an intrinsic silicon nanowire cooler. The temperature dependence of the Thomson effect has a significant influence on the cooling temperature. We also consider thermal nonequilibrium between electrons and phonons over the carrier cooling length in the nanowire. The results show that a strong energy exchange between electrons and phonons lowers the cooling performance, suggesting useful strategies for thermoelectric device design. / Ph. D.

Les matériaux thermoélectriques permettent de convertir de l'énergie thermique en énergie électrique. Leur rendement de conversion trop faible limite cependant leur utilisation à grande échelle. Plusieurs voies d'optimisation sont utilisés afin d'augmenter les rendements de conversion en diminuant la conductivité thermique. Dans cette thèse, nous modélisons les propriétés de transport thermique des matériaux half-Heusler parfaits et dopés qui présentent des propriétés thermoélectriques intéressantes. La méthode repose sur la théorie de la fonctionnelle de la densité pour calculer les propriétés harmoniques et anharmoniques des composés parfaits et déterminer les temps de vie des phonons. Ensuite, ces derniers sont utilisés pour écrire une équation de transport de Boltzmann pour la densité de phonons dont la résolution donne accès à la conductivité thermique. L'inclusion de défauts ponctuels a pour objectif de réduire la conductivité thermique par diffusion des phonons. Pour modéliser leur effet dans un régime de forte concentration une méthode champ moyen a été développée et appliquée aux half-Heusler. Pour traiter le régime dilué, une méthode faisant appel aux fonctions de Green a été utilisée. Ces deux méthodes montrent que des réductions significatives de conductivité thermique des composés NiTiSn, NiZrSn et NiHfSn sont déjà obtenues pour des concentrations de 10 % en dopants. / Thermoelectric materials provide a way to convert thermal energy into electrical energy. Nonetheless, their low efficiency is the main obstacle for global scale applications. Experimentally, specific treatments can lead to great improvement in the efficiency, mainly by lowering the thermal conductivity. This thesis is aimed at calculating from first principles, the thermal transport properties in perfect and doped half-Heusler thermoelectric materials. We begin with a theoretical analysis of the harmonic and anharmonic properties of phonons for perfect phases.The density functional theory is used to deduce the phonons lifetime from phonon-phonon interactions. The lifetimes are integrated into the Boltzmann transport equation for the phonon density, which solution allows us to compute fully ab initio the lattice thermal conductivity. The purpose of point defects is to scatter the phonons and thus reduce thermal conductivity. We developed two methods to account for the defects on thermal transport. The first one, based on a mean field approach, is suitable for the high concentration regimes. The second one in the framework of Green functions theory is used for dilute regimes. Both methods consistently show that the main reduction of thermal conductivity is already obtained within around 10 % of solute elements in NiTiSn, NiZrSn and NiHfSn.

In recent years, the use of first-principles based atomistic modeling technique has become extremely popular to gain better insights on the various locally modulated electronic properties of nano materials and structures. Atomistic modeling offers the benefit of predicting crystal structures, visualizing orbital distribution and electron density, as well as understanding material properties which are hard to access experimentally. The single layer MoS2 has emerged as a suitable choice for the next generation nano devices, owing to its distinctive electrical, optical and mechanical properties like, better electrostatics, increased photo luminescence, higher mechanical flexibility, etc. The realization of decananometer scale digital switches with the single layer MoS2 as the channel may provide many significant advantages such as, high On/Off current ratio, excellent electrostatic control of the gate, low leakage, etc. However, there are quite a few critical issues such as, forming low resistance source/drain contacts, achieving higher effective mobility, ensuring large scale controlled growth, etc. which need to be addressed for successful implementation of the atomically thin transistors in integrated circuits. Recent experimental demonstration showing the coexistence of metallic and semiconducting phases in the same monolayer MoS2, has attracted much attention for its use in ultra-low contact resistance-MoS2 transistors. Howbeit, the electronic structures of the metallic-to-semiconducting phase boundaries, which appear to dictate the carrier injection in such transistors, are not yet well understood. In this work, we first develop the geometrically optimized atomistic models of the 2H-1T′ hetero-phase structures with two distinct phase boundaries, β and γ. We then apply density functional theory to calculate the electronic structures for those optimized geometries. Furthermore, we employ non equilibrium Green’s function formalism to evaluate the transmission spectra and the local density of states in order to assess the Schottky barrier nature of the phase boundaries. Nonetheless, the symmetry of the source-channel and drain-channel junction, is a unique property of a metal-oxide semiconductor field effect transistor (MOSFET), which needs to be preserved while realizing sub-10 nm channel length devices using advanced technology. Employing experimental-findings-driven atomistic modeling technique, we demonstrate that such symmetry might not be preserved in an atomically thin phase-engineered MoS2- based MOSFET. It originates from the two distinct atomic patterns at phase boundaries (β and β*) when the semiconducting phase (channel) is sandwiched between the two metallic phases (source and drain). Next, using first principles based quantum transport calculations we demonstrate that due to the clusterization of “Mo” atoms in 1T′ MoS2, the transmission along the zigzag direction is significantly higher than that in the armchair direction. Moreover, to achieve excellent impedance matching with various metal contacts (such as, “Au”, “Pd”, etc.), we further develop the atomistic models of metal-1T′ MoS2 edge contact geometries and compute their resistance values. Other than the charge carrier transport, analysing the heat transport across the channel is also crucial in designing the ultra-thin next generation transistors. Hence, in this thesis work, we have investigated the electro-thermal transport properties of single layer MoS2, in quasi ballistic regime. Besides the perfect monolayer in its pristine form, we have also considered various line defects which have been experimentally observed in mechanically exfoliated MoS2 samples. Furthermore, a comprehensive study on the phonon thermal conductivity of a suspended monolayer MoS2, has been incorporated in this thesis. The studies presented in this thesis could be useful for understanding the carrier transport in atomically thin devices and designing the ultra-thin next generation transistors.