The correlated electron systems which are the subject of this thesis are the strong electron–phonon coupling superconductor HfV2, and the localised moment magnetic systems of the alloy series Pd2REIn (RE = Gd, Tb, Ho, Er and Yb).

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Magnetic properties are becoming increasingly important, especially with the advent of new technologies such as data storage, spintronics, and magnetic random access memory (MRAM). These technologies all benefit from the ability to characterize and optimize magnetic materials, which can be accomplished through the implementation of the magneto-optical Kerr effect (MOKE). This probing technique is described in detail along with the results of a self-built, longitudinal MOKE (L-MOKE) experiment that is used to determine the Kerr angle and ellipticity for the Heusler compound Fe2MnSn. The results from L-MOKE are combined with raw X-ray Diffraction (XRD) data in order to develop a complete picture of the material by connecting the Kerr response with the crystal structure. Trends in the crystal structure and magnetic properties of Fe2MnSn are developed and analyzed in order to isolate crystallographic directions that are primarily responsible for unique magnetic properties such as perpendicular magnetic anisotropy. Complementary techniques are also introduced to further the capabilities from a single geometry MOKE experiment to a compound experiment using all three geometries of MOKE with the ability to probe micro-structures, determine magneto-optical parameters, and create magnetic domain images.

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Thermoelectric materials convert temperature gradients into electricity and vice-versa. These materials utilize the Seebeck effect for power generation and function without moving parts and are highly reliable. The efficiency of thermoelectric devices is related to the dimensionless figure of merit for the constituent materials, defined as where S is the Seebeck coefficient, is the electrical conductivity, is the thermal conductivity and T is the temperature. Maximizing ZT is very challenging because of interdependence of parameters, for example, increasing the electrical conductivity by increasing the carrier concentration invariably lowers S and vice versa. Presently numerous thermoelectric materials are being investigated by different research groups. Despite having high thermal conductivity, half-Heusler materials are promising candidates for thermoelectric applications due to their relatively high power factor () and the ability to tune the thermal and electrical properties through substitutional doping. 2S In this research work, I have investigated the synthesis and transport properties of half Heusler series Zr 0.5Hf0.5Ni1-xPdxSn0.99Sb0.01 (0≤x≤1). Also the role of NiO and HfO2 nanoinclusions in half –Heusler matrix were studied. The half Heusler samples were prepared by solid state reaction. Resistivity, Seebeck coefficient and thermal conductivity were measured for all samples over a temperature range from room temperature to 750K. Hall effect measurements at room temperature were also performed. Addition of NiO inclusions did result in an improvement in ZT whereas addition of 3% vol HfO2 in Zr0.5Hf0.5Ni0.8Pd0.2Sn0.99Sb0.01 showed 19% improvement in ZT.

A study of the martensitic phase transition in the shape memory alloy Ni2MnGa has been carried out. Ni2MnGa is one of the group of "shape memory effect" alloys which are currently exciting considerable interest. The origin of this effect in the compound is in the phase change which takes place on cooling through T = 200 K from the cubic L21 Heusler structure to a tetragonal phase. Recently the results of band structure calculations have been used to conclude that in Ni2MnGa the structural phase transition is driven by a band Jahn-Teller distortion.

The magnetocaloric and thermomagnetic properties of the MnNiGe1-xAlx, Ni50Mn35(In1−xCrx)15 and (Mn1−xCrx)NiGe1.05 systems have been studied by x-ray diffraction, differential scanning calorimetry (DSC), and magnetization measurements. Partial substitution of Al for Ge in MnNiGe1−xAlx results in a first-order magnetostructural transition (MST) from a hexagonal ferromagnetic to an orthorhombic antiferromagnetic phase at 186 K (for x = 0.09). A large magnetic entropy change of ∆SM = -17.6 J/kg K for ∆H = 5 T was observed in the vicinity of TM = 186 K for x = 0.09. This value is comparable to those of well-known giant magnetocaloric materials, such as Gd5Si2Ge2, MnFeP0.45As0.55, and Ni50Mn37Sn13 [1]. The values of the latent heat (L = 6.6 J/g) and corresponding total entropy changes (∆ST = 35 J/kg K) have been evaluated for the MST using DSC measurements. Large negative values of ∆SM of -5.8 and -4.8 J/kg K for ∆H = 5 T in the vicinity of TC were observed for x = 0.09 and 0.085, respectively. Partial substitution of Cr for Mn in(Mn1−xCrx)NiGe1.05 results in a MST from a hexagonal paramagnetic to an orthorhombic paramagnetic phase near TM ~ 380 K (for x = 0.07). Partial substitution of Cr for In in Ni50Mn35(In1−xCrx)15 shifts the magnetostructural transition to a higher temperature (TM ~ 450 K) for x = 0.1. Large magnetic entropy changes of ∆SM = -12 (J/kgK) and ∆S = -11 (J/kgK), both for a magnetic field change of 5 T, were observed in the vicinity of TM for (Mn1−xCrx)NiGe1.05 and Ni50Mn35(In1−xCrx)15, respectively. The concentration-dependent (T-x) phase diagram of transition temperatures (magnetic, structural, and magnetostructural) has been generated using magnetic, XRD, and DSC data. The role of magnetic and structural changes on transition temperatures are discussed.

In this project, we have explored the possibility of growing high quality Heusler alloy thin films from multiphase targets. Bulk targets were found to be partially formed, i.e. not of homogeneous L21 structure, through x-ray diffraction measurements. Pulsed laser deposition is a technique that can provide a congruent transfer of material from the target to the substrate, even in some cases where the target is not of a single crystalline phase. It was the objective of this work to determine whether L21 structured thin films of Co2MnAsxGe(1-x) could be grown from multiphase targets. Measurements have been carried out to study the magnetic and structural properties of the Heusler alloys Co2MnAsxGe(1-x). The optimization parameters that were investigated were substrate type, growth temperature, laser parameters, film thickness, and other common deposition parameters. Temperature-dependent magneto-optic Kerr effect (MOKE) techniques were used to study the qualitative magnetic properties. Alternating current (AC) susceptibility (using a MOKE technique) measurements were made as a function of temperature to view the second-order transition and obtain the Curie temperatures. Frequency dependent AC susceptibility was measured to determine the frequency dependence of the AC susceptibility for Co2MnAsxGe(1-x).

High temperature waste heat recovery has been gaining attention in recent years as it forms one of the largest sources of available energy. A rapid development of thermoelectric (TE) materials that can directly convert heat into electricity through the Seebeck effect, opens promising pathway for harvesting the thermal energy from the surroundings. In order to harvest the high-quality waste heat at elevated temperature, excellent thermal and mechanical stability of the TE materials is critical for a sustainable energy harvesting. In this respect, half-Heusler (hH) alloys are one of the promising high-temperature TE materials due to their high dimensionless thermoelectric figure of merit (zT) along with excellent mechanical and thermal stability. This dissertation demonstrates novel hH compositions and microstructures for the waste heat recovery systems. Focus in the thesis is on development of high performance hH TE materials with excellent in-air thermal stability at high temperatures (>700K). This will allow manufacturing of high efficiency and durable high temperature thermoelectric generators (TEGs). In chapter 3 and 4, a comprehensive optimization of n-type MNiSn and p-type MCoSb (M = Hf, Zr, and Ti) compounds is investigated through systematic control of processing parameters during melting and sintering. The synthesis conditions were controlled to achieve the phase purity, desired microstructure and the enhanced charge-carrier transport. Optimized n-type and p-type compositions are found to exhibit zTmax ~ 1 at 773 K. Chapter 5 describes breakthrough in decoupling of TE parameters in n-type half-Heusler (hH) alloys through multi-scale nanocomposite architecture with tungsten nanoinclusions. The tungsten nanoparticles not only assist electron injection, thereby improving electrical conductivity, but also enhance the Seebeck coefficient through energy filtering effect. The microstructure comprises of disordered phases with feature sizes at multiple length scales, which assists in effective scattering of heat-carrying phonons over diverse mean-free-path ranges. Cumulatively, these effects are shown to result in outstanding thermoelectric performance of zTmax ~ 1.4 at 773 K and zTavg ~ 0.93 between 300 and 973 K. In order to deploy TE materials into a thermal energy conversion device, it is essential to understand the transformation behavior under thermal cycling at high temperatures. In-air thermal stability of the hH compositions is demonstrated in chapter 6. All the optimized compositions are found to be stable below 673 K in-air condition. The n-type MNiSn and p-type NbFeSb compounds were found to show good thermal stability even at higher temperatures (>773K), whereas MCoSb compounds did not exhibit similar level of stability. Building upon the improved material performance and thermal stability, uni-coupled TE generators are demonstrated that exhibit high power density of 13.81 W⸱cm-2 and conversion efficiency of 10.9 % under a temperature difference of 674 K. The uni-couple TEG device shows stable performance for more than 150 hours at 873 K in air. These results are very promising for deployment of TE materials in waste heat recovery systems. / Doctor of Philosophy / Based on the 2012 international energy agency (IEA) report, global waste heat energy is estimated to be in the range of 246 Exajoule (1 EJ = 10¹⁸ J). Tapping even small fraction of this wasted energy through thermal energy harvesting techniques will allow us to generate significant magnitude of green energy. Thermoelectrics (TEs) are one of the most promising thermal energy conversion materials as they offer cost-effective and environmentally friendly option with solid-state silent operation and scalability. Among many different options for high temperature TE materials, half-Heusler system is one of the leading candidates as it has the potential to provide high performance and thermal stability at temperatures as high as 873 K. The progress in developing practical half-Heusler materials has been limited for last two decades. Despite many publications, the maximum figure of merit (zT) of n-type half-Heusler materials has been stagnant (zT ~ 1.0). Further, there has been a lack of focus towards module development that can operate under realistic conditions. This dissertation provides comprehensive studies on novel thermoelectric compositions and nanocomposites that are suitable for manufacturing of high temperature modules. Microstructural architectures proposed here provide the ability to tailor electronic transport and phonon scattering beyond the commonly demonstrated regimes. Optimized materials were successfully implemented in efficient and stable thermoelectric generator exhibiting power density on the order of 13.81 W⸱cm⁻² , which is 1400 % higher than that of the fuel cell (~1 W⸱cm⁻² ).