Experimental investigations of energy carrier interactions with atomic disorders and artificial long-range orders




Smith, Brandon Paul

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The field of nanoscale energy transport, conversion, and storage is at an exciting time with next-generation devices manipulating discrete energy carriers, e.g. phonons, photons, and electrons, in confined dimensions arriving closer to commercialization, such as solid-state flexible electronics and optoelectronics utilizing one dimension (1D) and two dimensional (2D) nanomaterials. The transport dynamics of quasiparticles and their coupling are modified, notably in low dimensional nanomaterials, with the inclusion of disorder and artificial long-range order. Through this lens, it is possible to probe interesting physics and draw out intrinsic properties of the nanomaterials. This is especially important for electronic systems and energy conversion & storage devices where heat generation and dissipation within nano- and microscale locations of nonequilibrium impedes continued advancement. This thesis examines outstanding questions concerning nanoscale thermal and thermoelectric transport in low-dimensional materials to further understanding of crystal disorder and artificial long-range order. Specifically, the material systems investigated are alloy disorder and surface roughness in semiconducting silicon germanium (SiGe) nanowires, microscale rippling in layered molybdenum disulfide (MoS2) flakes, intra- and interlayer interactions in bulk and monolayer MoS2, and artificially created, long-range domain walls in twisted bilayer graphene (TBG). The fundamental questions are addressed through electrothermal, optothermal, and scanning probe metrology techniques. First, eight-probe thermal conductivity measurements of SiGe nanowires show that alloying suppresses thermal transport, and the mean-free-paths of low-frequency phonons are suppressed by diffuse surface roughness scattering in nanowires. The diffuse surface scattering results in length-independent thermal conductivity for lengths over two micrometers. Similarly, four-probe thermal conductivity measurements reveal that microscale ripples have negligible effects on phonon transport in 2D layers as the ripple wavelengths and curvatures are much larger than the phonon mean free paths and wavelengths. The peak thermal conductivity is found to increase with decreasing Raman scattering intensity in the frequency range with vanishing phonon density of states in MoS2 indicating an important role of point defect scattering. In addition, this dissertation presents an experimental effort to employ micro-Raman spectroscopy to investigate local nonequilibrium among different phonon polarizations in MoS2 inside the focused laser spot. It also describes an exploration of ultra-high vacuum scanning probe microscopy for probing the local thermoelectric property of twisted bilayer graphene moiré superstructures.


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