Thermal Conduction in Amorphous Materials and the Role of Collective Excitations

Citation

Moon, Jaeyun (2020) Thermal Conduction in Amorphous Materials and the Role of Collective Excitations. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/Z23D-Z566. https://resolver.caltech.edu/CaltechTHESIS:01162020-015608435

Abstract

The atomic vibrations and thermal properties of amorphous dielectric solids are of fundamental and practical interest. For applications, amorphous solids are widely used as thermal insulators in thermopile and other detectors where low thermal conductivity directly sets the sensitivity of the detector. Amorphous solids are of fundamental interest themselves because the lack of atomic periodicity complicates theoretical development. As a result, the lower limits of thermal conductivity in solids as well as the nature of the vibrational excitations that carry heat remain active topics of research.

In this thesis, we use numerical and experimental methods to investigate the thermal conduction in amorphous dielectrics. We begin by using molecular dynamics to investigate the thermal conductivity of amorphous nanocomposites. We find that mismatching the vibrational density of states of constituent materials in the composite is an effective route to achieve exceptionally low thermal conductivity in fully dense solids.

We then transition to examining the properties of the atomic vibrations transporting heat in amorphous solids. For decades, normal mode methods have been used extensively to study thermal transport in amorphous solids. These methods naturally assume that normal modes are the fundamental vibrational excitations transporting heat. We examine the predictions from normal mode analysis that are now able to be tested against experiments, and we find that the predictions from these methods do not agree with experimental observations. For instance, normal mode methods predict that the low frequency normal modes are scattered by anharmonic interactions as in single crystalline solids. However, temperature dependent thermal conductivity measurements demonstrate a typical glassy temperature dependence inconsistent with normal modes scattering through anharmonic interactions. These discrepancies suggest that normal modes are not the fundamental heat carriers in amorphous dielectrics.

To identify the actual heat carriers, we draw on fundamental concepts from many- body physics and inelastic scattering theory that dictate that the excitation energies of a many-body interacting system are given by the poles of the single-particle Green's function. The imaginary part of this function is proportional to the dynamic structure factor that is directly measured in inelastic scattering experiments. Collective excitations of a given energy and wavevector can thus be identified from peaks in the dynamic structure factor; their damping is given by the broadening of the peak. Using these concepts from many-body physics, the physical picture that emerges is that heat is carried in large part by a gas of weakly interacting collective excitations with a cutoff frequency that depends on the atomic structure and composition of the glass.

We test this picture using numerical and experimental inelastic scattering measurements on amorphous silicon, a commonly studied amorphous solid. We observe collective excitations up to 10 THz, well into the thermal spectrum, and far higher than previous inelastic scattering measurements on other glasses. Our numerical and experimental evidence also confirms that the collective excitations are damped by structural disorder rather than anharmonic interactions and that they dominate the thermal conduction in amorphous silicon. Subsequent analysis shows that these high frequency acoustic excitations are supported in amorphous silicon due to a large sound velocity and monatomic composition, suggesting that other monatomic amorphous solids with large sound velocities may also support these thermal excitations.

Overall, our results provide strong evidence that the heat carriers in amorphous dielectrics are collective excitations rather than normal modes. This change in physical picture advances our understanding of atomic dynamics in glasses and also provides a foundation for realizing dielectric solids with ultralow thermal conductivity.

Thesis Files