Polarization-Resolved, Oblique Incidence Terahertz Spectroscopy of Highly Uniform 2D Hybrid Perovskite Films

Author: Virgil, Kyle Allan

Year: 2024

Degree: Dissertation (Ph.D.)

Advisors: Blake, Geoffrey A.; Atwater, Harry Albert

Committee Members: Cushing, Scott K.; Goddard, William A., III; Dabiri, John O.; Blake, Geoffrey A.; Atwater, Harry Albert

Option: Chemistry

DOI: 10.7907/cr97-p373

Abstract

This thesis details the development and optimization of thin film THz transmission measurements to extract spectrally resolved vibrational anisotropy in high quality layered hybrid perovskite materials. After an introduction in Chapter 1, Chapter 2 details the design, construction, and characterization of a terahertz time-domain spectrometer from scratch. Generalized THz propagation models are presented which enable accurate and diverse implementation of THz analysis. In Chapter 3, hybrid perovskite materials are introduced and our efforts towards reliably synthesizing high quality thin film perovskites using spin coating techniques are discussed. We find that optimized thin films are achieved from tailored synthetic conditions which depend on perovskite composition. In Chapter 4, we present our investigation into the elusive yet highly influential THz vibrational properties of 2D hybrid perovskite systems. A novel implementation of oblique-incidence THz transmission measurements reveals previously unseen vibrational excitations which provide valuable insight into the fundamental photodynamics that govern perovskite optoelectronics. We conclude in Chapter 5. This thesis serves to enhance the accessibility of powerful THz spectroscopic techniques as well as support the realization of promising perovskite renewable energy technologies.

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