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


Virgil, Kyle Allan (2024) Polarization-Resolved, Oblique Incidence Terahertz Spectroscopy of Highly Uniform 2D Hybrid Perovskite Films. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/cr97-p373.


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.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:Terahertz spectroscopy, hybrid perovskite thin films, 2D perovskite synthesis, terahertz anisotropy, phonon dynamics, oblique incidence transmission
Degree Grantor:California Institute of Technology
Division:Chemistry and Chemical Engineering
Major Option:Chemistry
Awards:The Lucy Guernsey Service Award, 2019.
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Blake, Geoffrey A. (advisor)
  • Atwater, Harry Albert (advisor)
Thesis Committee:
  • Cushing, Scott K. (chair)
  • Goddard, William A., III
  • Dabiri, John O.
  • Blake, Geoffrey A.
  • Atwater, Harry Albert
Defense Date:28 August 2023
Funding AgencyGrant Number
Resnick Sustainability Institute Graduate Research FellowshipUNSPECIFIED
Caltech Space Solar Power ProjectUNSPECIFIED
Record Number:CaltechTHESIS:05192024-000137690
Persistent URL:
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:16391
Deposited By: Kyle Virgil
Deposited On:23 May 2024 16:18
Last Modified:17 Jun 2024 19:06

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