Graduation Year

2026

Document Type

Dissertation

Degree

Ph.D.

Degree Name

Doctor of Philosophy (Ph.D.)

Degree Granting Department

Chemistry

Major Professor

Ioannis Spanopoulos, Ph.D.

Committee Member

Xiaomei Jiang, Ph.D.

Committee Member

Kirpal Bisht, Ph.D.

Committee Member

Chavdar Slavov, Ph.D.

Keywords

Chiral Semiconductors, Environmentally Friendly, Fullerene-based Materials, Perovskites, Porous Materials

Abstract

Metal halide semiconductors have rejuvenated the attention of the scientific community for the last two decades owing to their photophysical and electronic properties. However, these materials have some limitations that hinder their commercialization and widespread application. One major limitation of these materials is their instability under ambient and operating conditions of moisture, head, light and radiation exposure. Here, we report multiple chemical design strategies to address the stability issues of these materials while simultaneously maintaining their exceptional optoelectronic properties. Such design strategies allowed the acquisition of the first members of the family of porous metal halide semiconductors which exhibit record stability performances for multiple years in water. Furthermore, we report the first crystalline fullerene-based metal halide semiconductor and its utilization as an interlayer among the light harvesting layer and the electron transport layer in ideal band-gap perovskite solar cells which had a significant improvement to their power conversion efficiencies and long-term operational stability. Another major result reported here is the development of environmentally stable and friendly chiral metal halide materials which allowed for investigating the structure-property relationships in such class of chiral semiconductors. Lastly, we uncovered the stability advantages of phosphonium-based (R-P(R’)3+) metal halide semiconductors over their ammonium-based (R-N(R’)3+) analogs and we investigated for the first time the electrochemical and PFAS sensing capabilities of hybrid phosphonium-based lead iodide materials.

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