Defense Date

5-12-2022

Graduation Date

Summer 8-13-2022

Availability

One-year Embargo

Submission Type

dissertation

Degree Name

PhD

Department

Chemistry and Biochemistry

Committee Chair

Jennifer A. Aitken

Committee Member

Michael Van Stipdonk

Committee Member

Aaron Bloomfield

Committee Member

Thomas Albrecht-Schoenzart

Keywords

quaternary, sulfides, noncentrosymmetric, diamond-like, nonlinear optical materials, crystal structure

Abstract

In this work, several new quaternary sulfides were synthesized and investigated for their potential applications in optics. Chapter 1 provides an overview of nonlinear optical (NLO) materials in general, including their applications, ideal characteristics, current deficiencies, and strategies for the discovery of new candidate NLO materials, particularly those for use in the infrared (IR). Two families of compounds are investigated in this work, including Ln3LiTS7 (3-1-1-7) compounds and I4-II-IV2-VI7 (4-1-2-7) diamond-like semiconductors (DLSs). All products were synthesized via traditional high-temperature, solid-state synthesis and their structures were solved and refined through single crystal X-ray diffraction. Chapter 2 focuses on the rare-earth-containing 3-1-1-7 compounds, including nine previously unreported and nine further characterized compounds. Following the general formula of Ln3LiTS7 where Ln = La, Ce, Pr, Nd, Sm, Gd, Dy and T = Si, Ge, Sn, a systematic study of homovalently substituted compounds was carried out. Chapter 3 reports the synthesis and crystal structures of two new Cu-containing 4-1-2-7 DLSs, Cu4FeGe2S7 and Cu4CoGe2S7. Chapter 4 focuses on a novel Li-containing 4-1-2-7 DLS, Li4CdGe2S7. This compound, derived from the hexagonal form of diamond, crystallizes in the Cc space group with the Cu5Si2S7 structure type.

Language

English

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