Skip to Main Content
 

Global Search Box

 
 
 

ETD Abstract Container

Abstract Header

Exploring the Electronic and Magnetic Properties of Low Dimensional Hybrid Transition Metal Halide Perovskite Derivatives

Holzapfel, Noah Philip
http://orcid.org/0000-0002-4566-4033
http://rave.ohiolink.edu/etdc/view?acc_num=osu1669912285839579

Abstract Details

2022, Doctor of Philosophy, Ohio State University, Chemistry.
Perovskite-based materials provide an exemplary platform to explore fundamental structure-property relationships. The relative simplicity of the perovskite crystal structure and a plethora of interesting properties related to purposes such as optoelectronics, multiferroics, and superconductivity, has sparked immense research interest. For halide perovskite variants, research has focused primarily on APbX3 (A = Cs+, CH3NH3+, NH2CHNH2+; X = Cl−, Br−, I−) perovskites for photovoltaic applications. One of the most impressive features of the halide perovskite is the ease of chemical substitution, which has resulted in a wide variety of structural variations. Halide perovskite materials containing transition metals offer a broader range of applications due to the possibility of diamagnetic and paramagnetic electronic configurations. Here we explore halide perovskite derivatives containing transition metals to understand the optical and magnetic properties that arise in low dimensional crystal structures. Following the first introductory chapter, Chapter 2 looks to expand on the known compositional space of the (CH3NH3)2M′MʺX6 halide double perovskites by introducing Rh3+ at the Mʺ site. Here, we synthesized (CH3NH¬3)2M′RhX6 (M′ = Na+, Ag+; X = Cl−, Br−) and looked to understand the optical properties that arise from the one-dimensional chain structure of these hexagonal 2H perovskite variants. This sets the foundation for Chapter 3, which explores two-dimensional layered perovskites containing the Ag–Rh–X inorganic framework. By replacing CH3NH3+ with a bulky organic cation, the crystal structure transitions from one-dimensional chains to two-dimensional layers. The optical properties are further explored in comparison to the previously studied hexagonal perovskites. Changes in the absorption spectra are explained by changes in the octahedral connectivity and ability of orbitals to hybridize. Chapter 4 focuses on the structural phase transitions and magnetic properties of a family of A’2MnCl4 (A’ = organic ammonium cation) layered perovskites. The presence of high-spin d5 Mn2+-centers leads to the observance of both two-dimensional and three-dimensional antiferromagnetic ordering. The structural phase transitions are explained by changes in the observed tilting schemes related to hydrogen bonding interactions. The magnetic transitions are understood through a combination of SQUID magnetometry and neutron powder diffraction. Chapter 5 further explores the structural phase transitions and magnetism in a similar series of compounds containing Cu2+. The d9 electronic configuration results in a Jahn-Teller electronic distortion which drastically alters the structural transitions and magnetic properties compared to the Mn2+ analogues. Chapter 6 further builds upon the structural driving forces explored in Chapters 4 and 5 with a series of diamagnetic layered perovskites (C6H5(CH2)nNH3)2CdCl4 (n = 1 and 2). Structural distortions that lead to polar crystal classes are observed and verified through single crystal X-ray diffraction and second harmonic generation measurements.
Patrick Woodward (Advisor)
Yiying Wu (Committee Member)
Joshua Goldberger (Committee Member)
259 p.
Chemistry; Materials Science
Perovskite; Optical Properties; Electronic Structure; Magnetism; Crystallography; Phase Transitions; Hybrid Materials; Metal Halide; Dielectric Properties;

Recommended Citations

Citations

  • Holzapfel, N. P. (2022). Exploring the Electronic and Magnetic Properties of Low Dimensional Hybrid Transition Metal Halide Perovskite Derivatives [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1669912285839579

    APA Style (7th edition)

  • Holzapfel, Noah. Exploring the Electronic and Magnetic Properties of Low Dimensional Hybrid Transition Metal Halide Perovskite Derivatives. 2022. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1669912285839579.

    MLA Style (8th edition)

  • Holzapfel, Noah. "Exploring the Electronic and Magnetic Properties of Low Dimensional Hybrid Transition Metal Halide Perovskite Derivatives." Doctoral dissertation, Ohio State University, 2022. http://rave.ohiolink.edu/etdc/view?acc_num=osu1669912285839579

    Chicago Manual of Style (17th edition)

osu1669912285839579
40
© 2022, all rights reserved.
This open access ETD is published by The Ohio State University and OhioLINK.