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Matthew R Linaburg masters thesis.pdf (6.33 MB)

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Studies of Halide Perovskites CsPbX3, RbPbX3 (X=Cl-, Br-, I-), and Their Solid Solutions

Linaburg, Matthew Ronald
http://orcid.org/0000-0002-4172-0771
http://rave.ohiolink.edu/etdc/view?acc_num=osu1449074303

Abstract Details

2015, Master of Science, Ohio State University, Chemistry.
Halide perovskites have garnered much attention in recent years as a potential material for photovoltaics, semiconductors, transparent conductors, thermistors, and electromagnetic radiation detectors. Lead halide perovskites with the formula APbX3, where A = Cs+ and X = Cl-, Br-, or I- have been shown to adopt a distorted perovskite structure (space group Pnma) with desirable band gaps and electronic properties for photovoltaic and detector applications. Experiments were conducted herein to better understand the stability limit of the lead halide perovskite structure through A-site substitution with a smaller Rb+ ion. Variable X-ray powder diffraction measurements were used to identify and characterize perovskite phase transitions at elevated temperatures for RbPbCl3, RbPbBr3, and RbPbI3, all of which form non-perovskite compounds at room temperature. Solid solutions Rb(x)Cs(1-x)PbCl3 and Rb(x)Cs(1-x)PbBr3 were synthesized as a means to stabilize the high temperature perovskite phases observed in the variable temperature experiments, and to further study the effects of octahedral tilting on the band gap of the compound. The RbPbX3 (X = Cl-, Br-, and I-) phases do not form as perovskites at room temperature, but RbPbCl3 and RbPbBr3 undergo phase transitions to perovskite structures at higher temperature. RbPbCl3 transitions first at 320 °C to a tetragonally distorted perovskite structure (space group P4/mbm) then to the cubic perovskite structure (space group Pm-3m) at 340 °C. RbPbBr3 also undergoes two phase transitions, first to an orthorhombically distorted perovskite structure (space group Pnma) at 250 °C then to a tetragonally distorted perovskite structure (space group P4/mbm) at 350 °C. Solid solutions of Rb(x)Cs(1-x)PbCl3 and Rb(x)Cs(1-x)PbBr3 resulted in a orthorhombic perovskite structure (space group Pnma) at room temperature. The orthorhombic distortion increased as the Rb+ content increased, due to increased tilting of the lead-centered octahedra. For the Cl- solid solution, the perovskite structure was retained for Rb+ substitution up to a value of x = 0.9, while for the Br- solid solutions a perovskite structure could be obtained up to x = 0.6. As the Rb+ substitution increases, the band gap of the compound increases. The band gap of the Rb(x)Cs(1-x)PbCl3 (x = 0 - 0.6) solid solution increases from 2.97 eV to 3.08 eV, while the Rb(x)Cs(1-x)PbBr3 solid solutions increases from 2.13 eV to 2.30 eV across the same x = 0 - 0.6 range. The increase is a result of greater octahedral distortions, which were characterized by measuring the Pb-X-Pb bond angles.
Patrick Woodward, Dr. (Advisor)
Anne Co, Dr. (Committee Member)
105 p.
Chemistry; Inorganic Chemistry; Materials Science
perovskite; crystallography; cubic; orthorhombic; tetragonal; perovskite; band gap; bond angle; lattice parameters; xrd refinement; XRD; variable temperature XRD; halide; chloride; bromide; rubidium; cesium; lead; diffractogram; powder XRD; solid solution

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Citations

  • Linaburg, M. R. (2015). Studies of Halide Perovskites CsPbX3, RbPbX3 (X=Cl-, Br-, I-), and Their Solid Solutions [Master's thesis, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1449074303

    APA Style (7th edition)

  • Linaburg, Matthew. Studies of Halide Perovskites CsPbX3, RbPbX3 (X=Cl-, Br-, I-), and Their Solid Solutions. 2015. Ohio State University, Master's thesis. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1449074303.

    MLA Style (8th edition)

  • Linaburg, Matthew. "Studies of Halide Perovskites CsPbX3, RbPbX3 (X=Cl-, Br-, I-), and Their Solid Solutions." Master's thesis, Ohio State University, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=osu1449074303

    Chicago Manual of Style (17th edition)

osu1449074303
5,469
© 2015, some rights reserved.Creative Commons License Studies of Halide Perovskites CsPbX3, RbPbX3 (X=Cl-, Br-, I-), and Their Solid Solutions by Matthew Ronald Linaburg is licensed under a Creative Commons Attribution-NonCommercial-NoDerivs 3.0 Unported License. Based on a work at etd.ohiolink.edu.
This open access ETD is published by The Ohio State University and OhioLINK.