Journal article
Tuning the Optical Absorption Edge of Vacancy-Ordered Double Perovskites through Metal Precursor and Solvent Selection
Chemistry of materials, Vol.36(19), pp.9625-9635
08 Oct 2024
PMID: 39398367
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
Vacancy-ordered double perovskites with the formula A(2)MX(6) (where A is a +1 cation, M is a +4 metal, and X is a halide ion) offer improved ambient stability over other main-group halide AMX 3 perovskites and potentially reduced toxicity compared to those containing lead. These compounds are readily formed through a number of synthetic routes; however, the manner in which the synthetic route affects the resulting structure or optoelectronic properties has not been examined. Here, we investigate the role of distinct precursors and solvents in the formation of the indirect band gap vacancy-ordered double perovskite Cs2TeBr6. While Cs2TeBr6 can be synthesized from TeBr(4 )or TeO2, we find that synthesis from TeBr4 is more sensitive to solvent selection, requiring a polar solvent to enable the conversion of TeBr4. Synthesis from TeO2 proceeds in all of the organic solvents tested, provided that HBr is added to solubilize TeO2 and enable the formation of [TeBr6](2-). Furthermore, the choice of metal precursor and solvent impacts the product color and optical absorption edge, which we find arises from particle size effects. The emission energy remains unaffected, consistent with the idea that emission in these zero-dimensional structures arises from the isolated [TeBr6](2-) octahedra, which undergo dynamic Jahn-Teller distortion rather than band-edge recombination. Our work highlights how even minor changes in synthetic procedures can lead to variability in metrics such as the absorption edge and emission lifetime and sheds light on how the optical properties of these semiconductors can be controlled for light-emitting applications.
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Details
- Title
- Tuning the Optical Absorption Edge of Vacancy-Ordered Double Perovskites through Metal Precursor and Solvent Selection
- Creators
- Alexandra Brumberg - University of California, Santa BarbaraOwen Kuklinski - University of California, Santa BarbaraGreggory T. Kent - University of California, Santa BarbaraEmily E. Morgan - University of California, Santa BarbaraAlexander A. Mikhailovsky - University of California, Santa BarbaraT. Amanda Strom - University of California, Santa BarbaraMichael L. Chabinyc - University of California, Santa BarbaraRam Seshadri - University of California, Santa BarbaraUniv. of California, Santa Barbara, CA (United States)
- Publication Details
- Chemistry of materials, Vol.36(19), pp.9625-9635
- Publisher
- Amer Chemical Soc
- Number of pages
- 11
- Grant note
- University of California, Santa Barbara; University of California System DoD ONR DURIP; United States Department of Defense; United States Navy; Office of Naval Research N00014-19-1-2527 / Optical Characterization Facility (DoD ARO DURIP) DE-AC02-06CH11357 / U.S. Department of Defense; United States Department of Defense 66886LSRIP / U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences; United States Department of Energy (DOE) University of California, Office of the President; University of California System
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemistry
- Web of Science ID
- WOS:001314262700001
- Scopus ID
- 2-s2.0-85204295646
- Other Identifier
- 991022053795104721
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- Web of Science research areas
- Chemistry, Physical
- Materials Science, Multidisciplinary