Low-energy electronic structure of perovskite and Ruddlesden-Popper semiconductors in the Ba-Zr-S system probed by bond-selective polarized x-ray absorption spectroscopy, infrared reflectivity, and Raman scattering

Ye, Kevin; Koocher, Nathan Z.; Filippone, Stephen; Niu, Shanyuan; Zhao, Boyang; Yeung, Matthew; Bone, Sharon; Robinson, Adam J.; Vora, Patrick; Schleife, André; Ju, Long; Boubnov, Alexey; Rondinelli, James M.; Ravichandran, Jayakanth; Jaramillo, R.

doi:10.1103/physrevb.105.195203

Title: Low-energy electronic structure of perovskite and Ruddlesden-Popper semiconductors in the Ba-Zr-S system probed by bond-selective polarized x-ray absorption spectroscopy, infrared reflectivity, and Raman scattering

Journal Article · Wed May 11 00:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.105.195203· OSTI ID:1877345

^[1]; Koocher, Nathan Z. ^[2]; Filippone, Stephen ^[1]; Niu, Shanyuan ^[3]; Zhao, Boyang ^[3]; Yeung, Matthew ^[1]; Bone, Sharon ^[4]; Robinson, Adam J. ^[5]; Vora, Patrick ^[5];

^[6]; Ju, Long ^[1]; Boubnov, Alexey ^[7];

^[2];

^[3];

^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Northwestern Univ., Evanston, IL (United States)
Univ. of Southern California, Los Angeles, CA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
George Mason Univ., Fairfax, VA (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)
Karlsruhe Inst. of Technology (KIT) (Germany)

Chalcogenides in perovskite and the related layered Ruddlesden-Popper crystal structures (chalcogenide perovskites for brevity) are an exciting family of semiconductors but remain experimentally little studied. Chalcogenide perovskites share crystal structures and some physical properties with ionic compounds such as oxide and halide perovskites, but the metal-chalcogen bonds responsible for semiconducting behavior are substantially more covalent than in these more-studied perovskites. In this study, we use complementary experimental and theoretical methods to study how the mixed ionic-covalent Zr-S bonds support the electronic structure and physical properties of perovskite BaZrS₃ and Ruddlesden-Popper Ba₃Zr₂S₇. We apply theoretical methods to assign features of experimentally measured x-ray absorption spectroscopy (XAS) to particular orbital transitions, enabling a clear physical interpretation of angle-dependent, polarized XAS data measured on single-crystal samples, and an atomistic view of the covalent bonding network that facilitates charge transport. Polarized Raman measurements identify signatures of crystalline anisotropy in Ba₃Zr₂S₇ and enable the first assignments of mode symmetry in this material. Infrared reflectivity reveals electronic transport properties that augur well for the use of chalcogenide perovskites in optoelectronic and energy-conversion technologies.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF); US Army Research Office (ARO); German Research Foundation (DFG)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; INST 40/575-1 FUGG

OSTI ID:: 1877345

Journal Information:: Physical Review. B, Vol. 105, Issue 19; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Low-energy electronic structure of perovskite and Ruddlesden-Popper semiconductors in the Ba-Zr-S system probed by bond-selective polarized x-ray absorption spectroscopy, infrared reflectivity, and Raman scattering

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