Lattice Dynamics and Optoelectronic Properties of Vacancy-Ordered Double Perovskite Cs2TeX6 (X = Cl–, Br–, I–) Single Crystals

Folgueras, Maria C.; Jin, Jianbo; Gao, Mengyu; Quan, Li Na; Steele, Julian A.; Srivastava, Shivani; Ross, Michael B.; Zhang, Rui; Seeler, Fabian; Schierle-Arndt, Kerstin; Asta, Mark; Yang, Peidong

doi:10.1021/acs.jpcc.1c08332

Title: Lattice Dynamics and Optoelectronic Properties of Vacancy-Ordered Double Perovskite Cs₂TeX₆ (X = Cl^–, Br^–, I^–) Single Crystals

Journal Article · Tue Nov 09 00:00:00 EST 2021 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.1c08332· OSTI ID:1833364

^[1];

^[2]; Quan, Li Na ^[3];

^[4]; Srivastava, Shivani ^[2];

^[5]; Zhang, Rui ^[6]; Seeler, Fabian ^[7]; Schierle-Arndt, Kerstin ^[8]; Asta, Mark ^[2];

^[9]

Univ. of California, Berkeley, CA (United States); California Research Alliance (CARA) and BASF Corporation, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Katholieke Univ. Leuven, Heverlee (Belgium). cMACS, Department of Microbial and Molecular Systems
Univ. of California, Berkeley, CA (United States)
California Research Alliance (CARA) and BASF Corporation, Berkeley, CA (United States)
BASF SE, Ludwigshafen am Rhein (Germany)
California Research Alliance (CARA) and BASF Corporation, Berkeley, CA (United States); BASF SE, Ludwigshafen am Rhein (Germany)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); California Research Alliance (CARA) and BASF Corporation, Berkeley, CA (United States)

The soft, dynamic lattice of inorganic lead halide perovskite CsPbX₃ (X = Cl^⁻, Br^⁻, I^⁻) leads to the emergence of many interesting photophysical and optoelectronic phenomena. However, probing their lattice dynamics with vibrational spectroscopy remains challenging. The influence of the fundamental octahedral building block in the perovskite lattice can be better resolved in zero-dimensional (0D) vacancy-ordered double perovskites of form A₂BX₆. Here we study Cs₂TeX₆ (X = Cl^⁻, Br^⁻, I^⁻) single crystals to yield detailed insight into the fundamental octahedral building block and to explore the effect that its isolation in the crystal structure has on structural and electronic properties. The isolated [TeX₆]^2- octahedral units serve as the vibrational, absorbing, and emitting centers within the crystal. Serving as the vibrational centers, the isolated octahedra inform the likelihood of a random distribution of 10 octahedral symmetries within the mixed-halide spaces, as well as the presence of strong exciton-phonon coupling and anharmonic lattice dynamics. Serving as the absorbing and emitting centers, the isolated octahedra exhibit compositionally tunable absorption (1.50-3.15 eV) and emission (1.31-2.11 eV) energies. Due to greater molecular orbital overlap between neighboring octahedra with increasing halide anion size, there is a transition from a more molecule-like electronic structure in Cs₂TeCl₆ and Cs₂TeBr₆-as expected from the effective 0D nature of these single crystals-to a dispersive electronic structure in Cs₂TeI₆, typical of three-dimensional (3D) bulk single crystals.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1833364

Journal Information:: Journal of Physical Chemistry. C, Vol. 125, Issue 45; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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CSD 2092634: Experimental Crystal Structure Determination C., Folgueras, Maria; Jianbo, Jin,; Mengyu, Gao, https://doi.org/10.25505/fiz.icsd.cc287kbf The current record is supplemented by this dataset	dataset	January 2021
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Title: Lattice Dynamics and Optoelectronic Properties of Vacancy-Ordered Double Perovskite Cs2TeX6 (X = Cl–, Br–, I–) Single Crystals

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Title: Lattice Dynamics and Optoelectronic Properties of Vacancy-Ordered Double Perovskite Cs₂TeX₆ (X = Cl^–, Br^–, I^–) Single Crystals