Orientational Glass Formation in Substituted Hybrid Perovskites

Mozur, Eve M.; Maughan, Annalise E.; Cheng, Yongqiang; Huq, Ashfia; Jalarvo, Niina; Daemen, Luke L.; Neilson, James R.

doi:10.1021/acs.chemmater.7b04017

Title: Orientational Glass Formation in Substituted Hybrid Perovskites

Journal Article · Tue Nov 07 00:00:00 EST 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.7b04017· OSTI ID:1410797

^[1]; Maughan, Annalise E. ^[1]; Cheng, Yongqiang ^[2]; Huq, Ashfia ^[2];

^[3]; Daemen, Luke L. ^[2];

^[1]

Colorado State Univ., Fort Collins, CO (United States). Dept. of Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) outstation Juelich Centre for Neutron Science (JCNS), Forschungszentrum Juelich GmbH

Hybrid organic–inorganic perovskites have gained notoriety in the photovoltaic community for their composition-tunable band gaps and long-lived electronic excited states, which are known to be related to the crystalline phase. While it is known that the inorganic and organic components are coupled through structural phase transitions, it remains unclear as to what role each plays in directing the structure of hybrid perovskites such as methylammonium lead halides (CH3NH3PbX3). Here, we present crystallographic and spectroscopic data for the series (CH3NH3)1–xCsxPbBr3. CH3NH3PbBr3 behaves as a plastic crystal in the high temperature cubic phase, and substitution of CH3NH3+ with Cs+ leads to the formation of an orientational glass. While the organic molecule exhibits slow, glassy reorientational dynamics, the inorganic framework continues to undergo crystallographic phase transitions. These crystallographic transitions occur in the absence of thermodynamic signatures in the specific heat from molecular orientation transitions, which suggests that the phase transitions result from underlying instabilities intrinsic to the inorganic lattice. However, these transitions are not decoupled from the reorientations of the organic molecule, as indicated by inelastic and quasielastic neutron scattering. Observation of a reentrant phase transition in (CH3NH3)0.8Cs0.2PbBr3 permits the resolution of these complex behaviors within the context of strain mediated interactions. Together, these results provide critical insight into the coupled phase behavior and dynamics in hybrid perovskites.

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Research Organization:: Colorado State Univ., Fort Collins, CO (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: SC0016083; AC02-06CH11357; AC05-00OR22725

OSTI ID:: 1410797

Alternate ID(s):: OSTI ID: 1440822

Journal Information:: Chemistry of Materials, Vol. 29, Issue 23; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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