Understanding the Role of Cesium on Chemical Complexity in Methylammonium-Free Metal Halide Perovskites

Yang, Jonghee; LaFollette, Diana K.; Lawrie, Benjamin J.; Ievlev, Anton V.; Liu, Yongtao; Kelley, Kyle P.; Kalinin, Sergei V.; Correa‐Baena, Juan‐Pablo; Ahmadi, Mahshid

doi:10.1002/aenm.202202880

Understanding the Role of Cesium on Chemical Complexity in Methylammonium-Free Metal Halide Perovskites

Journal Article · Fri Dec 16 00:00:00 EST 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202202880· OSTI ID:1961963

^[1]; LaFollette, Diana K. ^[2]; ^[3]; ^[3]; ^[3]; ^[3]; Kalinin, Sergei V. ^[1]; Correa‐Baena, Juan‐Pablo ^[2]; ^[1]

Univ. of Tennessee, Knoxville, TN (United States). Department of Materials Science and Engineering, Institute for Advanced Materials and Manufacturing
Georgia Institute of Technology, Atlanta, GA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Mixed cesium- and formamidinium-based metal halide perovskites (MHPs) are emerging as ideal photovoltaic materials due to their promising performance and improved stability. While theoretical predictions suggest that a larger composition ratio of Cs (≈30%) aids the formation of a pure photoactive α-phase, high photovoltaic performances can only be realized in MHPs with moderate Cs ratios. In fact, elemental mixing in a solution can result in chemical complexities with non-equilibrium phases, causing chemical inhomogeneities localized in the MHPs that are not traceable with global device-level measurements. Thus, the chemical origin of the complexities and understanding of their effect on stability and functionality remain elusive. Herein, through spatially resolved analyses, the fate of local chemical structures, particularly the evolution pathway of non-equilibrium phases and the resulting local inhomogeneities in MHPs is comprehensively explored. It is illustrated that Cs-rich MHPs have substantial local inhomogeneities at the initial crystallization step, which do not fully convert to the α-phase and thereby compromise the optoelectronic performance of the materials. These fundamental observations allow the authors to draw a complete chemical landscape of MHPs including nanoscale chemical mechanisms, providing indispensable insights into the realization of a functional materials platform.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: Center for Nanophase Materials Sciences (CNMS); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1961963

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: NA Vol. NA; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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