Understanding size dependence of phase stability and band gap in CsPbI3 perovskite nanocrystals

Yang, Ruo Xi; Tan, Liang Z.

doi:10.1063/1.5128016

Understanding size dependence of phase stability and band gap in CsPbI₃ perovskite nanocrystals

Journal Article · Wed Jan 15 23:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.5128016· OSTI ID:1604722

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Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Inorganic halide perovskites CsPbX₃ (X = Cl, Br, I) have been widely studied as colloidal quantum dots for their excellent optoelectronic properties. Not only is the long-term stability of these materials improved via nanostructuring, their optical bandgaps are also tunable by the nanocrystal (NC) size. However, theoretical understanding of the impact of the NC size on the phase stability and bandgap is still lacking. In this work, the relative phase stability of CsPbI₃ as a function of the crystal size and the chemical potential is investigated by density functional theory. The optically active phases (α- and γ-phase) are found to be thermodynamically stabilized against the yellow δ-phase by reducing the size of the NC below 5.6 nm in a CsI-rich environment. We developed a more accurate quantum confinement model to predict the change in bandgaps at the sub-10 nm regime by including a finite-well effect. Finally, these predictions have important implications for synthesizing ever more stable perovskite NCs and bandgap engineering.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1604722

Alternate ID(s):: OSTI ID: 1591973

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 3 Vol. 152; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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