90007802

open access

Accepted Manuscript

In Situ Exploration of the Structural Transition during Morphology- and Efficiency-Conserving Halide Exchange on a Single Perovskite Nanocrystal

Angewandte Chemie International Edition

60(5)

2548-2553

Wiley‐VCH Verlag

2021-02-01

2022-03-01

Controlled fabrication of semiconductor nanostructures with unique physicochemical properties is vital for future technologies. In this study, transformation from red-emitting metal halide perovskite CH3NH3PbI3 nanocrystals (NCs) to green-emitting CH3NH3PbBr3 NCs was achieved without significant morphological changes and loss of photoluminescence (PL) efficiency via a controlled halide exchange reaction. In situ single-particle PL imaging along with detailed structural and elemental characterizations revealed that sudden cooperative transitions between two light-emitting states via intermediate dark states with >100 s durations during halide exchange originate from two distinct defect-mediated reconstruction processes with different activation energies (0.072 and 0.40 eV), leading to an isokinetic temperature of ca. 314 K, across a solid-state miscibility gap between the I- and Br-rich phases inside a single NC.

single-particle spectroscopy

学術雑誌論文

© 2020 Wiley‐VCH GmbH. This is the peer reviewed version of the following article: [I. Karimata, T. Tachikawa, Angew. Chem. Int. Ed. 2021, 60, 2548-2553.], which has been published in final form at https://doi.org/10.1002/anie.202013386. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. This article may not be enhanced, enriched or otherwise transformed into a derivative work, without express permission from Wiley or by statutory rights under applicable legislation. Copyright notices must not be removed, obscured or modified. The article must be linked to Wiley’s version of record on Wiley Online Library and any embedding, framing or otherwise making available the article or pages thereof by third parties from platforms, services and websites other than Wiley Online Library must be prohibited.