Halide Mixing Inhibits Exciton Transport in Two-dimensional Perovskites Despite Phase Purity.

Autor: Seitz M; Condensed Matter Physics Center (IFIMAC), Autonomous University of Madrid, 28049 Madrid, Spain.; Department of Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain.; Rowland Institute at Harvard University, Cambridge, Massachusetts 02142, United States.; Department of Electrical Engineering, Stanford University, Stanford, California 94305, United States., Meléndez M; Department of Theoretical Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain., York P; Department of Chemistry, Mississippi State University, Mississippi State, Mississippi 39762, United States., Kurtz DA; Rowland Institute at Harvard University, Cambridge, Massachusetts 02142, United States., Magdaleno AJ; Condensed Matter Physics Center (IFIMAC), Autonomous University of Madrid, 28049 Madrid, Spain.; Department of Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain., Alcázar-Cano N; Condensed Matter Physics Center (IFIMAC), Autonomous University of Madrid, 28049 Madrid, Spain.; Department of Theoretical Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain., Kshirsagar AS; Department of Chemistry, Mississippi State University, Mississippi State, Mississippi 39762, United States., Gangishetty MK; Rowland Institute at Harvard University, Cambridge, Massachusetts 02142, United States.; Department of Chemistry, Mississippi State University, Mississippi State, Mississippi 39762, United States., Delgado-Buscalioni R; Condensed Matter Physics Center (IFIMAC), Autonomous University of Madrid, 28049 Madrid, Spain.; Department of Theoretical Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain., Congreve DN; Rowland Institute at Harvard University, Cambridge, Massachusetts 02142, United States.; Department of Electrical Engineering, Stanford University, Stanford, California 94305, United States., Prins F; Condensed Matter Physics Center (IFIMAC), Autonomous University of Madrid, 28049 Madrid, Spain.; Department of Condensed Matter Physics, Autonomous University of Madrid, 28049 Madrid, Spain.
Jazyk: angličtina
Zdroj: ACS energy letters [ACS Energy Lett] 2022 Jan 14; Vol. 7 (1), pp. 358-365. Date of Electronic Publication: 2021 Dec 22.
DOI: 10.1021/acsenergylett.1c02403
Abstrakt: Halide mixing is one of the most powerful techniques to tune the optical bandgap of metal-halide perovskites. However, halide mixing has commonly been observed to result in phase segregation, which reduces excited-state transport and limits device performance. While the current emphasis lies on the development of strategies to prevent phase segregation, it remains unclear how halide mixing may affect excited-state transport even if phase purity is maintained. Here, we study exciton transport in phase pure mixed-halide 2D perovskites of (PEA) 2 Pb(I 1- x Br x ) 4 . Using transient photoluminescence microscopy, we show that, despite phase purity, halide mixing inhibits exciton transport. We find a significant reduction even for relatively low alloying concentrations. By performing Brownian dynamics simulations, we are able to reproduce our experimental results and attribute the decrease in diffusivity to the energetically disordered potential landscape that arises due to the intrinsic random distribution of alloying sites.
Competing Interests: The authors declare no competing financial interest.
(© 2021 The Authors. Published by American Chemical Society.)
Databáze: MEDLINE
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