Issue 18, 2020

Charge localization control of electron–hole recombination in multilayer two-dimensional Dion–Jacobson hybrid perovskites

Abstract

Two-dimensional (2D) Dion–Jacobson (DJ) organic–inorganic hybrid halide perovskites hold great potential for optoelectronics and solar cells. Interestingly, experimental excited-state lifetime is longer in (3AMP)(MA)n−1PbnI3n+1 than (4AMP)(MA)n−1PbnI3n+1 (3AMP = 3-(aminomethyl)piperidinium, 4AMP = 4-(aminomethyl)piperidinium, MA = CH3NH3+) regardless of the value of n despite 3AMP having a smaller bandgap. Using ab initio nonadiabatic (NA) molecular dynamics combined with time-domain density functional theory, we focus on the n = 2 perovskite and demonstrate that stronger hydrogen bonding interaction and larger octahedral tilting cause significant delocalization of the hole wave function in (4AMP)(MA)Pb2I7 and accelerates the electron–hole recombination by a factor of 5 compared to (3AMP)(MA)Pb2I7 due to an increased NA coupling. The inorganic component stretching mode and coupled inorganic and organic collective motions accelerate decoherence to sub-4 fs in the two materials. The simulations rationalize the experimentally observed puzzle of excited-state lifetime in the 2D DJ perovskite and suggest a rational way to optimize the performance of perovskite devices.

Graphical abstract: Charge localization control of electron–hole recombination in multilayer two-dimensional Dion–Jacobson hybrid perovskites

Supplementary files

Article information

Article type
Paper
Submitted
18 Feb 2020
Accepted
13 Apr 2020
First published
14 Apr 2020

J. Mater. Chem. A, 2020,8, 9168-9176

Charge localization control of electron–hole recombination in multilayer two-dimensional Dion–Jacobson hybrid perovskites

R. Shi, Z. Zhang, W. Fang and R. Long, J. Mater. Chem. A, 2020, 8, 9168 DOI: 10.1039/D0TA01944E

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