The past six years have witnessed the rapid growth of interest in Dion–Jacobson (DJ) phase two-dimensional (2D) hybrid halide perovskites as optoelectronic materials with considerable intrinsic stability. The precise relationships between structural variations and the resulting charge carrier dynamics at finite temperature in these materials are keys to practical applications and are not yet completely understood. Here, we study 3-(aminomethyl) piperidinium (3AMP) and 4-(aminomethyl) piperidinium (4AMP) spacer cation-based lead iodide DJ phase systems and find these spacer cations to have a profound impact on the structural dynamics. Particularly, large conformational dynamics of the 3AMP-based perovskite compared to that of the 4AMP at room temperature leads to pronounced state energy fluctuation near band edges and further results in a shorter quantum coherence. The faster quantum decoherence of the 3AMP spacer-based perovskite underpins a longer nonradiative lifetime, offering insight into its superior performance as an optoelectronic material. This work sheds light on the relationship between structural fluctuations and charge carrier dynamics that can help in designing 2D perovskites with superior photophysical properties.
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15 November 2021
Research Article|
November 16 2021
Nonadiabatic molecular dynamics analysis of hybrid Dion–Jacobson 2D leads iodide perovskites
Ying Wang
;
Ying Wang
1
Department of Chemistry, University of Southern California
, Los Angeles, California 90089, USA
2
Theoretical Physics and Chemistry of Materials, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
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Laurent Pedesseau
;
Laurent Pedesseau
3
Univ Rennes, INSA Rennes, CNRS, Institut FOTON, UMR 6082
, Rennes F-35000, France
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Claudine Katan
;
Claudine Katan
4
Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes), UMR 6226
, Rennes F-35000, France
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Jacky Even
;
Jacky Even
3
Univ Rennes, INSA Rennes, CNRS, Institut FOTON, UMR 6082
, Rennes F-35000, France
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Oleg V. Prezhdo
;
Oleg V. Prezhdo
1
Department of Chemistry, University of Southern California
, Los Angeles, California 90089, USA
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Sergei Tretiak
;
Sergei Tretiak
2
Theoretical Physics and Chemistry of Materials, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
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Dibyajyoti Ghosh
;
Dibyajyoti Ghosh
a)
2
Theoretical Physics and Chemistry of Materials, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
5
Center for Nonlinear Studies, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
6
Department of Materials Science and Engineering and Department of Chemistry, Indian Institute of Technology, Delhi
, New Delhi 110016, India
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Amanda J. Neukirch
Amanda J. Neukirch
a)
2
Theoretical Physics and Chemistry of Materials, Los Alamos National Laboratory
, Los Alamos, New Mexico 87545, USA
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Note: This paper is part of the APL Special Collection on New Solution-processed Perovskites and Perovskite-inspired Optoelectronic Materials and Devices.
Appl. Phys. Lett. 119, 201102 (2021)
Article history
Received:
August 08 2021
Accepted:
November 02 2021
Citation
Ying Wang, Laurent Pedesseau, Claudine Katan, Jacky Even, Oleg V. Prezhdo, Sergei Tretiak, Dibyajyoti Ghosh, Amanda J. Neukirch; Nonadiabatic molecular dynamics analysis of hybrid Dion–Jacobson 2D leads iodide perovskites. Appl. Phys. Lett. 15 November 2021; 119 (20): 201102. https://doi.org/10.1063/5.0066087
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