Light-Induced Structural Dynamics and Charge Transport in Layered Halide Perovskite Thin Films

Hsinhan Tsai; Dibyajyoti Ghosh; Eli Kinigstein; Bogdan Dryzhakov; Honora Driscoll; Magdalena Owczarek; Bin Hu; Xiaoyi Zhang; Sergei Tretiak; Wanyi Nie

doi:10.1021/acs.nanolett.2c03403

Light-Induced Structural Dynamics and Charge Transport in Layered Halide Perovskite Thin Films

Hsinhan Tsai, Dibyajyoti Ghosh, Eli Kinigstein, Bogdan Dryzhakov, Honora Driscoll, Magdalena Owczarek, Bin Hu, Xiaoyi Zhang, Sergei Tretiak, Wanyi Nie

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

The dynamic nature of the metal halide perovskite lattice upon photoexcitation plays a vital role in their properties. Here we report an observation of light-induced structure dynamics in quasi-2D Ruddlesden-Popper phase perovskite thin films and its impact on the carrier transport properties. By a time-resolved X-ray scattering technique, we observe a rapid lattice expansion upon photoexcitation, followed by a slow relaxation over the course of 100 ns in the dark. Theoretical modeling suggests that the expansion originates from the lattice’s thermal fluctuations caused by photon energy deposition. Power dependent optical spectroscopy and photoconductivity indicate that high laser powers triggered a strong local structural disorder, which increased the charge dissociation activation energy that results in localized transport. Our study investigates the impact of laser energy deposition on the lattices and the subsequent carrier transport properties, that are relevant to device operations.

Original language	English
Pages (from-to)	429-436
Number of pages	8
Journal	Nano Letters
Volume	23
Issue number	2
DOIs	https://doi.org/10.1021/acs.nanolett.2c03403
State	Published - Jan 25 2023
Externally published	Yes

Funding

W.N. acknowledges the support from the Laboratory Directed Research Directions program (Directors Quantum Initiative project and ER project) at Los Alamos National Laboratory (LANL). W.N. and H.D. acknowledge the financial support from the Mission Foundation Research project at LANL. H.T. acknowledges the financial support from a J. Robert Oppenheimer (JRO) Distinguished Postdoc Fellowship at LANL. This work was performed, in part, at the Center for Integrated Nanotechnologies, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science. Los Alamos National Laboratory, an affirmative action equal opportunity employer, is managed by Triad National Security, LLC for the U.S. Department of Energy’s NNSA, under contract 89233218CNA000001. Part of this research used sectors 8-ID-E and 11-ID-D of the Advanced Photon Source, an Office of Science user facility supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357.

Keywords

2D perovskites
charge transport
structural dynamics
thin film

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10.1021/acs.nanolett.2c03403

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title = "Light-Induced Structural Dynamics and Charge Transport in Layered Halide Perovskite Thin Films",

abstract = "The dynamic nature of the metal halide perovskite lattice upon photoexcitation plays a vital role in their properties. Here we report an observation of light-induced structure dynamics in quasi-2D Ruddlesden-Popper phase perovskite thin films and its impact on the carrier transport properties. By a time-resolved X-ray scattering technique, we observe a rapid lattice expansion upon photoexcitation, followed by a slow relaxation over the course of 100 ns in the dark. Theoretical modeling suggests that the expansion originates from the lattice{\textquoteright}s thermal fluctuations caused by photon energy deposition. Power dependent optical spectroscopy and photoconductivity indicate that high laser powers triggered a strong local structural disorder, which increased the charge dissociation activation energy that results in localized transport. Our study investigates the impact of laser energy deposition on the lattices and the subsequent carrier transport properties, that are relevant to device operations.",

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AU - Tsai, Hsinhan

AU - Ghosh, Dibyajyoti

AU - Kinigstein, Eli

AU - Dryzhakov, Bogdan

AU - Driscoll, Honora

AU - Owczarek, Magdalena

AU - Hu, Bin

AU - Zhang, Xiaoyi

AU - Tretiak, Sergei

AU - Nie, Wanyi

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N2 - The dynamic nature of the metal halide perovskite lattice upon photoexcitation plays a vital role in their properties. Here we report an observation of light-induced structure dynamics in quasi-2D Ruddlesden-Popper phase perovskite thin films and its impact on the carrier transport properties. By a time-resolved X-ray scattering technique, we observe a rapid lattice expansion upon photoexcitation, followed by a slow relaxation over the course of 100 ns in the dark. Theoretical modeling suggests that the expansion originates from the lattice’s thermal fluctuations caused by photon energy deposition. Power dependent optical spectroscopy and photoconductivity indicate that high laser powers triggered a strong local structural disorder, which increased the charge dissociation activation energy that results in localized transport. Our study investigates the impact of laser energy deposition on the lattices and the subsequent carrier transport properties, that are relevant to device operations.

AB - The dynamic nature of the metal halide perovskite lattice upon photoexcitation plays a vital role in their properties. Here we report an observation of light-induced structure dynamics in quasi-2D Ruddlesden-Popper phase perovskite thin films and its impact on the carrier transport properties. By a time-resolved X-ray scattering technique, we observe a rapid lattice expansion upon photoexcitation, followed by a slow relaxation over the course of 100 ns in the dark. Theoretical modeling suggests that the expansion originates from the lattice’s thermal fluctuations caused by photon energy deposition. Power dependent optical spectroscopy and photoconductivity indicate that high laser powers triggered a strong local structural disorder, which increased the charge dissociation activation energy that results in localized transport. Our study investigates the impact of laser energy deposition on the lattices and the subsequent carrier transport properties, that are relevant to device operations.

KW - 2D perovskites

KW - charge transport

KW - structural dynamics

KW - thin film

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Light-Induced Structural Dynamics and Charge Transport in Layered Halide Perovskite Thin Films

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