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Title: Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals

Abstract

In this paper, we report the charge carrier recombination rate and spin coherence lifetimes in single crystals of two-dimensional (2D) Ruddlesden–Popper perovskites PEA 2PbI 4·(MAPbI 3) n-1 (PEA, phenethylammonium; MA, methylammonium; n = 1, 2, 3, 4). Layer thickness-dependent charge carrier recombination rates are observed, with the fastest rates for n = 1 because of the large exciton binding energy, and the slowest rates are observed for n = 2. Room-temperature spin coherence times also show a nonmonotonic layer thickness dependence with an increasing spin coherence lifetime with increasing layer thickness from n = 1 to n = 4, followed by a decrease in lifetime from n = 4 to ∞. The longest coherence lifetime of ~7 ps is observed in the n = 4 sample. Our results are consistent with two contributions: Rashba splitting increases the spin coherence lifetime going from the n = ∞ to the layered systems, while phonon scattering, which increases for smaller layers, decreases the spin coherence lifetime. Finally, the interplay between these two factors contributes to the layer thickness dependence.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemical and Nano Science Center
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Hybrid Organic-Inorganic Semiconductors for Energy (CHOISE); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1471290
Report Number(s):
NREL/JA-5900-71748
Journal ID: ISSN 2380-8195
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Chen, Xihan, Lu, Haipeng, Li, Zhen, Zhai, Yaxin, Ndione, Paul F., Berry, Joseph J., Zhu, Kai, Yang, Ye, and Beard, Matthew C. Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals. United States: N. p., 2018. Web. doi:10.1021/acsenergylett.8b01315.
Chen, Xihan, Lu, Haipeng, Li, Zhen, Zhai, Yaxin, Ndione, Paul F., Berry, Joseph J., Zhu, Kai, Yang, Ye, & Beard, Matthew C. Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals. United States. doi:10.1021/acsenergylett.8b01315.
Chen, Xihan, Lu, Haipeng, Li, Zhen, Zhai, Yaxin, Ndione, Paul F., Berry, Joseph J., Zhu, Kai, Yang, Ye, and Beard, Matthew C. Tue . "Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals". United States. doi:10.1021/acsenergylett.8b01315. https://www.osti.gov/servlets/purl/1471290.
@article{osti_1471290,
title = {Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals},
author = {Chen, Xihan and Lu, Haipeng and Li, Zhen and Zhai, Yaxin and Ndione, Paul F. and Berry, Joseph J. and Zhu, Kai and Yang, Ye and Beard, Matthew C.},
abstractNote = {In this paper, we report the charge carrier recombination rate and spin coherence lifetimes in single crystals of two-dimensional (2D) Ruddlesden–Popper perovskites PEA2PbI4·(MAPbI3)n-1 (PEA, phenethylammonium; MA, methylammonium; n = 1, 2, 3, 4). Layer thickness-dependent charge carrier recombination rates are observed, with the fastest rates for n = 1 because of the large exciton binding energy, and the slowest rates are observed for n = 2. Room-temperature spin coherence times also show a nonmonotonic layer thickness dependence with an increasing spin coherence lifetime with increasing layer thickness from n = 1 to n = 4, followed by a decrease in lifetime from n = 4 to ∞. The longest coherence lifetime of ~7 ps is observed in the n = 4 sample. Our results are consistent with two contributions: Rashba splitting increases the spin coherence lifetime going from the n = ∞ to the layered systems, while phonon scattering, which increases for smaller layers, decreases the spin coherence lifetime. Finally, the interplay between these two factors contributes to the layer thickness dependence.},
doi = {10.1021/acsenergylett.8b01315},
journal = {ACS Energy Letters},
number = 9,
volume = 3,
place = {United States},
year = {2018},
month = {8}
}

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