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Title: Transient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal

Abstract

Utilizing the spin degree of freedom of photoexcitations in hybrid organic inorganic perovskites for quantum information science applications has been recently proposed and explored. However, it is still unclear whether the stable photoexcitations in these compounds correspond to excitons, free/trapped electron-hole pairs, or charged exciton complexes such as trions. Here we investigate quantum beating oscillations in the picosecond time-resolved circularly polarized photoinduced reflection of single crystal methyl-ammonium tri-iodine perovskite (MAPbI3) measured at cryogenic temperatures. We observe two quantum beating oscillations (fast and slow) whose frequencies increase linearly with B with slopes that depend on the crystal orientation with respect to the applied magnetic field. We assign the quantum beatings to positive and negative trions whose Landé g-factors are determined by those of the electron and hole, respectively, or by the carriers left behind after trion recombination. These are $$g^{e}_{[001]}$$ = 2.52 and $$g^{e}_{[1\bar10]}$$ = 2.63 for electrons, whereas |$$g^{h}_{[001]}$$| = 0.28 and |$$g^{h}_{[1\bar10]}$$| = 0.57 for holes. The obtained g-values are in excellent agreement with an 8-band K.P calculation for orthorhombic MAPbI3. Using the technique of resonant spin amplification of the quantum beatings we measure a relatively long spin coherence time of ~ 11 (6) nanoseconds for electrons (holes) at 4 K.

Authors:
 [1];  [2];  [1];  [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. University of Utah, Salt Lake City, UT (United States)
  2. University of North Carolina, Chapel Hill, NC (United States)
  3. National Renewable Energy Laboratory (NREL), Golden, CO (United States). Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1904210
Grant/Contract Number:  
SC0014579; AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 13; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; magneto-optics; photonic crystals; optical spectroscopy; spintronics; ultrafast lasers

Citation Formats

Huynh, Uyen N., Liu, Ye, Chanana, Ashish, Khanal, Dipak R., Sercel, Peter C., Huang, Jinsong, and Vardeny, Z. Valy. Transient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal. United States: N. p., 2022. Web. doi:10.1038/s41467-022-29053-6.
Huynh, Uyen N., Liu, Ye, Chanana, Ashish, Khanal, Dipak R., Sercel, Peter C., Huang, Jinsong, & Vardeny, Z. Valy. Transient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal. United States. https://doi.org/10.1038/s41467-022-29053-6
Huynh, Uyen N., Liu, Ye, Chanana, Ashish, Khanal, Dipak R., Sercel, Peter C., Huang, Jinsong, and Vardeny, Z. Valy. Thu . "Transient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal". United States. https://doi.org/10.1038/s41467-022-29053-6. https://www.osti.gov/servlets/purl/1904210.
@article{osti_1904210,
title = {Transient quantum beatings of trions in hybrid organic tri-iodine perovskite single crystal},
author = {Huynh, Uyen N. and Liu, Ye and Chanana, Ashish and Khanal, Dipak R. and Sercel, Peter C. and Huang, Jinsong and Vardeny, Z. Valy},
abstractNote = {Utilizing the spin degree of freedom of photoexcitations in hybrid organic inorganic perovskites for quantum information science applications has been recently proposed and explored. However, it is still unclear whether the stable photoexcitations in these compounds correspond to excitons, free/trapped electron-hole pairs, or charged exciton complexes such as trions. Here we investigate quantum beating oscillations in the picosecond time-resolved circularly polarized photoinduced reflection of single crystal methyl-ammonium tri-iodine perovskite (MAPbI3) measured at cryogenic temperatures. We observe two quantum beating oscillations (fast and slow) whose frequencies increase linearly with B with slopes that depend on the crystal orientation with respect to the applied magnetic field. We assign the quantum beatings to positive and negative trions whose Landé g-factors are determined by those of the electron and hole, respectively, or by the carriers left behind after trion recombination. These are $g^{e}_{[001]}$ = 2.52 and $g^{e}_{[1\bar10]}$ = 2.63 for electrons, whereas |$g^{h}_{[001]}$| = 0.28 and |$g^{h}_{[1\bar10]}$| = 0.57 for holes. The obtained g-values are in excellent agreement with an 8-band K.P calculation for orthorhombic MAPbI3. Using the technique of resonant spin amplification of the quantum beatings we measure a relatively long spin coherence time of ~ 11 (6) nanoseconds for electrons (holes) at 4 K.},
doi = {10.1038/s41467-022-29053-6},
journal = {Nature Communications},
number = 1,
volume = 13,
place = {United States},
year = {Thu Mar 17 00:00:00 EDT 2022},
month = {Thu Mar 17 00:00:00 EDT 2022}
}

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