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:
-
- University of Utah, Salt Lake City, UT (United States)
- University of North Carolina, Chapel Hill, NC (United States)
- 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}
}
Works referenced in this record:
Rashba and Dresselhaus Effects in Hybrid Organic–Inorganic Perovskites: From Basics to Devices
journal, September 2015
- Kepenekian, Mikaël; Robles, Roberto; Katan, Claudine
- ACS Nano, Vol. 9, Issue 12
Ligand assisted growth of perovskite single crystals with low defect density
journal, March 2021
- Liu, Ye; Zheng, Xiaopeng; Fang, Yanjun
- Nature Communications, Vol. 12, Issue 1
Conductivity Tuning via Doping with Electron Donating and Withdrawing Molecules in Perovskite CsPbI 3 Nanocrystal Films
journal, May 2019
- Gaulding, E. Ashley; Hao, Ji; Kang, Hyun Suk
- Advanced Materials, Vol. 31, Issue 27
Coherent spin dynamics of electrons and holes in CsPbBr3 perovskite crystals
journal, February 2019
- Belykh, Vasilii V.; Yakovlev, Dmitri R.; Glazov, Mikhail M.
- Nature Communications, Vol. 10, Issue 1
Quantification of re-absorption and re-emission processes to determine photon recycling efficiency in perovskite single crystals
journal, February 2017
- Fang, Yanjun; Wei, Haotong; Dong, Qingfeng
- Nature Communications, Vol. 8, Issue 1
Resonant Spin Amplification in -Type GaAs
journal, May 1998
- Kikkawa, J. M.; Awschalom, D. D.
- Physical Review Letters, Vol. 80, Issue 19
Spin coherence and formation dynamics of charged excitons in quantum wells
journal, July 2000
- Vanelle, E.; Paillard, M.; Marie, X.
- Physical Review B, Vol. 62, Issue 4
Interface engineering of highly efficient perovskite solar cells
journal, July 2014
- Zhou, H.; Chen, Q.; Li, G.
- Science, Vol. 345, Issue 6196
High-performance photovoltaic perovskite layers fabricated through intramolecular exchange
journal, May 2015
- Yang, W. S.; Noh, J. H.; Jeon, N. J.
- Science, Vol. 348, Issue 6240
Magnetic field effects in hybrid perovskite devices
journal, March 2015
- Zhang, C.; Sun, D.; Sheng, C-X.
- Nature Physics, Vol. 11, Issue 5
Bright triplet excitons in caesium lead halide perovskites
journal, January 2018
- Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian
- Nature, Vol. 553, Issue 7687
Quantum Theory of Cyclotron Resonance in Semiconductors: General Theory
journal, May 1956
- Luttinger, J. M.
- Physical Review, Vol. 102, Issue 4
Overcoming the electroluminescence efficiency limitations of perovskite light-emitting diodes
journal, December 2015
- Cho, H.; Jeong, S. -H.; Park, M. -H.
- Science, Vol. 350, Issue 6265
The ground exciton state of formamidinium lead bromide perovskite nanocrystals is a singlet dark state
journal, May 2019
- Tamarat, Philippe; Bodnarchuk, Maryna I.; Trebbia, Jean-Baptiste
- Nature Materials, Vol. 18, Issue 7
Free Carriers versus Excitons in CH 3 NH 3 PbI 3 Perovskite Thin Films at Low Temperatures: Charge Transfer from the Orthorhombic Phase to the Tetragonal Phase
journal, June 2016
- Phuong, Le Quang; Yamada, Yasuhiro; Nagai, Masaya
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
Exciton Fine Structure in Perovskite Nanocrystals
journal, April 2019
- Sercel, Peter C.; Lyons, John L.; Wickramaratne, Darshana
- Nano Letters, Vol. 19, Issue 6
Bright light-emitting diodes based on organometal halide perovskite
journal, August 2014
- Tan, Zhi-Kuang; Moghaddam, Reza Saberi; Lai, May Ling
- Nature Nanotechnology, Vol. 9, Issue 9
Ambipolar solution-processed hybrid perovskite phototransistors
journal, September 2015
- Li, Feng; Ma, Chun; Wang, Hong
- Nature Communications, Vol. 6, Issue 1
Exciton versus Free Carrier Photogeneration in Organometal Trihalide Perovskites Probed by Broadband Ultrafast Polarization Memory Dynamics
journal, March 2015
- Sheng, ChuanXiang; Zhang, Chuang; Zhai, Yaxin
- Physical Review Letters, Vol. 114, Issue 11
Quasicubic model for metal halide perovskite nanocrystals
journal, December 2019
- Sercel, Peter C.; Lyons, John L.; Bernstein, Noam
- The Journal of Chemical Physics, Vol. 151, Issue 23
Multiband k·p Model for Tetragonal Crystals: Application to Hybrid Halide Perovskite Nanocrystals
journal, January 2020
- Ben Aich, R.; Ben Radhia, S.; Boujdaria, K.
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 3
Fine structure of neutral and charged excitons in self-assembled In(Ga)As/(Al)GaAs quantum dots
journal, May 2002
- Bayer, M.; Ortner, G.; Stern, O.
- Physical Review B, Vol. 65, Issue 19
First-Principles Study of Lead Iodide Perovskite Tetragonal and Orthorhombic Phases for Photovoltaics
journal, August 2014
- Geng, Wei; Zhang, Le; Zhang, Yan-Ning
- The Journal of Physical Chemistry C, Vol. 118, Issue 34
A Note on the Quantum‐Mechanical Perturbation Theory
journal, November 1951
- Löwdin, Per‐Olov
- The Journal of Chemical Physics, Vol. 19, Issue 11
Theory of the Effect of Spin-Orbit Coupling on Magnetic Resonance in Some Semiconductors
journal, October 1954
- Elliott, R. J.
- Physical Review, Vol. 96, Issue 2
Low-temperature solution-processed wavelength-tunable perovskites for lasing
journal, March 2014
- Xing, Guichuan; Mathews, Nripan; Lim, Swee Sien
- Nature Materials, Vol. 13, Issue 5
Resolving spatial and energetic distributions of trap states in metal halide perovskite solar cells
journal, March 2020
- Ni, Zhenyi; Bao, Chunxiong; Liu, Ye
- Science, Vol. 367, Issue 6484
Electron and Hole g -Factors and Spin Dynamics of Negatively Charged Excitons in CdSe/CdS Colloidal Nanoplatelets with Thick Shells
journal, November 2017
- Shornikova, Elena V.; Biadala, Louis; Yakovlev, Dmitri R.
- Nano Letters, Vol. 18, Issue 1
Lead‐Dominated Hyperfine Interaction Impacting the Carrier Spin Dynamics in Halide Perovskites
journal, October 2021
- Kirstein, Erik; Yakovlev, Dmitri R.; Glazov, Mikhail M.
- Advanced Materials, Vol. 34, Issue 1
Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr3 Single Crystal
journal, September 2019
- Baranowski, Michał; Galkowski, Krzysztof; Surrente, Alessandro
- Nano Letters, Vol. 19, Issue 10
Charge carrier recombination channels in the low-temperature phase of organic-inorganic lead halide perovskite thin films
journal, August 2014
- Wehrenfennig, Christian; Liu, Mingzhen; Snaith, Henry J.
- APL Materials, Vol. 2, Issue 8
Electrical spin injection and transport in semiconductor nanowires: challenges, progress and perspectives
journal, January 2015
- Tang, Jianshi; Wang, Kang L.
- Nanoscale, Vol. 7, Issue 10
Trap States in Lead Iodide Perovskites
journal, January 2015
- Wu, Xiaoxi; Trinh, M. Tuan; Niesner, Daniel
- Journal of the American Chemical Society, Vol. 137, Issue 5
Efficient inorganic–organic hybrid heterojunction solar cells containing perovskite compound and polymeric hole conductors
journal, May 2013
- Heo, Jin Hyuck; Im, Sang Hyuk; Noh, Jun Hong
- Nature Photonics, Vol. 7, Issue 6, p. 486-491
Correlated electron–hole plasma in organometal perovskites
journal, September 2014
- Saba, Michele; Cadelano, Michele; Marongiu, Daniela
- Nature Communications, Vol. 5, Issue 1
Narrow Linewidth Excitonic Emission in Organic–Inorganic Lead Iodide Perovskite Single Crystals
journal, November 2016
- Diab, Hiba; Trippé-Allard, Gaëlle; Lédée, Ferdinand
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 24
Excitons versus free charges in organo-lead tri-halide perovskites
journal, April 2014
- D’Innocenzo, Valerio; Grancini, Giulia; Alcocer, Marcelo J. P.
- Nature Communications, Vol. 5, Issue 1
Spin-polarized exciton quantum beating in hybrid organic–inorganic perovskites
journal, May 2017
- Odenthal, Patrick; Talmadge, William; Gundlach, Nathan
- Nature Physics, Vol. 13, Issue 9
Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites
journal, June 2016
- Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita
- Science Advances, Vol. 2, Issue 6
Effective-mass model and magneto-optical properties in hybrid perovskites
journal, June 2016
- Yu, Z. G.
- Scientific Reports, Vol. 6, Issue 1
Efficient planar heterojunction perovskite solar cells by vapour deposition
journal, September 2013
- Liu, Mingzhen; Johnston, Michael B.; Snaith, Henry J.
- Nature, Vol. 501, Issue 7467, p. 395-398
Coherent single-photon emission from colloidal lead halide perovskite quantum dots
journal, February 2019
- Utzat, Hendrik; Sun, Weiwei; Kaplan, Alexander E. K.
- Science, Vol. 363, Issue 6431
Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012
- Lee, M. M.; Teuscher, J.; Miyasaka, T.
- Science, Vol. 338, Issue 6107, p. 643-647
Experimental Evidence of Localized Shallow States in Orthorhombic Phase of CH 3 NH 3 PbI 3 Perovskite Thin Films Revealed by Photocurrent Beat Spectroscopy
journal, January 2016
- Tahara, Hirokazu; Endo, Masaru; Wakamiya, Atsushi
- The Journal of Physical Chemistry C, Vol. 120, Issue 10
Quantum cryptography
journal, March 2002
- Gisin, Nicolas; Ribordy, Grégoire; Tittel, Wolfgang
- Reviews of Modern Physics, Vol. 74, Issue 1
Qualifying composition dependent p and n self-doping in CH 3 NH 3 PbI 3
journal, October 2014
- Wang, Qi; Shao, Yuchuan; Xie, Haipeng
- Applied Physics Letters, Vol. 105, Issue 16
Spin coherence of two-dimensional electron gas in CdTe/(Cd,Mg)Te quantum wells
journal, March 2006
- Zhukov, E. A.; Yakovlev, D. R.; Bayer, M.
- physica status solidi (b), Vol. 243, Issue 4
Importance of Spin–Orbit Coupling in Hybrid Organic/Inorganic Perovskites for Photovoltaic Applications
journal, August 2013
- Even, Jacky; Pedesseau, Laurent; Jancu, Jean-Marc
- The Journal of Physical Chemistry Letters, Vol. 4, Issue 17
Solid-State Physics Perspective on Hybrid Perovskite Semiconductors
journal, April 2015
- Even, Jacky; Pedesseau, Laurent; Katan, Claudine
- The Journal of Physical Chemistry C, Vol. 119, Issue 19
Giant Rashba Splitting in Organic-Inorganic Perovskite
journal, September 2016
- Niesner, Daniel; Wilhelm, Max; Levchuk, Ievgen
- Physical Review Letters, Vol. 117, Issue 12
Spin-optoelectronic devices based on hybrid organic-inorganic trihalide perovskites
journal, January 2019
- Wang, Jingying; Zhang, Chuang; Liu, Haoliang
- Nature Communications, Vol. 10, Issue 1