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 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.
- Authors:
-
- 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 Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- 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. https://doi.org/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. https://doi.org/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 = {Tue Aug 28 00:00:00 EDT 2018},
month = {Tue Aug 28 00:00:00 EDT 2018}
}
Web of Science
Works referenced in this record:
2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications
journal, June 2015
- Cao, Duyen H.; Stoumpos, Constantinos C.; Farha, Omar K.
- Journal of the American Chemical Society, Vol. 137, Issue 24
A Layered Hybrid Perovskite Solar-Cell Absorber with Enhanced Moisture Stability
journal, September 2014
- Smith, Ian C.; Hoke, Eric T.; Solis-Ibarra, Diego
- Angewandte Chemie International Edition, Vol. 53, Issue 42
Conjugated Organic Cations to Improve the Optoelectronic Properties of 2D/3D Perovskites
journal, August 2017
- Rodríguez-Romero, Jesús; Hames, Bruno Clasen; Mora-Seró, Iván
- ACS Energy Letters, Vol. 2, Issue 9
Low-Dimensional Organometal Halide Perovskites
journal, November 2017
- Lin, Haoran; Zhou, Chenkun; Tian, Yu
- ACS Energy Letters, Vol. 3, Issue 1
Charge-Carrier Dynamics and Crystalline Texture of Layered Ruddlesden–Popper Hybrid Lead Iodide Perovskite Thin Films
journal, January 2018
- Venkatesan, Naveen R.; Labram, John G.; Chabinyc, Michael L.
- ACS Energy Letters, Vol. 3, Issue 2
Rashba and Dresselhaus Couplings in Halide Perovskites: Accomplishments and Opportunities for Spintronics and Spin–Orbitronics
journal, July 2017
- Kepenekian, Mikaël; Even, Jacky
- The Journal of Physical Chemistry Letters, Vol. 8, Issue 14
Large polarization-dependent exciton optical Stark effect in lead iodide perovskites
journal, August 2016
- Yang, Ye; Yang, Mengjin; Zhu, Kai
- Nature Communications, Vol. 7, 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
Optical spintronics in organic-inorganic perovskite photovoltaics
journal, April 2016
- Li, Junwen; Haney, Paul M.
- Physical Review B, Vol. 93, Issue 15
Excitonic Effects in Methylammonium Lead Halide Perovskites
journal, May 2018
- Chen, Xihan; Lu, Haipeng; Yang, Ye
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 10
Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies
journal, July 2017
- Zhai, Yaxin; Baniya, Sangita; Zhang, Chuang
- Science Advances, Vol. 3, Issue 7
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
Low surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal
journal, August 2015
- Yang, Ye; Yan, Yong; Yang, Mengjin
- Nature Communications, Vol. 6, Issue 1
Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors
journal, April 2016
- Stoumpos, Constantinos C.; Cao, Duyen H.; Clark, Daniel J.
- Chemistry of Materials, Vol. 28, Issue 8, p. 2852-2867
Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites
journal, March 2017
- Blancon, J. -C.; Tsai, H.; Nie, W.
- Science, Vol. 355, Issue 6331
Ultralow Self-Doping in Two-dimensional Hybrid Perovskite Single Crystals
journal, June 2017
- Peng, Wei; Yin, Jun; Ho, Kang-Ting
- Nano Letters, Vol. 17, Issue 8
How Surface Potential Determines the Kinetics of the First Hole Transfer of Photocatalytic Water Oxidation
journal, July 2014
- Waegele, Matthias M.; Chen, Xihan; Herlihy, David M.
- Journal of the American Chemical Society, Vol. 136, Issue 30
The Formation Time of Ti–O • and Ti–O • –Ti Radicals at the n-SrTiO 3 /Aqueous Interface during Photocatalytic Water Oxidation
journal, December 2016
- Chen, Xihan; Choing, Stephanie N.; Aschaffenburg, Daniel J.
- Journal of the American Chemical Society, Vol. 139, Issue 5
Observation of a hot-phonon bottleneck in lead-iodide perovskites
journal, October 2015
- Yang, Ye; Ostrowski, David P.; France, Ryan M.
- Nature Photonics, Vol. 10, Issue 1
Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films
journal, January 2017
- Yang, Ye; Yang, Mengjin; Moore, David T.
- Nature Energy, Vol. 2, Issue 2
Comparison of Recombination Dynamics in CH 3 NH 3 PbBr 3 and CH 3 NH 3 PbI 3 Perovskite Films: Influence of Exciton Binding Energy
journal, November 2015
- Yang, Ye; Yang, Mengjin; Li, Zhen
- The Journal of Physical Chemistry Letters, Vol. 6, Issue 23
Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites
journal, November 2017
- Gélvez-Rueda, María C.; Hutter, Eline M.; Cao, Duyen H.
- The Journal of Physical Chemistry C, Vol. 121, Issue 47
Image charge effect on two-dimensional excitons in an inorganic-organic quantum-well crystal
journal, January 2005
- Tanaka, Kenichiro; Takahashi, Takayuki; Kondo, Takashi
- Physical Review B, Vol. 71, Issue 4
Excitons in ultrathin organic-inorganic perovskite crystals
journal, July 2015
- Yaffe, Omer; Chernikov, Alexey; Norman, Zachariah M.
- Physical Review B, Vol. 92, Issue 4
The influence of the Rashba effect
journal, April 2018
- Stranks, Samuel D.; Plochocka, Paulina
- Nature Materials, Vol. 17, Issue 5
Semiconductors with a loop of extrema
journal, May 2015
- Rashba, E. I.
- Journal of Electron Spectroscopy and Related Phenomena, Vol. 201
Spintronics: Fundamentals and applications
journal, April 2004
- Žutić, Igor; Fabian, Jaroslav; Das Sarma, S.
- Reviews of Modern Physics, Vol. 76, Issue 2
Highly Spin-Polarized Carrier Dynamics and Ultralarge Photoinduced Magnetization in CH 3 NH 3 PbI 3 Perovskite Thin Films
journal, February 2015
- Giovanni, David; Ma, Hong; Chua, Julianto
- Nano Letters, Vol. 15, Issue 3
Electron–Phonon Scattering in Atomically Thin 2D Perovskites
journal, October 2016
- Guo, Zhi; Wu, Xiaoxi; Zhu, Tong
- ACS Nano, Vol. 10, Issue 11
Phonon Mode Transformation Across the Orthohombic–Tetragonal Phase Transition in a Lead Iodide Perovskite CH 3 NH 3 PbI 3 : A Terahertz Time-Domain Spectroscopy Approach
journal, December 2015
- La-o-vorakiat, Chan; Xia, Huanxin; Kadro, Jeannette
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 1
Electron–phonon coupling in hybrid lead halide perovskites
journal, May 2016
- Wright, Adam D.; Verdi, Carla; Milot, Rebecca L.
- Nature Communications, Vol. 7, Issue 1
Optical phonons in methylammonium lead halide perovskites and implications for charge transport
journal, January 2016
- Sendner, Michael; Nayak, Pabitra K.; Egger, David A.
- Materials Horizons, Vol. 3, Issue 6
Lattice dynamics and vibrational spectra of the orthorhombic, tetragonal, and cubic phases of methylammonium lead iodide
journal, October 2015
- Brivio, Federico; Frost, Jarvist M.; Skelton, Jonathan M.
- Physical Review B, Vol. 92, Issue 14
Giant anharmonic phonon scattering in PbTe
journal, June 2011
- Delaire, O.; Ma, J.; Marty, K.
- Nature Materials, Vol. 10, Issue 8, p. 614-619
Phonon broadening from supercell lattice dynamics: Random and correlated disorder: Phonon broadening from supercell lattice dynamics
journal, November 2016
- Overy, Alistair R.; Simonov, Arkadiy; Chater, Philip A.
- physica status solidi (b), Vol. 254, Issue 4
Room‐temperature electron spin dynamics in GaAs/AlGaAs quantum wells
journal, February 1996
- Tackeuchi, Atsushi; Nishikawa, Yuji; Wada, Osamu
- Applied Physics Letters, Vol. 68, Issue 6
Electron spin relaxation in InGaAs/InP multiple-quantum wells
journal, March 1997
- Tackeuchi, Atsushi; Wada, Osamu; Nishikawa, Yuji
- Applied Physics Letters, Vol. 70, Issue 9
Works referencing / citing this record:
Enhanced Charge Transport by Incorporating Formamidinium and Cesium Cations into Two‐Dimensional Perovskite Solar Cells
journal, July 2019
- Gao, Liguo; Zhang, Fei; Chen, Xihan
- Angewandte Chemie, Vol. 131, Issue 34
Upconverted excitonic photoluminescence from a two-dimensional lead-halide perovskite
journal, December 2019
- Yamada, Takumi; Aharen, Tomoko; Kanemitsu, Yoshihiko
- The Journal of Chemical Physics, Vol. 151, Issue 23
Improving Charge Transport via Intermediate‐Controlled Crystal Growth in 2D Perovskite Solar Cells
journal, April 2019
- Gao, Liguo; Zhang, Fei; Xiao, Chuanxiao
- Advanced Functional Materials, Vol. 29, Issue 47
Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells
journal, January 2020
- Liu, Xiaojie; Chanana, Ashish; Huynh, Uyen
- Nature Communications, Vol. 11, Issue 1
Spin-dependent charge transport through 2D chiral hybrid lead-iodide perovskites
journal, December 2019
- Lu, Haipeng; Wang, Jingying; Xiao, Chuanxiao
- Science Advances, Vol. 5, Issue 12
Long-lived charge separation in two-dimensional ligand-perovskite heterostructures
journal, January 2020
- Deng, Shibin; Snaider, Jordan M.; Gao, Yao
- The Journal of Chemical Physics, Vol. 152, Issue 4
Ruddlesden–Popper Perovskites: Synthesis and Optical Properties for Optoelectronic Applications
journal, October 2019
- Gao, Xupeng; Zhang, Xiangtong; Yin, Wenxu
- Advanced Science, Vol. 6, Issue 22
Long-range exciton transport and slow annihilation in two-dimensional hybrid perovskites
journal, January 2020
- Deng, Shibin; Shi, Enzheng; Yuan, Long
- Nature Communications, Vol. 11, Issue 1
Enhanced Charge Transport by Incorporating Formamidinium and Cesium Cations into Two-Dimensional Perovskite Solar Cells
journal, July 2019
- Gao, Liguo; Zhang, Fei; Chen, Xihan
- Angewandte Chemie International Edition, Vol. 58, Issue 34
Biexciton Auger Recombination Differs in Hybrid and Inorganic Halide Perovskite Quantum Dots
journal, December 2017
- Eperon, Giles E.; Jedlicka, Erin; Ginger, David S.
- The Journal of Physical Chemistry Letters, Vol. 9, Issue 1
Incorporating Large A Cations into Lead Iodide Perovskite Cages: Relaxed Goldschmidt Tolerance Factor and Impact on Exciton–Phonon Interaction
journal, July 2019
- Fu, Yongping; Hautzinger, Matthew P.; Luo, Ziyu
- ACS Central Science, Vol. 5, Issue 8