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

Chen, Xihan; Lu, Haipeng; Li, Zhen; Zhai, Yaxin; Ndione, Paul F.; Berry, Joseph J.; Zhu, Kai; Yang, Ye; Beard, Matthew C.

doi:10.1021/acsenergylett.8b01315

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

Journal Article · Tue Aug 28 00:00:00 EDT 2018 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.8b01315· OSTI ID:1471290

^[1]; ^[1]; ^[1]; Zhai, Yaxin ^[1]; ^[1]; Berry, Joseph J. ^[1]; ^[1]; Yang, Ye ^[1]; ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemical and Nano Science Center

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.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1471290

Report Number(s):: NREL/JA--5900-71748

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 9 Vol. 3; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (37)

A Layered Hybrid Perovskite Solar-Cell Absorber with Enhanced Moisture Stability Smith, Ian C.; Hoke, Eric T.; Solis-Ibarra, Diego Angewandte Chemie International Edition, Vol. 53, Issue 42 https://doi.org/10.1002/anie.201406466	journal	September 2014
Phonon broadening from supercell lattice dynamics: Random and correlated disorder: Phonon broadening from supercell lattice dynamics Overy, Alistair R.; Simonov, Arkadiy; Chater, Philip A. physica status solidi (b), Vol. 254, Issue 4 https://doi.org/10.1002/pssb.201600586	journal	November 2016
Semiconductors with a loop of extrema Rashba, E. I. Journal of Electron Spectroscopy and Related Phenomena, Vol. 201 https://doi.org/10.1016/j.elspec.2014.10.002	journal	May 2015
Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors Stoumpos, Constantinos C.; Cao, Duyen H.; Clark, Daniel J. Chemistry of Materials, Vol. 28, Issue 8, p. 2852-2867 https://doi.org/10.1021/acs.chemmater.6b00847	journal	April 2016
Interconversion between Free Charges and Bound Excitons in 2D Hybrid Lead Halide Perovskites Gélvez-Rueda, María C.; Hutter, Eline M.; Cao, Duyen H. The Journal of Physical Chemistry C, Vol. 121, Issue 47 https://doi.org/10.1021/acs.jpcc.7b10705	journal	November 2017
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 La-o-vorakiat, Chan; Xia, Huanxin; Kadro, Jeannette The Journal of Physical Chemistry Letters, Vol. 7, Issue 1 https://doi.org/10.1021/acs.jpclett.5b02223	journal	December 2015
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 Yang, Ye; Yang, Mengjin; Li, Zhen The Journal of Physical Chemistry Letters, Vol. 6, Issue 23 https://doi.org/10.1021/acs.jpclett.5b02290	journal	November 2015
Rashba and Dresselhaus Couplings in Halide Perovskites: Accomplishments and Opportunities for Spintronics and Spin–Orbitronics Kepenekian, Mikaël; Even, Jacky The Journal of Physical Chemistry Letters, Vol. 8, Issue 14 https://doi.org/10.1021/acs.jpclett.7b01015	journal	July 2017
Excitonic Effects in Methylammonium Lead Halide Perovskites Chen, Xihan; Lu, Haipeng; Yang, Ye The Journal of Physical Chemistry Letters, Vol. 9, Issue 10 https://doi.org/10.1021/acs.jpclett.8b00526	journal	May 2018
Ultralow Self-Doping in Two-dimensional Hybrid Perovskite Single Crystals Peng, Wei; Yin, Jun; Ho, Kang-Ting Nano Letters, Vol. 17, Issue 8 https://doi.org/10.1021/acs.nanolett.7b01475	journal	June 2017
Conjugated Organic Cations to Improve the Optoelectronic Properties of 2D/3D Perovskites Rodríguez-Romero, Jesús; Hames, Bruno Clasen; Mora-Seró, Iván ACS Energy Letters, Vol. 2, Issue 9 https://doi.org/10.1021/acsenergylett.7b00654	journal	August 2017
Low-Dimensional Organometal Halide Perovskites Lin, Haoran; Zhou, Chenkun; Tian, Yu ACS Energy Letters, Vol. 3, Issue 1 https://doi.org/10.1021/acsenergylett.7b00926	journal	November 2017
Charge-Carrier Dynamics and Crystalline Texture of Layered Ruddlesden–Popper Hybrid Lead Iodide Perovskite Thin Films Venkatesan, Naveen R.; Labram, John G.; Chabinyc, Michael L. ACS Energy Letters, Vol. 3, Issue 2 https://doi.org/10.1021/acsenergylett.7b01245	journal	January 2018
Electron–Phonon Scattering in Atomically Thin 2D Perovskites Guo, Zhi; Wu, Xiaoxi; Zhu, Tong ACS Nano, Vol. 10, Issue 11 https://doi.org/10.1021/acsnano.6b04265	journal	October 2016
How Surface Potential Determines the Kinetics of the First Hole Transfer of Photocatalytic Water Oxidation Waegele, Matthias M.; Chen, Xihan; Herlihy, David M. Journal of the American Chemical Society, Vol. 136, Issue 30 https://doi.org/10.1021/ja503603k	journal	July 2014
2D Homologous Perovskites as Light-Absorbing Materials for Solar Cell Applications Cao, Duyen H.; Stoumpos, Constantinos C.; Farha, Omar K. Journal of the American Chemical Society, Vol. 137, Issue 24 https://doi.org/10.1021/jacs.5b03796	journal	June 2015
The Formation Time of Ti–O ^• and Ti–O ^• –Ti Radicals at the n-SrTiO ₃ /Aqueous Interface during Photocatalytic Water Oxidation Chen, Xihan; Choing, Stephanie N.; Aschaffenburg, Daniel J. Journal of the American Chemical Society, Vol. 139, Issue 5 https://doi.org/10.1021/jacs.6b09550	journal	December 2016
Highly Spin-Polarized Carrier Dynamics and Ultralarge Photoinduced Magnetization in CH ₃ NH ₃ PbI ₃ Perovskite Thin Films Giovanni, David; Ma, Hong; Chua, Julianto Nano Letters, Vol. 15, Issue 3 https://doi.org/10.1021/nl5039314	journal	February 2015
Electron–phonon coupling in hybrid lead halide perovskites Wright, Adam D.; Verdi, Carla; Milot, Rebecca L. Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11755	journal	May 2016
Large polarization-dependent exciton optical Stark effect in lead iodide perovskites Yang, Ye; Yang, Mengjin; Zhu, Kai Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms12613	journal	August 2016
Low surface recombination velocity in solution-grown CH3NH3PbBr3 perovskite single crystal Yang, Ye; Yan, Yong; Yang, Mengjin Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms8961	journal	August 2015
Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films Yang, Ye; Yang, Mengjin; Moore, David T. Nature Energy, Vol. 2, Issue 2 https://doi.org/10.1038/nenergy.2016.207	journal	January 2017
Giant anharmonic phonon scattering in PbTe Delaire, O.; Ma, J.; Marty, K. Nature Materials, Vol. 10, Issue 8, p. 614-619 https://doi.org/10.1038/nmat3035	journal	June 2011
Observation of a hot-phonon bottleneck in lead-iodide perovskites Yang, Ye; Ostrowski, David P.; France, Ryan M. Nature Photonics, Vol. 10, Issue 1 https://doi.org/10.1038/nphoton.2015.213	journal	October 2015
Spin-polarized exciton quantum beating in hybrid organic–inorganic perovskites Odenthal, Patrick; Talmadge, William; Gundlach, Nathan Nature Physics, Vol. 13, Issue 9 https://doi.org/10.1038/nphys4145	journal	May 2017
The influence of the Rashba effect Stranks, Samuel D.; Plochocka, Paulina Nature Materials, Vol. 17, Issue 5 https://doi.org/10.1038/s41563-018-0067-8	journal	April 2018
Optical phonons in methylammonium lead halide perovskites and implications for charge transport Sendner, Michael; Nayak, Pabitra K.; Egger, David A. Materials Horizons, Vol. 3, Issue 6 https://doi.org/10.1039/C6MH00275G	journal	January 2016
Room‐temperature electron spin dynamics in GaAs/AlGaAs quantum wells Tackeuchi, Atsushi; Nishikawa, Yuji; Wada, Osamu Applied Physics Letters, Vol. 68, Issue 6 https://doi.org/10.1063/1.116536	journal	February 1996
Electron spin relaxation in InGaAs/InP multiple-quantum wells Tackeuchi, Atsushi; Wada, Osamu; Nishikawa, Yuji Applied Physics Letters, Vol. 70, Issue 9 https://doi.org/10.1063/1.118506	journal	March 1997
Image charge effect on two-dimensional excitons in an inorganic-organic quantum-well crystal Tanaka, Kenichiro; Takahashi, Takayuki; Kondo, Takashi Physical Review B, Vol. 71, Issue 4 https://doi.org/10.1103/PhysRevB.71.045312	journal	January 2005
Excitons in ultrathin organic-inorganic perovskite crystals Yaffe, Omer; Chernikov, Alexey; Norman, Zachariah M. Physical Review B, Vol. 92, Issue 4 https://doi.org/10.1103/PhysRevB.92.045414	journal	July 2015
Lattice dynamics and vibrational spectra of the orthorhombic, tetragonal, and cubic phases of methylammonium lead iodide Brivio, Federico; Frost, Jarvist M.; Skelton, Jonathan M. Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.144308	journal	October 2015
Optical spintronics in organic-inorganic perovskite photovoltaics Li, Junwen; Haney, Paul M. Physical Review B, Vol. 93, Issue 15 https://doi.org/10.1103/PhysRevB.93.155432	journal	April 2016
Spintronics: Fundamentals and applications Žutić, Igor; Fabian, Jaroslav; Das Sarma, S. Reviews of Modern Physics, Vol. 76, Issue 2 https://doi.org/10.1103/RevModPhys.76.323	journal	April 2004
Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita Science Advances, Vol. 2, Issue 6 https://doi.org/10.1126/sciadv.1600477	journal	June 2016
Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies Zhai, Yaxin; Baniya, Sangita; Zhang, Chuang Science Advances, Vol. 3, Issue 7 https://doi.org/10.1126/sciadv.1700704	journal	July 2017
Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites Blancon, J. -C.; Tsai, H.; Nie, W. Science, Vol. 355, Issue 6331 https://doi.org/10.1126/science.aal4211	journal	March 2017

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Biexciton Auger Recombination Differs in Hybrid and Inorganic Halide Perovskite Quantum Dots Eperon, Giles E.; Jedlicka, Erin; Ginger, David S. The Journal of Physical Chemistry Letters, Vol. 9, Issue 1 https://doi.org/10.1021/acs.jpclett.7b02805	journal	December 2017
Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells Liu, Xiaojie; Chanana, Ashish; Huynh, Uyen Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-019-14073-6	journal	January 2020
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Upconverted excitonic photoluminescence from a two-dimensional lead-halide perovskite Yamada, Takumi; Aharen, Tomoko; Kanemitsu, Yoshihiko The Journal of Chemical Physics, Vol. 151, Issue 23 https://doi.org/10.1063/1.5129779	journal	December 2019
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