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Title: Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods

Abstract

Charge carrier mobilities help determine semiconductor performance in optoelectronic applications, but measurement of the individual electron and hole mobilities usually involves indirect methods or probes with electrical contacts that are influenced by the quality of the interface or contact. Here, a noncontact method is introduced to distinguish the mobilities of electrons and holes by combining time-resolved terahertz spectroscopy (TRTS) and optical transient reflection (TR) spectroscopy. The validation of this method is first demonstrated on a semi-insulator GaAs wafer, and then, three lead-halide perovskite polycrystalline films with different cation mixtures are studied. We find that the hole mobility is significantly higher (~10x) than that of the electron mobility in all of the perovskite thin films studied. The highly alloyed triple cation polycrystalline film shows the highest mobility, longest bulk carrier lifetime, and lowest surface recombination velocity.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States); Xiamen Univ., Xiamen (China)
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)
OSTI Identifier:
1580494
Report Number(s):
NREL/JA-5900-74898
Journal ID: ISSN 2380-8195
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; carrier mobility; THz; perovskite thin films

Citation Formats

Zhai, Yaxin, Wang, Kang, Zhang, Fei, Xiao, Chuanxiao, Rose, Aaron H., Zhu, Kai, and Beard, Matthew C. Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.9b02310.
Zhai, Yaxin, Wang, Kang, Zhang, Fei, Xiao, Chuanxiao, Rose, Aaron H., Zhu, Kai, & Beard, Matthew C. Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods. United States. doi:10.1021/acsenergylett.9b02310.
Zhai, Yaxin, Wang, Kang, Zhang, Fei, Xiao, Chuanxiao, Rose, Aaron H., Zhu, Kai, and Beard, Matthew C. Thu . "Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods". United States. doi:10.1021/acsenergylett.9b02310. https://www.osti.gov/servlets/purl/1580494.
@article{osti_1580494,
title = {Individual Electron and Hole Mobilities in Lead-Halide Perovskites Revealed by Noncontact Methods},
author = {Zhai, Yaxin and Wang, Kang and Zhang, Fei and Xiao, Chuanxiao and Rose, Aaron H. and Zhu, Kai and Beard, Matthew C.},
abstractNote = {Charge carrier mobilities help determine semiconductor performance in optoelectronic applications, but measurement of the individual electron and hole mobilities usually involves indirect methods or probes with electrical contacts that are influenced by the quality of the interface or contact. Here, a noncontact method is introduced to distinguish the mobilities of electrons and holes by combining time-resolved terahertz spectroscopy (TRTS) and optical transient reflection (TR) spectroscopy. The validation of this method is first demonstrated on a semi-insulator GaAs wafer, and then, three lead-halide perovskite polycrystalline films with different cation mixtures are studied. We find that the hole mobility is significantly higher (~10x) than that of the electron mobility in all of the perovskite thin films studied. The highly alloyed triple cation polycrystalline film shows the highest mobility, longest bulk carrier lifetime, and lowest surface recombination velocity.},
doi = {10.1021/acsenergylett.9b02310},
journal = {ACS Energy Letters},
number = 1,
volume = 5,
place = {United States},
year = {2019},
month = {11}
}

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Works referenced in this record:

Efficient Hybrid Solar Cells Based on Meso-Superstructured Organometal Halide Perovskites
journal, October 2012


Sequential deposition as a route to high-performance perovskite-sensitized solar cells
journal, July 2013

  • Burschka, Julian; Pellet, Norman; Moon, Soo-Jin
  • Nature, Vol. 499, Issue 7458, p. 316-319
  • DOI: 10.1038/nature12340

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
  • DOI: 10.1038/nature12509

Understanding the physical properties of hybrid perovskites for photovoltaic applications
journal, July 2017


Giant Rashba splitting in 2D organic-inorganic halide perovskites measured by transient spectroscopies
journal, July 2017


Spin-optoelectronic devices based on hybrid organic-inorganic trihalide perovskites
journal, January 2019


Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors
journal, April 2015

  • Zhu, Haiming; Fu, Yongping; Meng, Fei
  • Nature Materials, Vol. 14, Issue 6
  • DOI: 10.1038/nmat4271

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
  • DOI: 10.1038/nnano.2014.149

Halide Perovskites: Is It All about the Interfaces?
journal, March 2019


Ultrafast Spectroscopy of Photoexcitations in Organometal Trihalide Perovskites
journal, February 2016

  • Zhai, Yaxin; Sheng, Chuan Xiang; Zhang, Chuang
  • Advanced Functional Materials, Vol. 26, Issue 10
  • DOI: 10.1002/adfm.201505115

Electron-Hole Diffusion Lengths Exceeding 1 Micrometer in an Organometal Trihalide Perovskite Absorber
journal, October 2013

  • Stranks, S. D.; Eperon, G. E.; Grancini, G.
  • Science, Vol. 342, Issue 6156, p. 341-344
  • DOI: 10.1126/science.1243982

Charge-Carrier Mobilities in Metal Halide Perovskites: Fundamental Mechanisms and Limits
journal, June 2017


Minority and Majority Charge Carrier Mobility in Cu2ZnSnSe4 revealed by Terahertz Spectroscopy
journal, September 2018


Low trap-state density and long carrier diffusion in organolead trihalide perovskite single crystals
journal, January 2015


Electron and hole drift mobility measurements on methylammonium lead iodide perovskite solar cells
journal, April 2016

  • Maynard, Brian; Long, Qi; Schiff, Eric A.
  • Applied Physics Letters, Vol. 108, Issue 17
  • DOI: 10.1063/1.4948344

Highly stable and efficient all-inorganic lead-free perovskite solar cells with native-oxide passivation
journal, January 2019


Formamidinium lead trihalide: a broadly tunable perovskite for efficient planar heterojunction solar cells
journal, January 2014

  • Eperon, Giles E.; Stranks, Samuel D.; Menelaou, Christopher
  • Energy & Environmental Science, Vol. 7, Issue 3
  • DOI: 10.1039/c3ee43822h

Empirical low-field mobility model for III–V compounds applicable in device simulation codes
journal, March 2000

  • Sotoodeh, M.; Khalid, A. H.; Rezazadeh, A. A.
  • Journal of Applied Physics, Vol. 87, Issue 6
  • DOI: 10.1063/1.372274

Electronic Traps and Their Correlations to Perovskite Solar Cell Performance via Compositional and Thermal Annealing Controls
journal, January 2019

  • Hwang, Taehyun; Yun, Alan Jiwan; Kim, Jinhyun
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 7
  • DOI: 10.1021/acsami.8b17431

Tailored interfaces of unencapsulated perovskite solar cells for >1,000 hour operational stability
journal, January 2018


Suppressing defects through the synergistic effect of a Lewis base and a Lewis acid for highly efficient and stable perovskite solar cells
journal, January 2018

  • Zhang, Fei; Bi, Dongqin; Pellet, Norman
  • Energy & Environmental Science, Vol. 11, Issue 12
  • DOI: 10.1039/C8EE02252F

Self-Seeding Growth for Perovskite Solar Cells with Enhanced Stability
journal, June 2019


Tuning the crystal growth of perovskite thin-films by adding the 2-pyridylthiourea additive for highly efficient and stable solar cells prepared in ambient air
journal, January 2017

  • Sun, Mengna; Zhang, Fei; Liu, Hongli
  • Journal of Materials Chemistry A, Vol. 5, Issue 26
  • DOI: 10.1039/C7TA00894E

Top and bottom surfaces limit carrier lifetime in lead iodide perovskite films
journal, January 2017


Transient photoconductivity in GaAs as measured by time-resolved terahertz spectroscopy
journal, December 2000

  • Beard, Matthew C.; Turner, Gordon M.; Schmuttenmaer, Charles A.
  • Physical Review B, Vol. 62, Issue 23
  • DOI: 10.1103/PhysRevB.62.15764

Propagation of terahertz pulses in photoexcited media: Analytical theory for layered systems
journal, July 2007

  • Kužel, P.; Kadlec, F.; Němec, H.
  • The Journal of Chemical Physics, Vol. 127, Issue 2
  • DOI: 10.1063/1.2748402

Carrier dynamics in semiconductors studied with time-resolved terahertz spectroscopy
journal, June 2011


Enhanced mobility CsPbI 3 quantum dot arrays for record-efficiency, high-voltage photovoltaic cells
journal, October 2017

  • Sanehira, Erin M.; Marshall, Ashley R.; Christians, Jeffrey A.
  • Science Advances, Vol. 3, Issue 10
  • DOI: 10.1126/sciadv.aao4204

Elucidating the role of disorder and free-carrier recombination kinetics in CH3NH3PbI3 perovskite films
journal, July 2015

  • La-o-vorakiat, Chan; Salim, Teddy; Kadro, Jeannette
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8903

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
  • DOI: 10.1021/acs.jpclett.5b02223

Monitoring Electron–Phonon Interactions in Lead Halide Perovskites Using Time-Resolved THz Spectroscopy
journal, July 2019


Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements
journal, August 2016


Ultrafast THz Probe of Photoinduced Polarons in Lead-Halide Perovskites
journal, April 2019


Phonon features in terahertz photoconductivity spectra due to data analysis artifact: A case study on organometallic halide perovskites
journal, March 2017

  • La-o-vorakiat, Chan; Cheng, Liang; Salim, Teddy
  • Applied Physics Letters, Vol. 110, Issue 12
  • DOI: 10.1063/1.4978688

Intrinsic femtosecond charge generation dynamics in single crystal CH 3 NH 3 PbI 3
journal, January 2015

  • Valverde-Chávez, David A.; Ponseca, Carlito S.; Stoumpos, Constantinos C.
  • Energy & Environmental Science, Vol. 8, Issue 12
  • DOI: 10.1039/C5EE02503F

Grain-Size-Limited Mobility in Methylammonium Lead Iodide Perovskite Thin Films
journal, August 2016


Temperature-Dependent Charge-Carrier Dynamics in CH 3 NH 3 PbI 3 Perovskite Thin Films
journal, September 2015

  • Milot, Rebecca L.; Eperon, Giles E.; Snaith, Henry J.
  • Advanced Functional Materials, Vol. 25, Issue 39
  • DOI: 10.1002/adfm.201502340

The effect of structural dimensionality on carrier mobility in lead-halide perovskites
journal, January 2019

  • Hartono, Noor Titan Putri; Sun, Shijing; Gélvez-Rueda, María C.
  • Journal of Materials Chemistry A, Vol. 7, Issue 41
  • DOI: 10.1039/C9TA05241K

Long Minority-Carrier Diffusion Length and Low Surface-Recombination Velocity in Inorganic Lead-Free CsSnI 3 Perovskite Crystal for Solar Cells
journal, January 2017

  • Wu, Bo; Zhou, Yuanyuan; Xing, Guichuan
  • Advanced Functional Materials, Vol. 27, Issue 7
  • DOI: 10.1002/adfm.201604818

Ultrafast probes at the interfaces of solar energy conversion materials
journal, January 2019

  • Chen, Xihan; Wang, Kang; Beard, Matthew C.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 30
  • DOI: 10.1039/C9CP02768H

The ambipolar diffusion coefficient in silicon: Dependence on excess‐carrier concentration and temperature
journal, September 1994

  • Rosling, M.; Bleichner, H.; Jonsson, P.
  • Journal of Applied Physics, Vol. 76, Issue 5
  • DOI: 10.1063/1.358504

Temperature-Dependent Ambipolar Charge Carrier Mobility in Large-Crystal Hybrid Halide Perovskite Thin Films
journal, May 2019

  • Biewald, Alexander; Giesbrecht, Nadja; Bein, Thomas
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 23
  • DOI: 10.1021/acsami.9b04592

Intragrain charge transport in kesterite thin films—Limits arising from carrier localization
journal, November 2016

  • Hempel, Hannes; Redinger, Alex; Repins, Ingrid
  • Journal of Applied Physics, Vol. 120, Issue 17
  • DOI: 10.1063/1.4965868

Applicability of the thin-film approximation in terahertz photoconductivity measurements
journal, December 2018

  • Neu, Jens; Regan, Kevin P.; Swierk, John R.
  • Applied Physics Letters, Vol. 113, Issue 23
  • DOI: 10.1063/1.5052232

Tailoring Organic Cation of 2D Air-Stable Organometal Halide Perovskites for Highly Efficient Planar Solar Cells
journal, May 2017


Improved Understanding of the Electronic and Energetic Landscapes of Perovskite Solar Cells: High Local Charge Carrier Mobility, Reduced Recombination, and Extremely Shallow Traps
journal, September 2014

  • Oga, Hikaru; Saeki, Akinori; Ogomi, Yuhei
  • Journal of the American Chemical Society, Vol. 136, Issue 39
  • DOI: 10.1021/ja506936f

Direct Observation of Long Electron-Hole Diffusion Distance in CH3NH3PbI3 Perovskite Thin Film
journal, September 2015

  • Li, Yu; Yan, Weibo; Li, Yunlong
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep14485

Electron-hole diffusion lengths > 175 μm in solution-grown CH 3 NH 3 PbI 3 single crystals
journal, January 2015


The In-Gap Electronic State Spectrum of Methylammonium Lead Iodide Single-Crystal Perovskites
journal, March 2016

  • Adinolfi, Valerio; Yuan, Mingjian; Comin, Riccardo
  • Advanced Materials, Vol. 28, Issue 17
  • DOI: 10.1002/adma.201505162

Terahertz Emission from Hybrid Perovskites Driven by Ultrafast Charge Separation and Strong Electron-Phonon Coupling
journal, January 2018

  • Guzelturk, Burak; Belisle, Rebecca A.; Smith, Matthew D.
  • Advanced Materials, Vol. 30, Issue 11
  • DOI: 10.1002/adma.201704737

Insights into charge carrier dynamics in organo-metal halide perovskites: from neat films to solar cells
journal, January 2017

  • Peng, Jiajun; Chen, Yani; Zheng, Kaibo
  • Chemical Society Reviews, Vol. 46, Issue 19
  • DOI: 10.1039/C6CS00942E