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Title: Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements

Abstract

Impressive performance of hybrid perovskite solar cells reported in recent years still awaits a comprehensive understanding of its microscopic origins. In this work, the intrinsic Hall mobility and photocarrier recombination coefficient are directly measured in these materials in steady-state transport studies. The results show that electron-hole recombination and carrier trapping rates in hybrid perovskites are very low. The bimolecular recombination coefficient (10–11 to 10–10 cm3 s–1) is found to be on par with that in the best direct-band inorganic semiconductors, even though the intrinsic Hall mobility in hybrid perovskites is considerably lower (up to 60 cm2 V–1 s–1). Measured here, steady-state carrier lifetimes (of up to 3 ms) and diffusion lengths (as long as 650 μm) are significantly longer than those in high-purity crystalline inorganic semiconductors. As a result, we suggest that these experimental findings are consistent with the polaronic nature of charge carriers, resulting from an interaction of charges with methylammonium dipoles.

Authors:
 [1];  [1];  [2];  [3];  [3];  [4];  [5];  [6];  [2];  [1]
+ Show Author Affiliations
  1. Rutgers Univ., Piscataway, NJ (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Univ. of Texas at Dallas, Richardson, TX (United States)
  4. The National Univ. of Science and Technology, MISIS, Moscow (Russia)
  5. Landau Institute for Theoretical Physics, Moscow (Russia)
  6. Univ. of Texas at Dallas, Richardson, TX (United States; The National Univ. of Science and Technology, MISIS, Moscow (Russia)
Publication Date:
Research Org.:
Univ. of Texas at Dallas, Richardson, TX (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1326629
Grant/Contract Number:  
SC0010697
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Chen, Y., Yi, H. T., Wu, X., Haroldson, R., Gartstein, Y. N., Rodionov, Y. I., Tikhonov, K. S., Zakhidov, A., Zhu, X. -Y., and Podzorov, V. Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements. United States: N. p., 2016. Web. doi:10.1038/ncomms12253.
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Chen, Y., Yi, H. T., Wu, X., Haroldson, R., Gartstein, Y. N., Rodionov, Y. I., Tikhonov, K. S., Zakhidov, A., Zhu, X. -Y., & Podzorov, V. Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements. United States. https://doi.org/10.1038/ncomms12253
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Chen, Y., Yi, H. T., Wu, X., Haroldson, R., Gartstein, Y. N., Rodionov, Y. I., Tikhonov, K. S., Zakhidov, A., Zhu, X. -Y., and Podzorov, V. Mon . "Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements". United States. https://doi.org/10.1038/ncomms12253. https://www.osti.gov/servlets/purl/1326629.
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@article{osti_1326629,
title = {Extended carrier lifetimes and diffusion in hybrid perovskites revealed by Hall effect and photoconductivity measurements},
author = {Chen, Y. and Yi, H. T. and Wu, X. and Haroldson, R. and Gartstein, Y. N. and Rodionov, Y. I. and Tikhonov, K. S. and Zakhidov, A. and Zhu, X. -Y. and Podzorov, V.},
abstractNote = {Impressive performance of hybrid perovskite solar cells reported in recent years still awaits a comprehensive understanding of its microscopic origins. In this work, the intrinsic Hall mobility and photocarrier recombination coefficient are directly measured in these materials in steady-state transport studies. The results show that electron-hole recombination and carrier trapping rates in hybrid perovskites are very low. The bimolecular recombination coefficient (10–11 to 10–10 cm3 s–1) is found to be on par with that in the best direct-band inorganic semiconductors, even though the intrinsic Hall mobility in hybrid perovskites is considerably lower (up to 60 cm2 V–1 s–1). Measured here, steady-state carrier lifetimes (of up to 3 ms) and diffusion lengths (as long as 650 μm) are significantly longer than those in high-purity crystalline inorganic semiconductors. As a result, we suggest that these experimental findings are consistent with the polaronic nature of charge carriers, resulting from an interaction of charges with methylammonium dipoles.},
doi = {10.1038/ncomms12253},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Mon Aug 01 00:00:00 EDT 2016},
month = {Mon Aug 01 00:00:00 EDT 2016}
}
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    • APL Materials, Vol. 7, Issue 12
    • DOI: 10.1063/1.5117306

    Understanding the physical properties of hybrid perovskites for photovoltaic applications
    text, January 2017

    • Y., Shao,; J., Huang,; Y., Yan,
    • The University of North Carolina at Chapel Hill University Libraries
    • DOI: 10.17615/r8v8-0t85

    Back-Contact Perovskite Solar Cells
    journal, January 2018

    • Friend, Richard H.; Deschler, Felix; Pazos-Outón, Luis M.
    • Scientific Video Protocols, Vol. 1, Issue 1
    • DOI: 10.32386/scivpro.000005

    First‐Principles Simulation of Carrier Recombination Mechanisms in Halide Perovskites
    journal, April 2020

    • Zhang, Xie; Shen, Jimmy‐Xuan; Van de Walle, Chris G.
    • Advanced Energy Materials, Vol. 10, Issue 13
    • DOI: 10.1002/aenm.201902830

    Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy
    journal, April 2017

    Understanding, Optimizing, and Utilizing Nonideal Transistors Based on Organic or Organic Hybrid Semiconductors
    journal, August 2019

    • Yang, Tengzhou; Wu, Qian; Dai, Fuhua
    • Advanced Functional Materials, Vol. 30, Issue 20
    • DOI: 10.1002/adfm.201903889

    Tracking Structural Phase Transitions in Lead‐Halide Perovskites by Means of Thermal Expansion
    text, January 2019

    • Keshavarz, Masoumeh; Ottesen, Martin; Wiedmann, Steffen
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-04498

    Tracking Structural Phase Transitions in Lead‐Halide Perovskites by Means of Thermal Expansion
    journal, April 2019

    Polaronic transport in CH3NH3PbI3 single crystals
    journal, December 2019

    • Jin, Lei; Qian, Yuqin; Zhang, Yipei
    • Journal of Materials Science: Materials in Electronics, Vol. 31, Issue 3
    • DOI: 10.1007/s10854-019-02713-y

    Low-frequency lattice phonons in halide perovskites explain high defect tolerance toward electron-hole recombination
    journal, February 2020

    The first-principle study of mechanical, optoelectronic and thermoelectric properties of CsGeBr 3 and CsSnBr 3 perovskites
    journal, January 2019

    Lead halide perovskites: Crystal-liquid duality, phonon glass electron crystals, and large polaron formation
    text, January 2017

    • Miyata, Kiyoshi; Atallah, Timothy Luke; Zhu, Xiaoyang
    • Columbia University
    • DOI: 10.7916/d8281kg3

    Structural origins of the electronic properties of materials via time-resolved infrared spectroscopy
    journal, January 2019

    • Munson, Kyle T.; Kennehan, Eric R.; Asbury, John B.
    • Journal of Materials Chemistry C, Vol. 7, Issue 20
    • DOI: 10.1039/c9tc01348b

    Properties of Excitons and Photogenerated Charge Carriers in Metal Halide Perovskites
    journal, September 2018

    Morphological and chemical tuning of lead halide perovskite mesocrystals as long-life anode materials in lithium-ion batteries
    journal, January 2019

    • Wang, Qun; Yang, Tao; Wang, Huanhuan
    • CrystEngComm, Vol. 21, Issue 6
    • DOI: 10.1039/c8ce01779d

    Divalent Anionic Doping in Perovskite Solar Cells for Enhanced Chemical Stability
    journal, July 2018

    • Gong, Jue; Yang, Mengjin; Rebollar, Dominic
    • Advanced Materials, Vol. 30, Issue 34
    • DOI: 10.1002/adma.201800973

    Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites
    journal, August 2018

    Quantifying Polaron Formation and Charge Carrier Cooling in Lead-Iodide Perovskites
    journal, May 2018

    • Bretschneider, Simon A.; Ivanov, Ivan; Wang, Hai I.
    • Advanced Materials, Vol. 30, Issue 29
    • DOI: 10.1002/adma.201707312

    Reactions at noble metal contacts with methylammonium lead triiodide perovskites: Role of underpotential deposition and electrochemistry
    journal, April 2019

    • Kerner, Ross A.; Schulz, Philip; Christians, Jeffrey A.
    • APL Materials, Vol. 7, Issue 4
    • DOI: 10.1063/1.5083812

    Origin of long lifetime of band-edge charge carriers in organic–inorganic lead iodide perovskites
    journal, July 2017

    • Chen, Tianran; Chen, Wei-Liang; Foley, Benjamin J.
    • Proceedings of the National Academy of Sciences, Vol. 114, Issue 29
    • DOI: 10.1073/pnas.1704421114

    Doping and Switchable Photovoltaic Effect in Lead-Free Perovskites Enabled by Metal Cation Transmutation
    journal, July 2018

    • Harikesh, Padinhare Cholakkal; Wu, Bo; Ghosh, Biplab
    • Advanced Materials, Vol. 30, Issue 34
    • DOI: 10.1002/adma.201802080

    Crystal structures and rotational dynamics of a two-dimensional metal halide perovskite (OA) 2 PbI 4
    journal, January 2020

    • Hu, Xiao; Zhang, Depei; Chen, Tianran
    • The Journal of Chemical Physics, Vol. 152, Issue 1
    • DOI: 10.1063/1.5131667

    Optimizing reaction kinetics of sequential deposition technique for ambient air and solution processed hybrid perovskite thin films
    journal, January 2019

    • Khan, Zikriya; Hussain, Zakir; Liaqat, M. Arman
    • Journal of Materials Science: Materials in Electronics, Vol. 30, Issue 4
    • DOI: 10.1007/s10854-019-00716-3

    High thermal conductivity in cubic boron arsenide crystals
    journal, July 2018

    Advances in Alternating Current Electroluminescent Devices
    journal, January 2019

    • Wang, Lin; Xiao, Lian; Gu, Haoshuang
    • Advanced Optical Materials, Vol. 7, Issue 7
    • DOI: 10.1002/adom.201801154

    Dipolar cations confer defect tolerance in wide-bandgap metal halide perovskites
    journal, August 2018

    Quantifying Charge‐Carrier Mobilities and Recombination Rates in Metal Halide Perovskites from Time‐Resolved Microwave Photoconductivity Measurements
    journal, February 2020

    • Savenije, Tom J.; Guo, Dengyang; Caselli, Valentina M.
    • Advanced Energy Materials, Vol. 10, Issue 26
    • DOI: 10.1002/aenm.201903788

    The mechanism of universal green antisolvents for intermediate phase controlled high-efficiency formamidinium-based perovskite solar cells
    journal, January 2020

    • Wang, Luyao; Wang, Xin; Deng, Lin-Long
    • Materials Horizons, Vol. 7, Issue 3
    • DOI: 10.1039/c9mh01679a

    Molecular behavior of zero-dimensional perovskites
    journal, December 2017

    • Yin, Jun; Maity, Partha; De Bastiani, Michele
    • Science Advances, Vol. 3, Issue 12
    • DOI: 10.1126/sciadv.1701793
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