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Title: Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites

Abstract

Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. Here, this work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.

Authors:
 [1];  [2];  [3];  [4]; ORCiD logo [5];  [5];  [3]; ORCiD logo [3];  [6];  [7];  [3];  [3];  [3];  [3];  [8];  [1];  [8];  [3]; ORCiD logo [5];  [7] more »;  [2]; ORCiD logo [9] « less
+ Show Author Affiliations
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States). Makineni Theoretical Lab., Dept. of Chemistry
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  5. Columbia Univ., New York, NY (United States). Dept. of Chemistry
  6. Carnegie Inst. for Science, Washington, DC (United States). Extreme Materials Initiative, Geophysical Lab.
  7. Weizmann Inst. of Science, Rehovoth (Israel). Dept. of Materials and Interfaces
  8. Stanford Univ., CA (United States). Dept. of Chemistry
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Austrian Science Fund (FWF)
OSTI Identifier:
1380107
Grant/Contract Number:  
AC02-76SF00515; ER46980; N00014-17-1-2574; DGE-114747; ECCS-1542152
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Wu, Xiaoxi, Tan, Liang Z., Shen, Xiaozhe, Hu, Te, Miyata, Kiyoshi, Trinh, M. Tuan, Li, Renkai, Coffee, Ryan, Liu, Shi, Egger, David A., Makasyuk, Igor, Zheng, Qiang, Fry, Alan, Robinson, Joseph S., Smith, Matthew D., Guzelturk, Burak, Karunadasa, Hemamala I., Wang, Xijie, Zhu, Xiaoyang, Kronik, Leeor, Rappe, Andrew M., and Lindenberg, Aaron M. Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites. United States: N. p., 2017. Web. doi:10.1126/sciadv.1602388.
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Wu, Xiaoxi, Tan, Liang Z., Shen, Xiaozhe, Hu, Te, Miyata, Kiyoshi, Trinh, M. Tuan, Li, Renkai, Coffee, Ryan, Liu, Shi, Egger, David A., Makasyuk, Igor, Zheng, Qiang, Fry, Alan, Robinson, Joseph S., Smith, Matthew D., Guzelturk, Burak, Karunadasa, Hemamala I., Wang, Xijie, Zhu, Xiaoyang, Kronik, Leeor, Rappe, Andrew M., & Lindenberg, Aaron M. Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites. United States. https://doi.org/10.1126/sciadv.1602388
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Wu, Xiaoxi, Tan, Liang Z., Shen, Xiaozhe, Hu, Te, Miyata, Kiyoshi, Trinh, M. Tuan, Li, Renkai, Coffee, Ryan, Liu, Shi, Egger, David A., Makasyuk, Igor, Zheng, Qiang, Fry, Alan, Robinson, Joseph S., Smith, Matthew D., Guzelturk, Burak, Karunadasa, Hemamala I., Wang, Xijie, Zhu, Xiaoyang, Kronik, Leeor, Rappe, Andrew M., and Lindenberg, Aaron M. Wed . "Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites". United States. https://doi.org/10.1126/sciadv.1602388. https://www.osti.gov/servlets/purl/1380107.
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@article{osti_1380107,
title = {Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites},
author = {Wu, Xiaoxi and Tan, Liang Z. and Shen, Xiaozhe and Hu, Te and Miyata, Kiyoshi and Trinh, M. Tuan and Li, Renkai and Coffee, Ryan and Liu, Shi and Egger, David A. and Makasyuk, Igor and Zheng, Qiang and Fry, Alan and Robinson, Joseph S. and Smith, Matthew D. and Guzelturk, Burak and Karunadasa, Hemamala I. and Wang, Xijie and Zhu, Xiaoyang and Kronik, Leeor and Rappe, Andrew M. and Lindenberg, Aaron M.},
abstractNote = {Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. Here, this work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.},
doi = {10.1126/sciadv.1602388},
journal = {Science Advances},
number = 7,
volume = 3,
place = {United States},
year = {Wed Jul 26 00:00:00 EDT 2017},
month = {Wed Jul 26 00:00:00 EDT 2017}
}
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https://doi.org/10.1126/sciadv.1602388
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High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization
journal, July 2015

  • Saidaminov, Makhsud I.; Abdelhady, Ahmed L.; Murali, Banavoth
  • Nature Communications, Vol. 6, Article No. 7586
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Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide
journal, October 2016

  • Whitfield, P. S.; Herron, N.; Guise, W. E.
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Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
journal, July 2015

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  • Review of Scientific Instruments, Vol. 86, Issue 7
  • DOI: 10.1063/1.4926994

Atomic-Scale Visualization of Inertial Dynamics
journal, April 2005

A hole-conductor-free, fully printable mesoscopic perovskite solar cell with high stability
journal, July 2014

Atomistic origins of high-performance in hybrid halide perovskite solar cells
text, January 2014

Photoferroelectric and Photopiezoelectric Properties of Organometal Halide Perovskites
preprint, January 2015

Local polar fluctuations in lead halide perovskite crystals
text, January 2016

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    The Physics of Light Emission in Halide Perovskite Devices
    journal, September 2018

    • Stranks, Samuel D.; Hoye, Robert L. Z.; Di, Dawei
    • Advanced Materials, Vol. 31, Issue 47
    • DOI: 10.1002/adma.201803336

    Photorefractive Effect in Organic–Inorganic Hybrid Perovskites and Its Application to Optical Phase Shifter
    journal, March 2018

    • Tahara, Hirokazu; Aharen, Tomoko; Wakamiya, Atsushi
    • Advanced Optical Materials, Vol. 6, Issue 11
    • DOI: 10.1002/adom.201701366

    Free Carrier, Exciton, and Phonon Dynamics in Lead‐Halide Perovskites Studied with Ultrafast Terahertz Spectroscopy
    journal, August 2019

    Progress of Surface Science Studies on ABX 3 ‐Based Metal Halide Perovskite Solar Cells
    journal, April 2020

    • Qiu, Longbin; He, Sisi; Ono, Luis K.
    • Advanced Energy Materials, Vol. 10, Issue 13
    • DOI: 10.1002/aenm.201902726

    Kopplung von hoch- und niederfrequenten Schwingungsmoden in organisch-anorganischen Perowskiten
    journal, September 2018

    • Grechko, Maksim; Bretschneider, Simon A.; Vietze, Laura
    • Angewandte Chemie, Vol. 130, Issue 41
    • DOI: 10.1002/ange.201806676

    Vibrational Coupling between Organic and Inorganic Sublattices of Hybrid Perovskites
    journal, September 2018

    • Grechko, Maksim; Bretschneider, Simon A.; Vietze, Laura
    • Angewandte Chemie International Edition, Vol. 57, Issue 41
    • DOI: 10.1002/anie.201806676

    Slow thermal equilibration in methylammonium lead iodide revealed by transient mid-infrared spectroscopy
    journal, July 2018

    Unraveling exciton–phonon coupling in individual FAPbI3 nanocrystals emitting near-infrared single photons
    journal, August 2018

    Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices
    journal, January 2019

    Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites
    journal, March 2019

    Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI3 perovskite nanocrystals
    journal, October 2019

    Entropy in halide perovskites
    journal, April 2018

    Large electrostrictive response in lead halide perovskites
    journal, September 2018

    Hot electron injection into semiconducting polymers in polymer based-perovskite solar cells and their fate
    journal, January 2019

    • Jiménez-López, Jesús; Puscher, Bianka M. D.; Cambarau, Werther
    • Nanoscale, Vol. 11, Issue 48
    • DOI: 10.1039/c9nr06297a

    Long-term stable perovskite solar cells with room temperature processed metal oxide carrier transporters
    journal, January 2019

    • Lei, Lei; Yang, Songwang; Yu, Yu
    • Journal of Materials Chemistry A, Vol. 7, Issue 37
    • DOI: 10.1039/c9ta06875a

    Light enhanced moisture degradation of perovskite solar cell material CH 3 NH 3 PbI 3
    journal, January 2019

    • Lu, Ying-Bo; Cong, Wei-Yan; Guan, ChengBo
    • Journal of Materials Chemistry A, Vol. 7, Issue 48
    • DOI: 10.1039/c9ta10443g

    Can we use time-resolved measurements to get steady-state transport data for halide perovskites?
    journal, September 2018

    • Levine, Igal; Gupta, Satyajit; Bera, Achintya
    • Journal of Applied Physics, Vol. 124, Issue 10
    • DOI: 10.1063/1.5037637

    Research progress on organic–inorganic halide perovskite materials and solar cells
    journal, February 2018

    Light-induced lattice expansion leads to high-efficiency perovskite solar cells
    journal, April 2018

    • Tsai, Hsinhan; Asadpour, Reza; Blancon, Jean-Christophe
    • Science, Vol. 360, Issue 6384
    • DOI: 10.1126/science.aap8671

    Recent Advances in Ultrafast Structural Techniques
    journal, April 2019

    Synergistic Effect of Elevated Device Temperature and Excess Charge Carriers on the Rapid Light-Induced Degradation of Perovskite Solar Cells
    text, January 2019

    • Y., Liu,; J., Song,; J., Huang,
    • The University of North Carolina at Chapel Hill University Libraries
    • DOI: 10.17615/zj42-ct77

    The Physics of Light Emission in Halide Perovskite Devices.
    journalarticle, January 2019

    Large electrostrictive response in lead halide perovskites
    text, January 2018

    • E., Mosconi,; B., Chen,; J., Song,
    • The University of North Carolina at Chapel Hill University Libraries
    • DOI: 10.17615/fjfy-8b57

    Hot Electron Injection into Semiconducting Polymers in Polymer Based-Perovskite Solar Cells and Their Fate
    journal, January 2018

    • Jiménez-López, Jesús; Puscher, Bianka M. D.; Cambarau, Werther
    • SSRN Electronic Journal
    • DOI: 10.2139/ssrn.3305584

    Unraveling exciton-phonon coupling in individual FAPbI(3) nanocrystals emitting near-infrared single photons
    text, January 2018

    Slow cooling of hot polarons in halide perovskite solar cells
    text, January 2017

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