Local polar fluctuations in lead halide perovskite crystals
Abstract
Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low-frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in the cubic phase of both hybrid (CH3NH3PbBr3) and all-inorganic (CsPbBr3) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations indicate that head-to-head Cs motion coupled to Br face expansion, occurring on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr3.
- Authors:
-
- Columbia Univ., New York, NY (United States)
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Weizmann Institute of Science, Rehovoth (Israel)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Columbia Univ., New York, NY (United States); Univ. Federal de Minas Gerais, Belo Horizonte (Brazil)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC); Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1352545
- Alternate Identifier(s):
- OSTI ID: 1349148; OSTI ID: 1494837
- Grant/Contract Number:
- SC0001085; IOF-622653; N00014-14-1-0761; N00014-12-1-1033; FG02-07ER46431; J3608-N20; NA0002522; AC02-76SF00515
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 118; Journal Issue: 13; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; 36 MATERIALS SCIENCE; local polar fluctuations; hybrid perovskites; low frequency Raman scattering; molecular dynamics; radiation detection; Central peak
Citation Formats
Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., and Brus, Louis E. Local polar fluctuations in lead halide perovskite crystals. United States: N. p., 2017.
Web. doi:10.1103/PhysRevLett.118.136001.
Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., & Brus, Louis E. Local polar fluctuations in lead halide perovskite crystals. United States. https://doi.org/10.1103/PhysRevLett.118.136001
Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., and Brus, Louis E. Tue .
"Local polar fluctuations in lead halide perovskite crystals". United States. https://doi.org/10.1103/PhysRevLett.118.136001. https://www.osti.gov/servlets/purl/1352545.
@article{osti_1352545,
title = {Local polar fluctuations in lead halide perovskite crystals},
author = {Yaffe, Omer and Guo, Yinsheng and Tan, Liang Z. and Egger, David A. and Hull, Trevor and Stoumpos, Constantinos C. and Zheng, Fan and Heinz, Tony F. and Kronik, Leeor and Kanatzidis, Mercouri G. and Owen, Jonathan S. and Rappe, Andrew M. and Pimenta, Marcos A. and Brus, Louis E.},
abstractNote = {Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low-frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in the cubic phase of both hybrid (CH3NH3PbBr3) and all-inorganic (CsPbBr3) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations indicate that head-to-head Cs motion coupled to Br face expansion, occurring on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr3.},
doi = {10.1103/PhysRevLett.118.136001},
journal = {Physical Review Letters},
number = 13,
volume = 118,
place = {United States},
year = {Tue Mar 28 00:00:00 EDT 2017},
month = {Tue Mar 28 00:00:00 EDT 2017}
}
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FIG. 1. : Low-frequency Raman spectra of hybrid and inorganic lead-halide perovskite crystals. The spectral region obscured by the notch-filter, between ±10 cm−1 (marked by the vertical dashed lines), has been deleted. (a) CH3NH3PbBr3 and (b) CsPbBr3 in the orthorhombic phase (blue), tetragonal phase (green), and cubic phase (red), showingmore »
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Low-temperature Benchtop-synthesis of All-inorganic Perovskite Nanowires
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