Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites
Abstract
Excitation localization involving dynamic nanoscale distortions is a central aspect of photocatalysis, quantum materials and molecular optoelectronics. Experimental characterization of such distortions requires techniques sensitive to the formation of point-defect-like local structural rearrangements in real time. Here, we visualize excitation-induced strain fields in a prototypical member of the lead halide perovskites via femtosecond resolution diffuse X-ray scattering measurements. Here, this enables momentum-resolved phonon spectroscopy of the locally distorted structure and reveals radially expanding nanometre-scale strain fields associated with the formation and relaxation of polarons in photoexcited perovskites. Quantitative estimates of the magnitude and shape of this polaronic distortion are obtained, providing direct insights into the dynamic structural distortions that occur in these materials. Optical pump–probe reflection spectroscopy corroborates these results and shows how these large polaronic distortions transiently modify the carrier effective mass, providing a unified picture of the coupled structural and electronic dynamics that underlie the optoelectronic functionality of the hybrid perovskites.
- Authors:
-
[1];
[2];
[3];
[5];
[5];
[7]
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
- Univ. of Cambridge (United Kingdom); Aarhus Univ. (Denmark)
- Univ. of Cambridge (United Kingdom)
- Stanford Univ., CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Paderborn Univ. (Germany)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
- Univ. of Cambridge (United Kingdom); Technical Univ. of Munich, Garching (Germany)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1767932
- Alternate Identifier(s):
- OSTI ID: 1784952; OSTI ID: 1837052
- Grant/Contract Number:
- AC02-76SF00515; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 5; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electronic properties and materials; Materials for energy and catalysis; Solar cells; Structural properties; Structure of solids and liquids
Citation Formats
Guzelturk, Burak, Winkler, Thomas, Van de Goor, Tim J., Smith, Matthew D., Bourelle, Sean A., Feldmann, Sascha, Trigo, Mariano, Teitelbaum, Samuel W., Steinrück, Hans-Georg, de la Pena, Gilberto A., Alonso-Mori, Roberto, Zhu, Diling, Sato, Takahiro, Karunadasa, Hemamala I., Toney, Michael F., Deschler, Felix, and Lindenberg, Aaron M. Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites. United States: N. p., 2021.
Web. doi:10.1038/s41563-020-00865-5.
Guzelturk, Burak, Winkler, Thomas, Van de Goor, Tim J., Smith, Matthew D., Bourelle, Sean A., Feldmann, Sascha, Trigo, Mariano, Teitelbaum, Samuel W., Steinrück, Hans-Georg, de la Pena, Gilberto A., Alonso-Mori, Roberto, Zhu, Diling, Sato, Takahiro, Karunadasa, Hemamala I., Toney, Michael F., Deschler, Felix, & Lindenberg, Aaron M. Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites. United States. https://doi.org/10.1038/s41563-020-00865-5
Guzelturk, Burak, Winkler, Thomas, Van de Goor, Tim J., Smith, Matthew D., Bourelle, Sean A., Feldmann, Sascha, Trigo, Mariano, Teitelbaum, Samuel W., Steinrück, Hans-Georg, de la Pena, Gilberto A., Alonso-Mori, Roberto, Zhu, Diling, Sato, Takahiro, Karunadasa, Hemamala I., Toney, Michael F., Deschler, Felix, and Lindenberg, Aaron M. Mon .
"Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites". United States. https://doi.org/10.1038/s41563-020-00865-5. https://www.osti.gov/servlets/purl/1767932.
@article{osti_1767932,
title = {Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites},
author = {Guzelturk, Burak and Winkler, Thomas and Van de Goor, Tim J. and Smith, Matthew D. and Bourelle, Sean A. and Feldmann, Sascha and Trigo, Mariano and Teitelbaum, Samuel W. and Steinrück, Hans-Georg and de la Pena, Gilberto A. and Alonso-Mori, Roberto and Zhu, Diling and Sato, Takahiro and Karunadasa, Hemamala I. and Toney, Michael F. and Deschler, Felix and Lindenberg, Aaron M.},
abstractNote = {Excitation localization involving dynamic nanoscale distortions is a central aspect of photocatalysis, quantum materials and molecular optoelectronics. Experimental characterization of such distortions requires techniques sensitive to the formation of point-defect-like local structural rearrangements in real time. Here, we visualize excitation-induced strain fields in a prototypical member of the lead halide perovskites via femtosecond resolution diffuse X-ray scattering measurements. Here, this enables momentum-resolved phonon spectroscopy of the locally distorted structure and reveals radially expanding nanometre-scale strain fields associated with the formation and relaxation of polarons in photoexcited perovskites. Quantitative estimates of the magnitude and shape of this polaronic distortion are obtained, providing direct insights into the dynamic structural distortions that occur in these materials. Optical pump–probe reflection spectroscopy corroborates these results and shows how these large polaronic distortions transiently modify the carrier effective mass, providing a unified picture of the coupled structural and electronic dynamics that underlie the optoelectronic functionality of the hybrid perovskites.},
doi = {10.1038/s41563-020-00865-5},
journal = {Nature Materials},
number = 5,
volume = 20,
place = {United States},
year = {Mon Jan 04 00:00:00 EST 2021},
month = {Mon Jan 04 00:00:00 EST 2021}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Band-gap narrowing in heavily doped many-valley semiconductors
journal, August 1981
- Berggren, K. -F.; Sernelius, B. E.
- Physical Review B, Vol. 24, Issue 4
Hybrid organic—inorganic perovskites: low-cost semiconductors with intriguing charge-transport properties
journal, January 2016
- Brenner, Thomas M.; Egger, David A.; Kronik, Leeor
- Nature Reviews Materials, Vol. 1, Issue 1
Time-Resolved X-Ray Diffraction from Coherent Phonons during a Laser-Induced Phase Transition
journal, January 2000
- Lindenberg, A. M.; Kang, I.; Johnson, S. L.
- Physical Review Letters, Vol. 84, Issue 1
Large polarons in lead halide perovskites
journal, August 2017
- Miyata, Kiyoshi; Meggiolaro, Daniele; Trinh, M. Tuan
- Science Advances, Vol. 3, Issue 8
Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites
journal, January 2019
- Thouin, Félix; Valverde-Chávez, David A.; Quarti, Claudio
- Nature Materials, Vol. 18, Issue 4
Origins of band-gap renormalization in degenerately doped semiconductors
journal, August 2008
- Walsh, Aron; Da Silva, Juarez L. F.; Wei, Su-Huai
- Physical Review B, Vol. 78, Issue 7
Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces
journal, May 2017
- Shcherbakov, Maxim R.; Liu, Sheng; Zubyuk, Varvara V.
- Nature Communications, Vol. 8, Issue 1
Dielectric Response: Answer to Many Questions in the Methylammonium Lead Halide Solar Cell Absorbers
journal, May 2017
- Anusca, Irina; Balčiūnas, Sergejus; Gemeiner, Pascale
- Advanced Energy Materials, Vol. 7, Issue 19
A map of high-mobility molecular semiconductors
journal, September 2017
- Fratini, S.; Ciuchi, S.; Mayou, D.
- Nature Materials, Vol. 16, Issue 10
Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite
journal, May 2019
- Lan, Yang; Dringoli, Benjamin J.; Valverde-Chávez, David A.
- Science Advances, Vol. 5, Issue 5
Dynamic emission Stokes shift and liquid-like dielectric solvation of band edge carriers in lead-halide perovskites
journal, March 2019
- Guo, Yinsheng; Yaffe, Omer; Hull, Trevor D.
- Nature Communications, Vol. 10, Issue 1
Picosecond X-ray diffraction studies of laser-excited acoustic phonons in InSb
journal, October 2002
- Larsson, J.; Allen, A.; Bucksbaum, P. H.
- Applied Physics A: Materials Science & Processing, Vol. 75, Issue 4
Optical phonons in methylammonium lead halide perovskites and implications for charge transport
journal, January 2016
- Sendner, Michael; Nayak, Pabitra K.; Egger, David A.
- Materials Horizons, Vol. 3, Issue 6
Transmission Electron Microscopy and Diffractometry of Materials
book, January 2013
- Fultz, Brent; Howe, James
- Graduate Texts in Physics
The X-ray Pump–Probe instrument at the Linac Coherent Light Source
journal, April 2015
- Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco
- Journal of Synchrotron Radiation, Vol. 22, Issue 3
Excitation-wavelength-dependent small polaron trapping of photoexcited carriers in α-Fe2O3
journal, July 2017
- Carneiro, Lucas M.; Cushing, Scott K.; Liu, Chong
- Nature Materials, Vol. 16, Issue 8
Defect Properties from X-Ray Scattering Experiments
journal, December 1976
- Peisl, H.
- Le Journal de Physique Colloques, Vol. 37, Issue C7
Carrier-induced change in refractive index of InP, GaAs and InGaAsP
journal, January 1990
- Bennett, B. R.; Soref, R. A.; Del Alamo, J. A.
- IEEE Journal of Quantum Electronics, Vol. 26, Issue 1
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
Electron-Phonon Interaction and Charge Carrier Mass Enhancement in
journal, June 2008
- van Mechelen, J. L. M.; van der Marel, D.; Grimaldi, C.
- Physical Review Letters, Vol. 100, Issue 22
Polarons in Halide Perovskites: A Perspective
journal, March 2020
- Ghosh, Dibyajyoti; Welch, Eric; Neukirch, Amanda J.
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 9
The influence of the Rashba effect
journal, April 2018
- Stranks, Samuel D.; Plochocka, Paulina
- Nature Materials, Vol. 17, Issue 5
Atomistic Origins of High-Performance in Hybrid Halide Perovskite Solar Cells
journal, April 2014
- Frost, Jarvist M.; Butler, Keith T.; Brivio, Federico
- Nano Letters, Vol. 14, Issue 5
Ferroelectric large polarons
journal, April 2018
- Miyata, Kiyoshi; Zhu, X. -Y.
- Nature Materials, Vol. 17, Issue 5
Time-Frequency Spectroscopy of Transient Dispersion Using Few-Cycle Pump-Probe Reflectometry
journal, May 2020
- Jani, Hemang; Duan, Lingze
- Physical Review Applied, Vol. 13, Issue 5
Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites
journal, July 2017
- Wu, Xiaoxi; Tan, Liang Z.; Shen, Xiaozhe
- Science Advances, Vol. 3, Issue 7
Imaging magnetic polarons in the doped Fermi–Hubbard model
journal, August 2019
- Koepsell, Joannis; Vijayan, Jayadev; Sompet, Pimonpan
- Nature, Vol. 572, Issue 7769
Ultrafast THz Probe of Photoinduced Polarons in Lead-Halide Perovskites
journal, April 2019
- Cinquanta, Eugenio; Meggiolaro, Daniele; Motti, Silvia G.
- Physical Review Letters, Vol. 122, Issue 16
Polarons in Halide Perovskites: A Perspective
journal, March 2020
- Ghosh, Dibyajyoti; Welch, Eric; Neukirch, Amanda J.
- The Journal of Physical Chemistry Letters, Vol. 11, Issue 9
A map of high-mobility molecular semiconductors
journal, September 2017
- Fratini, S.; Ciuchi, S.; Mayou, D.
- Nature Materials, Vol. 16, Issue 10
Inversion symmetry and bulk Rashba effect in methylammonium lead iodide perovskite single crystals
journal, May 2018
- Frohna, Kyle; Deshpande, Tejas; Harter, John
- Nature Communications, Vol. 9, Issue 1
The influence of the Rashba effect
journal, April 2018
- Stranks, Samuel D.; Plochocka, Paulina
- Nature Materials, Vol. 17, Issue 5