Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films
Abstract
The effect of carrier–carrier and carrier–phonon interactions is presented in n = 1 (2D) (BA)2PbI4 Ruddlesden–Popper thin films, and their effect is compared to that of conventional MAPbI3. While temperature-dependent photoluminescence shows the well-studied structural phase transitions and evidence of longitudinal optical (LO) phonon scattering in MPbI3, the 2D (BA)2PbI4 films produce subtler properties. At low temperatures, evidence of two competing intrinsic exciton transitions is observed (P1 and P3), in addition to several extrinsic transitions attributed to the impurities in the (BA)2PbI4 film. At higher temperatures, (BA)2PbI4 is dominated by the two intrinsic excitons that are attributed to varying degrees of localization caused by deformations of the PbI4 framework mediated by structural relaxation. Although both exciton complexes are well separated from the continuum (490 meV or greater), their interaction with phonons is quite different. In the case of the more strongly bound complex (P3), the strong excitonic nature and short-range interaction are mediated by the emission of LO phonon replicas. In the case of the exciton with the smaller binding energy (P1), the more extended wavefunction manifests itself in strong carrier–phonon scattering and evidence of large, stable polarons.
- Authors:
-
[1];
[1];
[2];
[4];
[4];
- Univ. of Oklahoma, Norman, OK (United States)
- Univ. of Washington, Seattle, WA (United States); Univ. of Cambridge (United Kingdom). Cavendish Lab.
- Univ. of Washington, Seattle, WA (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Oklahoma, Norman, OK (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; European Union (EU); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1660109
- Alternate Identifier(s):
- OSTI ID: 1606388
- Report Number(s):
- NREL/JA-5900-74534
Journal ID: ISSN 1932-7447; MainId:6727;UUID:a5f02f31-37b6-e911-9c24-ac162d87dfe5;MainAdminID:14118
- Grant/Contract Number:
- AC36-08GO28308; SC0019384; 699935
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 124; Journal Issue: 17; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 2D perovskites; excitons; LO phonons; polarons; 36 MATERIALS SCIENCE; Phonons; Energy; Phase transitions; Perovskites
Citation Formats
Esmaielpour, H., Whiteside, V. R., Sourabh, S., Eperon, G. E., Precht, J. T., Beard, M. C., Lu, H., Durant, B. K., and Sellers, I. R. Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.9b12032.
Esmaielpour, H., Whiteside, V. R., Sourabh, S., Eperon, G. E., Precht, J. T., Beard, M. C., Lu, H., Durant, B. K., & Sellers, I. R. Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films. United States. https://doi.org/10.1021/acs.jpcc.9b12032
Esmaielpour, H., Whiteside, V. R., Sourabh, S., Eperon, G. E., Precht, J. T., Beard, M. C., Lu, H., Durant, B. K., and Sellers, I. R. Sun .
"Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films". United States. https://doi.org/10.1021/acs.jpcc.9b12032. https://www.osti.gov/servlets/purl/1660109.
@article{osti_1660109,
title = {Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films},
author = {Esmaielpour, H. and Whiteside, V. R. and Sourabh, S. and Eperon, G. E. and Precht, J. T. and Beard, M. C. and Lu, H. and Durant, B. K. and Sellers, I. R.},
abstractNote = {The effect of carrier–carrier and carrier–phonon interactions is presented in n = 1 (2D) (BA)2PbI4 Ruddlesden–Popper thin films, and their effect is compared to that of conventional MAPbI3. While temperature-dependent photoluminescence shows the well-studied structural phase transitions and evidence of longitudinal optical (LO) phonon scattering in MPbI3, the 2D (BA)2PbI4 films produce subtler properties. At low temperatures, evidence of two competing intrinsic exciton transitions is observed (P1 and P3), in addition to several extrinsic transitions attributed to the impurities in the (BA)2PbI4 film. At higher temperatures, (BA)2PbI4 is dominated by the two intrinsic excitons that are attributed to varying degrees of localization caused by deformations of the PbI4 framework mediated by structural relaxation. Although both exciton complexes are well separated from the continuum (490 meV or greater), their interaction with phonons is quite different. In the case of the more strongly bound complex (P3), the strong excitonic nature and short-range interaction are mediated by the emission of LO phonon replicas. In the case of the exciton with the smaller binding energy (P1), the more extended wavefunction manifests itself in strong carrier–phonon scattering and evidence of large, stable polarons.},
doi = {10.1021/acs.jpcc.9b12032},
journal = {Journal of Physical Chemistry. C},
number = 17,
volume = 124,
place = {United States},
year = {Sun Mar 29 00:00:00 EDT 2020},
month = {Sun Mar 29 00:00:00 EDT 2020}
}
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