Large polaron self-trapped states in three-dimensional metal-halide perovskites
In recent years, metal halide perovskites have generated tremendous interest for optoelectronic applications and their underlying fundamental properties. Due to the large electron-phonon coupling characteristic of soft lattices, self-trapping phenomena are expected to dominate hybrid perovskite phot...
| Main Authors: | , , , , , , , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2021
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/147043 |
| _version_ | 1811695661824868352 |
|---|---|
| author | Wong, Walter P. D. Yin, Jun Chaudary, Bhumika Chin, Xin Yu Cortecchia, Daniele Lo, Shu-Zee A. Grimsdale, Andrew C. Mohammed, Omar F. Lanzani, Guglielmo Soci, Cesare |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Wong, Walter P. D. Yin, Jun Chaudary, Bhumika Chin, Xin Yu Cortecchia, Daniele Lo, Shu-Zee A. Grimsdale, Andrew C. Mohammed, Omar F. Lanzani, Guglielmo Soci, Cesare |
| author_sort | Wong, Walter P. D. |
| collection | NTU |
| description | In recent years, metal halide perovskites have generated tremendous interest for optoelectronic applications and their underlying fundamental properties. Due to the large electron-phonon coupling characteristic of soft lattices, self-trapping phenomena are expected to dominate hybrid perovskite photoexcitation dynamics. Yet, while the photogeneration of small polarons was proven in low dimensional perovskites, the nature of polaron excitations in technologically relevant 3D perovskites, and their influence on charge carrier transport, remain elusive. In this study, we used a combination of first principle calculations and advanced spectroscopy techniques spanning the entire optical frequency range to pin down polaron features in 3D metal halide perovskites. Mid-infrared photoinduced absorption shows the photogeneration of states associated to low energy intragap electronic transitions with lifetime up to the ms time scale, and vibrational mode renormalization in both frequency and amplitude. Density functional theory supports the assignment of the spectroscopic features to large polarons leading to new intra gap transitions, hardening of phonon mode frequency, and renormalization of the oscillator strength. Theory provides quantitative estimation for the charge carrier masses and mobilities increase upon polaron formation, confirming experimental results. Overall, this work contributes to complete the scenario of elementary photoexcitations in metal halide perovskites and highlights the importance of polaronic transport in perovskite-based optoelectronic devices. |
| first_indexed | 2024-10-01T07:27:01Z |
| format | Journal Article |
| id | ntu-10356/147043 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T07:27:01Z |
| publishDate | 2021 |
| record_format | dspace |
| spelling | ntu-10356/1470432023-02-28T19:50:57Z Large polaron self-trapped states in three-dimensional metal-halide perovskites Wong, Walter P. D. Yin, Jun Chaudary, Bhumika Chin, Xin Yu Cortecchia, Daniele Lo, Shu-Zee A. Grimsdale, Andrew C. Mohammed, Omar F. Lanzani, Guglielmo Soci, Cesare School of Physical and Mathematical Sciences School of Materials Science and Engineering Interdisciplinary Graduate School (IGS) Energy Research Institute @ NTU (ERI@N) Engineering::Materials::Energy materials Science::Physics::Optics and light Perovskite Polaron In recent years, metal halide perovskites have generated tremendous interest for optoelectronic applications and their underlying fundamental properties. Due to the large electron-phonon coupling characteristic of soft lattices, self-trapping phenomena are expected to dominate hybrid perovskite photoexcitation dynamics. Yet, while the photogeneration of small polarons was proven in low dimensional perovskites, the nature of polaron excitations in technologically relevant 3D perovskites, and their influence on charge carrier transport, remain elusive. In this study, we used a combination of first principle calculations and advanced spectroscopy techniques spanning the entire optical frequency range to pin down polaron features in 3D metal halide perovskites. Mid-infrared photoinduced absorption shows the photogeneration of states associated to low energy intragap electronic transitions with lifetime up to the ms time scale, and vibrational mode renormalization in both frequency and amplitude. Density functional theory supports the assignment of the spectroscopic features to large polarons leading to new intra gap transitions, hardening of phonon mode frequency, and renormalization of the oscillator strength. Theory provides quantitative estimation for the charge carrier masses and mobilities increase upon polaron formation, confirming experimental results. Overall, this work contributes to complete the scenario of elementary photoexcitations in metal halide perovskites and highlights the importance of polaronic transport in perovskite-based optoelectronic devices. Ministry of Education (MOE) National Research Foundation (NRF) Accepted version Research was supported by the National Research Foundation (NRF-CRP14-2014-03) and by the Ministry of Education (MOE2016-T1-1-164) of Singapore. 2021-03-22T02:14:05Z 2021-03-22T02:14:05Z 2020 Journal Article Wong, W. P. D., Yin, J., Chaudary, B., Chin, X. Y., Cortecchia, D., Lo, S. A., Grimsdale, A. C., Mohammed, O. F., Lanzani, G. & Soci, C. (2020). Large polaron self-trapped states in three-dimensional metal-halide perovskites. ACS Materials Letters, 2(1), 20-27. https://dx.doi.org/10.1021/acsmaterialslett.9b00276 2639-4979 https://hdl.handle.net/10356/147043 10.1021/acsmaterialslett.9b00276 1 2 20 27 en NRF-CRP14-2014-03 MOE2016-T1-1-164 ACS Materials Letters This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Materials Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsmaterialslett.9b00276 application/pdf application/pdf |
| spellingShingle | Engineering::Materials::Energy materials Science::Physics::Optics and light Perovskite Polaron Wong, Walter P. D. Yin, Jun Chaudary, Bhumika Chin, Xin Yu Cortecchia, Daniele Lo, Shu-Zee A. Grimsdale, Andrew C. Mohammed, Omar F. Lanzani, Guglielmo Soci, Cesare Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title | Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title_full | Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title_fullStr | Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title_full_unstemmed | Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title_short | Large polaron self-trapped states in three-dimensional metal-halide perovskites |
| title_sort | large polaron self trapped states in three dimensional metal halide perovskites |
| topic | Engineering::Materials::Energy materials Science::Physics::Optics and light Perovskite Polaron |
| url | https://hdl.handle.net/10356/147043 |
| work_keys_str_mv | AT wongwalterpd largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT yinjun largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT chaudarybhumika largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT chinxinyu largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT cortecchiadaniele largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT loshuzeea largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT grimsdaleandrewc largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT mohammedomarf largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT lanzaniguglielmo largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites AT socicesare largepolaronselftrappedstatesinthreedimensionalmetalhalideperovskites |