Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy
Halide perovskites are promising materials for development in hot carrier (HC) solar cells, where the excess energy of above-bandgap photons is harvested before being wasted as heat to enhance device efficiency. Presently, HC separation and transfer processes at higher-energy states remain poorly un...
| Main Authors: | , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
| Published: |
2020
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| Online Access: | https://hdl.handle.net/10356/143937 |
| _version_ | 1811692757652078592 |
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| author | Lim, Swee Sien Giovanni, David Zhang, Qiannan Solanki, Ankur Nur Fadilah Jamaludin Lim, Melvin Jia Wei Mathews, Nripan Mhaisalkar, Subodh Pshenichnikov, Maxim S. Sum, Tze Chien |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Lim, Swee Sien Giovanni, David Zhang, Qiannan Solanki, Ankur Nur Fadilah Jamaludin Lim, Melvin Jia Wei Mathews, Nripan Mhaisalkar, Subodh Pshenichnikov, Maxim S. Sum, Tze Chien |
| author_sort | Lim, Swee Sien |
| collection | NTU |
| description | Halide perovskites are promising materials for development in hot carrier (HC) solar cells, where the excess energy of above-bandgap photons is harvested before being wasted as heat to enhance device efficiency. Presently, HC separation and transfer processes at higher-energy states remain poorly understood. Here, we investigate the excited state dynamics in CH3NH3PbI3 using pump-push-probe spectroscopy. It has its intrinsic advantages for studying these dynamics over conventional transient spectroscopy, albeit complementary to one another. By exploiting the broad excited-state absorption characteristics, our findings reveal the transfer of HCs from these higher-energy states into bathophenanthroline (bphen), an energy selective organic acceptor far above perovskite's band edges. Complete HC extraction is realized only after overcoming the interfacial barrier formed at the heterojunction, estimated to be between 1.01 and 1.08 eV above bphen's lowest unoccupied molecular orbital level. The insights gained here are essential for the development of a new class of optoelectronics. |
| first_indexed | 2024-10-01T06:40:52Z |
| format | Journal Article |
| id | ntu-10356/143937 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:40:52Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1439372023-02-28T19:52:55Z Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy Lim, Swee Sien Giovanni, David Zhang, Qiannan Solanki, Ankur Nur Fadilah Jamaludin Lim, Melvin Jia Wei Mathews, Nripan Mhaisalkar, Subodh Pshenichnikov, Maxim S. Sum, Tze Chien School of Materials Science and Engineering School of Physical and Mathematical Sciences Interdisciplinary Graduate School (IGS) Energy Research Institute @ NTU (ERI@N) Science::Physics Hot Carrier Spectroscopy Halide perovskites are promising materials for development in hot carrier (HC) solar cells, where the excess energy of above-bandgap photons is harvested before being wasted as heat to enhance device efficiency. Presently, HC separation and transfer processes at higher-energy states remain poorly understood. Here, we investigate the excited state dynamics in CH3NH3PbI3 using pump-push-probe spectroscopy. It has its intrinsic advantages for studying these dynamics over conventional transient spectroscopy, albeit complementary to one another. By exploiting the broad excited-state absorption characteristics, our findings reveal the transfer of HCs from these higher-energy states into bathophenanthroline (bphen), an energy selective organic acceptor far above perovskite's band edges. Complete HC extraction is realized only after overcoming the interfacial barrier formed at the heterojunction, estimated to be between 1.01 and 1.08 eV above bphen's lowest unoccupied molecular orbital level. The insights gained here are essential for the development of a new class of optoelectronics. Ministry of Education (MOE) National Research Foundation (NRF) Published version Financial support from the Nanyang Technological University start-up grant M4080514, the JSPS-NTU Joint Research Project M4082176, the Ministry of Education AcRF Tier 1 grant RG173/16 and Tier 2 grants MOE2015-T2-2-015, MOE2016-T2-1-034, and MOE2017-T2-2-002, the U.S. Office of Naval Research (ONRGNICOPN62909-17-1-2155), and the Singapore National Research Foundation (Programs NRF-CRP14-2014-03, NRF2018-ITC001-001, and NRF-NRFI-2018-04) is acknowledged. 2020-10-02T02:16:59Z 2020-10-02T02:16:59Z 2019 Journal Article Lim, S. S., Giovanni, D., Zhang, Q., Solanki, A., Nur Fadilah Jamaludin, Lim, M. J. W., ... Sum, T. C. (2019). Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy. Science Advances, 5(11), eaax3620-. doi:10.1126/sciadv.aax3620 2375-2548 https://hdl.handle.net/10356/143937 10.1126/sciadv.aax3620 31763450 11 5 eaax3620 en Science Advances https://doi.org/10.21979/N9/RZUNHG © 2019 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S.Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). application/pdf |
| spellingShingle | Science::Physics Hot Carrier Spectroscopy Lim, Swee Sien Giovanni, David Zhang, Qiannan Solanki, Ankur Nur Fadilah Jamaludin Lim, Melvin Jia Wei Mathews, Nripan Mhaisalkar, Subodh Pshenichnikov, Maxim S. Sum, Tze Chien Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title | Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title_full | Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title_fullStr | Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title_full_unstemmed | Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title_short | Hot carrier extraction in CH3NH3PbI3 unveiled by pump-push-probe spectroscopy |
| title_sort | hot carrier extraction in ch3nh3pbi3 unveiled by pump push probe spectroscopy |
| topic | Science::Physics Hot Carrier Spectroscopy |
| url | https://hdl.handle.net/10356/143937 |
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