Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime
Time-domain investigations of the nonadiabatic coupling between electronic and vibrational degrees of freedom have focused primarily on the formation of electronic superpositions induced by atomic motion. The effect of electronic nonstationary-state dynamics on atomic motion remains unexplored. H...
| Main Authors: | , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2014
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| Online Access: | https://hdl.handle.net/10356/101655 http://hdl.handle.net/10220/18680 |
| _version_ | 1826113290515775488 |
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| author | Nie, Zhaogang. Long, Run. Li, Jialin. Zheng, Yi Ying. Prezhdo, Oleg V. Loh, Zhi-Heng. |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Nie, Zhaogang. Long, Run. Li, Jialin. Zheng, Yi Ying. Prezhdo, Oleg V. Loh, Zhi-Heng. |
| author_sort | Nie, Zhaogang. |
| collection | NTU |
| description | Time-domain investigations of the nonadiabatic coupling between
electronic and vibrational degrees of freedom have focused primarily on the formation
of electronic superpositions induced by atomic motion. The effect of electronic
nonstationary-state dynamics on atomic motion remains unexplored. Here, phasecoherent
excitation of the two lowest electronic transitions in semiconducting singlewalled
carbon nanotubes by broadband <5-fs pulses directly triggers coherent exciton
motion along the axis of the nanotubes. Optical pump−probe spectroscopy with sub-10-fs
time resolution reveals that exciton motion selectively excites the high-frequency G mode
coherent phonon, in good agreement with results obtained from time-domain ab initio
simulations. This observed phenomenon arises from the direct modulation of the C−C
interatomic potential by coherent exciton motion on a time scale that is commensurate
with atomic motion. Our results suggest the possibility of employing light-field
manipulation of electron densities in the non-Born−Oppenheimer regime to initiate
selective atomic motion. |
| first_indexed | 2024-10-01T03:21:06Z |
| format | Journal Article |
| id | ntu-10356/101655 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T03:21:06Z |
| publishDate | 2014 |
| record_format | dspace |
| spelling | ntu-10356/1016552023-02-28T19:42:48Z Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime Nie, Zhaogang. Long, Run. Li, Jialin. Zheng, Yi Ying. Prezhdo, Oleg V. Loh, Zhi-Heng. School of Physical and Mathematical Sciences DRNTU::Science::Chemistry::Physical chemistry Time-domain investigations of the nonadiabatic coupling between electronic and vibrational degrees of freedom have focused primarily on the formation of electronic superpositions induced by atomic motion. The effect of electronic nonstationary-state dynamics on atomic motion remains unexplored. Here, phasecoherent excitation of the two lowest electronic transitions in semiconducting singlewalled carbon nanotubes by broadband <5-fs pulses directly triggers coherent exciton motion along the axis of the nanotubes. Optical pump−probe spectroscopy with sub-10-fs time resolution reveals that exciton motion selectively excites the high-frequency G mode coherent phonon, in good agreement with results obtained from time-domain ab initio simulations. This observed phenomenon arises from the direct modulation of the C−C interatomic potential by coherent exciton motion on a time scale that is commensurate with atomic motion. Our results suggest the possibility of employing light-field manipulation of electron densities in the non-Born−Oppenheimer regime to initiate selective atomic motion. ASTAR (Agency for Sci., Tech. and Research, S’pore) Accepted version 2014-01-22T04:15:41Z 2019-12-06T20:42:20Z 2014-01-22T04:15:41Z 2019-12-06T20:42:20Z 2013 2013 Journal Article Nie, Z., Long, R., Li, J., Zheng, Y. Y., Prezhdo, O. V., & Loh, Z. H. (2013). Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime. The journal of physical chemistry letters, 4(24), 4260-4266. 1948-7185 https://hdl.handle.net/10356/101655 http://hdl.handle.net/10220/18680 10.1021/jz401945m 179870 en The journal of physical chemistry letters © 2013 American Chemical Society. This is the author created version of a work that has been peer reviewed and accepted for publication by The Journal of Physical Chemistry Letters, American Chemical Society. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1021/jz401945m]. 7 p. application/pdf application/pdf |
| spellingShingle | DRNTU::Science::Chemistry::Physical chemistry Nie, Zhaogang. Long, Run. Li, Jialin. Zheng, Yi Ying. Prezhdo, Oleg V. Loh, Zhi-Heng. Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title | Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title_full | Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title_fullStr | Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title_full_unstemmed | Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title_short | Selective excitation of atomic-scale dynamics by coherent exciton motion in the non-born–Oppenheimer regime |
| title_sort | selective excitation of atomic scale dynamics by coherent exciton motion in the non born oppenheimer regime |
| topic | DRNTU::Science::Chemistry::Physical chemistry |
| url | https://hdl.handle.net/10356/101655 http://hdl.handle.net/10220/18680 |
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