Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene.
Coupling of nuclear and electronic degrees of freedom mediates energy flow in molecules after optical excitation. The associated coherent dynamics in polyatomic systems, however, remain experimentally unexplored. Here, we combined transient absorption spectroscopy with electronic population control...
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| Format: | Journal article |
| Language: | English |
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American Physical Society
2014
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| _version_ | 1797062949013028864 |
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| author | Liebel, M Schnedermann, C Kukura, P |
| author_facet | Liebel, M Schnedermann, C Kukura, P |
| author_sort | Liebel, M |
| collection | OXFORD |
| description | Coupling of nuclear and electronic degrees of freedom mediates energy flow in molecules after optical excitation. The associated coherent dynamics in polyatomic systems, however, remain experimentally unexplored. Here, we combined transient absorption spectroscopy with electronic population control to reveal nuclear wave packet dynamics during the S2 → S1 internal conversion in β-carotene. We show that passage through a conical intersection is vibrationally coherent and thereby provides direct feedback on the role of different vibrational coordinates in the breakdown of the Born-Oppenheimer approximation. |
| first_indexed | 2024-03-06T20:52:50Z |
| format | Journal article |
| id | oxford-uuid:382fb613-5cc7-4a90-99b3-62520919490c |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-06T20:52:50Z |
| publishDate | 2014 |
| publisher | American Physical Society |
| record_format | dspace |
| spelling | oxford-uuid:382fb613-5cc7-4a90-99b3-62520919490c2022-03-26T13:48:28ZVibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:382fb613-5cc7-4a90-99b3-62520919490cEnglishSymplectic Elements at OxfordAmerican Physical Society2014Liebel, MSchnedermann, CKukura, PCoupling of nuclear and electronic degrees of freedom mediates energy flow in molecules after optical excitation. The associated coherent dynamics in polyatomic systems, however, remain experimentally unexplored. Here, we combined transient absorption spectroscopy with electronic population control to reveal nuclear wave packet dynamics during the S2 → S1 internal conversion in β-carotene. We show that passage through a conical intersection is vibrationally coherent and thereby provides direct feedback on the role of different vibrational coordinates in the breakdown of the Born-Oppenheimer approximation. |
| spellingShingle | Liebel, M Schnedermann, C Kukura, P Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title | Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title_full | Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title_fullStr | Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title_full_unstemmed | Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title_short | Vibrationally coherent crossing and coupling of electronic states during internal conversion in β-carotene. |
| title_sort | vibrationally coherent crossing and coupling of electronic states during internal conversion in β carotene |
| work_keys_str_mv | AT liebelm vibrationallycoherentcrossingandcouplingofelectronicstatesduringinternalconversioninbcarotene AT schnedermannc vibrationallycoherentcrossingandcouplingofelectronicstatesduringinternalconversioninbcarotene AT kukurap vibrationallycoherentcrossingandcouplingofelectronicstatesduringinternalconversioninbcarotene |