Rotation in attosecond vibronic coherence spectroscopy for molecules
Abstract Excitation or ionization of a molecule by ultrafast laser pulses can create a superposition of electronic states, whose dynamics is influenced by the interplay of electronic coherence and nuclear motion, resulting in charge migration and possibly charge transfer. Probing the vibronic cohere...
| Main Authors: | , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2024-04-01
|
| Series: | Communications Physics |
| Online Access: | https://doi.org/10.1038/s42005-024-01607-8 |
| _version_ | 1827291540335099904 |
|---|---|
| author | Chi-Hong Yuen Chii-Dong Lin |
| author_facet | Chi-Hong Yuen Chii-Dong Lin |
| author_sort | Chi-Hong Yuen |
| collection | DOAJ |
| description | Abstract Excitation or ionization of a molecule by ultrafast laser pulses can create a superposition of electronic states, whose dynamics is influenced by the interplay of electronic coherence and nuclear motion, resulting in charge migration and possibly charge transfer. Probing the vibronic coherence is therefore vital to monitoring electronic dynamics and controlling chemical reactivity, as recently demonstrated in molecules via attosecond transient absorption spectroscopy (ATAS). However, theories supporting the interpretation of ATAS experiments neglect the effects of molecular rotation, often leading to inaccurate interpretation of experimental data. Here, we develop a comprehensive theory for ATAS of molecules encompassing the entire pump-probe process. Applying the theory to N2, we demonstrate that the emergence of coherent signals critically depends on the consideration of molecular rotation. This work contributes to close the gap between theory and ATAS experiments, paving the way for monitoring electronic motion and controlling chemical reactivity in diverse molecular systems. |
| first_indexed | 2024-04-24T12:39:49Z |
| format | Article |
| id | doaj.art-cda32108e1b2435dbc00f34009edb73d |
| institution | Directory Open Access Journal |
| issn | 2399-3650 |
| language | English |
| last_indexed | 2024-04-24T12:39:49Z |
| publishDate | 2024-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Physics |
| spelling | doaj.art-cda32108e1b2435dbc00f34009edb73d2024-04-07T11:21:00ZengNature PortfolioCommunications Physics2399-36502024-04-01711710.1038/s42005-024-01607-8Rotation in attosecond vibronic coherence spectroscopy for moleculesChi-Hong Yuen0Chii-Dong Lin1J. R. Macdonald Laboratory, Department of Physics, Kansas State UniversityJ. R. Macdonald Laboratory, Department of Physics, Kansas State UniversityAbstract Excitation or ionization of a molecule by ultrafast laser pulses can create a superposition of electronic states, whose dynamics is influenced by the interplay of electronic coherence and nuclear motion, resulting in charge migration and possibly charge transfer. Probing the vibronic coherence is therefore vital to monitoring electronic dynamics and controlling chemical reactivity, as recently demonstrated in molecules via attosecond transient absorption spectroscopy (ATAS). However, theories supporting the interpretation of ATAS experiments neglect the effects of molecular rotation, often leading to inaccurate interpretation of experimental data. Here, we develop a comprehensive theory for ATAS of molecules encompassing the entire pump-probe process. Applying the theory to N2, we demonstrate that the emergence of coherent signals critically depends on the consideration of molecular rotation. This work contributes to close the gap between theory and ATAS experiments, paving the way for monitoring electronic motion and controlling chemical reactivity in diverse molecular systems.https://doi.org/10.1038/s42005-024-01607-8 |
| spellingShingle | Chi-Hong Yuen Chii-Dong Lin Rotation in attosecond vibronic coherence spectroscopy for molecules Communications Physics |
| title | Rotation in attosecond vibronic coherence spectroscopy for molecules |
| title_full | Rotation in attosecond vibronic coherence spectroscopy for molecules |
| title_fullStr | Rotation in attosecond vibronic coherence spectroscopy for molecules |
| title_full_unstemmed | Rotation in attosecond vibronic coherence spectroscopy for molecules |
| title_short | Rotation in attosecond vibronic coherence spectroscopy for molecules |
| title_sort | rotation in attosecond vibronic coherence spectroscopy for molecules |
| url | https://doi.org/10.1038/s42005-024-01607-8 |
| work_keys_str_mv | AT chihongyuen rotationinattosecondvibroniccoherencespectroscopyformolecules AT chiidonglin rotationinattosecondvibroniccoherencespectroscopyformolecules |