High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration
High-harmonic spectroscopy is an all-optical technique with inherent attosecond temporal resolution that has been successfully employed to reconstruct charge migration, electron-tunneling dynamics, and conical-intersection dynamics. Here, we demonstrate the extension of two key components of high-ha...
| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
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AIP Publishing LLC and ACA
2024-01-01
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| Series: | Structural Dynamics |
| Online Access: | http://dx.doi.org/10.1063/4.0000227 |
| _version_ | 1797278300852191232 |
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| author | Andres Tehlar Jakob T. Casanova Andrey Dnestryan Frank Jensen Lars Bojer Madsen Oleg I. Tolstikhin Hans Jakob Wörner |
| author_facet | Andres Tehlar Jakob T. Casanova Andrey Dnestryan Frank Jensen Lars Bojer Madsen Oleg I. Tolstikhin Hans Jakob Wörner |
| author_sort | Andres Tehlar |
| collection | DOAJ |
| description | High-harmonic spectroscopy is an all-optical technique with inherent attosecond temporal resolution that has been successfully employed to reconstruct charge migration, electron-tunneling dynamics, and conical-intersection dynamics. Here, we demonstrate the extension of two key components of high-harmonic spectroscopy, i.e., impulsive alignment and measurements with multiple driving wavelengths to 1,3-cyclohexadiene and benzene. In the case of 1,3-cyclohexadiene, we find that the temporal sequence of maximal and minimal emitted high-harmonic intensities as a function of the delay between the alignment and probe pulses inverts between 25 and 30 eV and again between 35 and 40 eV when an 800-nm driver is used, but no inversions are observed with a 1420-nm driver. This observation is explained by the wavelength-dependent interference of emission from multiple molecular orbitals (HOMO to HOMO-3), as demonstrated by calculations based on the weak-field asymptotic theory and accurate photorecombination matrix elements. These results indicate that attosecond charge migration takes place in the 1,3-cyclohexadiene cation and can potentially be reconstructed with the help of additional measurements. Our experiments also demonstrate a pathway toward studying photochemical reactions in the molecular frame of 1,3-cyclohexadiene. |
| first_indexed | 2024-03-07T16:01:21Z |
| format | Article |
| id | doaj.art-af3b6284354f41b799cbb83e1e85f55a |
| institution | Directory Open Access Journal |
| issn | 2329-7778 |
| language | English |
| last_indexed | 2024-03-07T16:01:21Z |
| publishDate | 2024-01-01 |
| publisher | AIP Publishing LLC and ACA |
| record_format | Article |
| series | Structural Dynamics |
| spelling | doaj.art-af3b6284354f41b799cbb83e1e85f55a2024-03-04T20:40:25ZengAIP Publishing LLC and ACAStructural Dynamics2329-77782024-01-01111014304014304-1010.1063/4.0000227High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migrationAndres Tehlar0Jakob T. Casanova1Andrey Dnestryan2Frank Jensen3Lars Bojer Madsen4Oleg I. Tolstikhin5Hans Jakob Wörner6 Laboratory of Physical Chemistry, ETH Zürich, 8093 Zürich, Switzerland Laboratory of Physical Chemistry, ETH Zürich, 8093 Zürich, Switzerland Moscow Institute of Physics and Technology, Dolgoprudny 141700, Russia Department of Chemistry, Aarhus University, 8000 Aarhus C, Denmark Department of Physics and Astronomy, Aarhus University, 8000 Aarhus C, Denmark Moscow Institute of Physics and Technology, Dolgoprudny 141700, Russia Laboratory of Physical Chemistry, ETH Zürich, 8093 Zürich, SwitzerlandHigh-harmonic spectroscopy is an all-optical technique with inherent attosecond temporal resolution that has been successfully employed to reconstruct charge migration, electron-tunneling dynamics, and conical-intersection dynamics. Here, we demonstrate the extension of two key components of high-harmonic spectroscopy, i.e., impulsive alignment and measurements with multiple driving wavelengths to 1,3-cyclohexadiene and benzene. In the case of 1,3-cyclohexadiene, we find that the temporal sequence of maximal and minimal emitted high-harmonic intensities as a function of the delay between the alignment and probe pulses inverts between 25 and 30 eV and again between 35 and 40 eV when an 800-nm driver is used, but no inversions are observed with a 1420-nm driver. This observation is explained by the wavelength-dependent interference of emission from multiple molecular orbitals (HOMO to HOMO-3), as demonstrated by calculations based on the weak-field asymptotic theory and accurate photorecombination matrix elements. These results indicate that attosecond charge migration takes place in the 1,3-cyclohexadiene cation and can potentially be reconstructed with the help of additional measurements. Our experiments also demonstrate a pathway toward studying photochemical reactions in the molecular frame of 1,3-cyclohexadiene.http://dx.doi.org/10.1063/4.0000227 |
| spellingShingle | Andres Tehlar Jakob T. Casanova Andrey Dnestryan Frank Jensen Lars Bojer Madsen Oleg I. Tolstikhin Hans Jakob Wörner High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration Structural Dynamics |
| title | High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration |
| title_full | High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration |
| title_fullStr | High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration |
| title_full_unstemmed | High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration |
| title_short | High-harmonic spectroscopy of impulsively aligned 1,3-cyclohexadiene: Signatures of attosecond charge migration |
| title_sort | high harmonic spectroscopy of impulsively aligned 1 3 cyclohexadiene signatures of attosecond charge migration |
| url | http://dx.doi.org/10.1063/4.0000227 |
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