Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations
We present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H _2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features ar...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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IOP Publishing
2015-01-01
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| Series: | New Journal of Physics |
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| Online Access: | https://doi.org/10.1088/1367-2630/17/5/053011 |
| _version_ | 1797751263807406080 |
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| author | Lukas Medišauskas Felipe Morales Alicia Palacios Alberto González-Castrillo Lev Plimak Olga Smirnova Fernando Martín Misha Yu Ivanov |
| author_facet | Lukas Medišauskas Felipe Morales Alicia Palacios Alberto González-Castrillo Lev Plimak Olga Smirnova Fernando Martín Misha Yu Ivanov |
| author_sort | Lukas Medišauskas |
| collection | DOAJ |
| description | We present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H _2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals. |
| first_indexed | 2024-03-12T16:44:57Z |
| format | Article |
| id | doaj.art-da262a07b08e4dfbaabc1564e2152201 |
| institution | Directory Open Access Journal |
| issn | 1367-2630 |
| language | English |
| last_indexed | 2024-03-12T16:44:57Z |
| publishDate | 2015-01-01 |
| publisher | IOP Publishing |
| record_format | Article |
| series | New Journal of Physics |
| spelling | doaj.art-da262a07b08e4dfbaabc1564e21522012023-08-08T14:17:26ZengIOP PublishingNew Journal of Physics1367-26302015-01-0117505301110.1088/1367-2630/17/5/053011Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculationsLukas Medišauskas0Felipe Morales1Alicia Palacios2Alberto González-Castrillo3Lev Plimak4Olga Smirnova5Fernando Martín6Misha Yu Ivanov7Department of Physics, Imperial College London , South Kensington Campus, SW7 2AZ London, UK; Max-Born-Institut , Max-Born Strasse 2 A, D-12489 Berlin, GermanyMax-Born-Institut , Max-Born Strasse 2 A, D-12489 Berlin, GermanyDepartamento de Química, Universidad Autánoma de Madrid , 28049 Madrid, SpainDepartamento de Química, Universidad Autánoma de Madrid , 28049 Madrid, SpainMax-Born-Institut , Max-Born Strasse 2 A, D-12489 Berlin, GermanyMax-Born-Institut , Max-Born Strasse 2 A, D-12489 Berlin, GermanyDepartamento de Química, Universidad Autánoma de Madrid , 28049 Madrid, SpainDepartment of Physics, Imperial College London , South Kensington Campus, SW7 2AZ London, UK; Max-Born-Institut , Max-Born Strasse 2 A, D-12489 Berlin, Germany; Department of Physics, Humboldt University , Newtonstr. 15, D-12489 Berlin, GermanyWe present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H _2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals.https://doi.org/10.1088/1367-2630/17/5/053011attosecond dynamicstime-dependent WKBsemiclassicalautoionization |
| spellingShingle | Lukas Medišauskas Felipe Morales Alicia Palacios Alberto González-Castrillo Lev Plimak Olga Smirnova Fernando Martín Misha Yu Ivanov Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations New Journal of Physics attosecond dynamics time-dependent WKB semiclassical autoionization |
| title | Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations |
| title_full | Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations |
| title_fullStr | Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations |
| title_full_unstemmed | Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations |
| title_short | Signatures of attosecond electronic–nuclear dynamics in the one-photon ionization of molecular hydrogen: analytical model versus ab initio calculations |
| title_sort | signatures of attosecond electronic nuclear dynamics in the one photon ionization of molecular hydrogen analytical model versus ab initio calculations |
| topic | attosecond dynamics time-dependent WKB semiclassical autoionization |
| url | https://doi.org/10.1088/1367-2630/17/5/053011 |
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