Time-dependent photoionization of azulene: Competition between ionization and relaxation in highly excited states
| Autor: | Ivan Anton Garcia, Iain Wilkinson, Benjamin J. Whitaker, Béatrice Chatel, Bertrand Girard, Giorgio Turri, Valérie Blanchet, Kevin Raffael |
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| Přispěvatelé: | Femto (LCAR), Laboratoire Collisions Agrégats Réactivité (LCAR), Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS), School of Chemistry [Leeds], University of Leeds, ANR-06-BLAN-0004,cocomouv,Shaped tunable ultraviolet femtosecond source: Application to coherent control in atoms and molecules.(2006), Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Institut National des Sciences Appliquées (INSA)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut National des Sciences Appliquées - Toulouse (INSA Toulouse), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées |
| Rok vydání: | 2008 |
| Předmět: |
azulene
time-resolved photoelectron spectroscopy Photoemission spectroscopy femtochemistry Population General Physics and Astronomy FOS: Physical sciences Photoionization 010402 general chemistry 01 natural sciences symbols.namesake chemistry.chemical_compound Physics - Chemical Physics Ionization 0103 physical sciences Physics::Atomic and Molecular Clusters Physics::Atomic Physics Physical and Theoretical Chemistry education Physics Chemical Physics (physics.chem-ph) education.field_of_study 010304 chemical physics Azulene 0104 chemical sciences Vibronic coupling chemistry Excited state Rydberg formula symbols [PHYS.PHYS.PHYS-CHEM-PH]Physics [physics]/Physics [physics]/Chemical Physics [physics.chem-ph] Atomic physics |
| Zdroj: | Journal of Chemical Physics Journal of Chemical Physics, American Institute of Physics, 2008, 128 (16), pp.164318. ⟨10.1063/1.2913167⟩ |
| ISSN: | 0021-9606 1089-7690 |
| DOI: | 10.48550/arxiv.0806.3400 |
| Popis: | Pump-probe photoionization has been used to map the relaxation processes taking place from highly vibrationally excited levels of the S(2) state of azulene, populated directly or via internal conversion from the S(4) state. Photoelectron spectra obtained by 1+2(') two-color time-resolved photoelectron imaging are invariant (apart from in intensity) to the pump-probe time delay and to the pump wavelength. This reveals a photoionization process which is driven by an unstable electronic state (e.g., doubly excited state) lying below the ionization potential. This state is postulated to be populated by a probe transition from S(2) and to rapidly relax via an Auger-like process onto highly vibrationally excited Rydberg states. This accounts for the time invariance of the photoelectron spectrum. The intensity of the photoelectron spectrum is proportional to the population in S(2). An exponential energy gap law is used to describe the internal conversion rate from S(2) to S(0). The vibronic coupling strength is found to be larger than 60+/-5 microeV. |
| Databáze: | OpenAIRE |
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