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Probing nonadiabatic dynamics with attosecond pulse trains and soft x-ray Raman spectroscopy
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-8852-1016
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0003-3305-9140
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-2288-2548
Number of Authors: 32022 (English)In: Structural Dynamics, E-ISSN 2329-7778, Vol. 9, no 3, article id 034101Article in journal (Refereed) Published
Abstract [en]

Linear off-resonant x-ray Raman techniques are capable of detecting the ultrafast electronic coherences generated when a photoexcited wave packet passes through a conical intersection. A hybrid femtosecond or attosecond probe pulse is employed to excite the system and stimulate the emission of the signal photon, where both fields are components of a hybrid pulse scheme. In this paper, we investigate how attosecond pulse trains, as provided by high-harmonic generation processes, perform as probe pulses in the framework of this spectroscopic technique, instead of single Gaussian pulses. We explore different combination schemes for the probe pulse as well as the impact of parameters of the pulse trains on the signals. Furthermore, we show how Raman selection rules and symmetry consideration affect the spectroscopic signal, and we discuss the importance of vibrational contributions to the overall signal. We use two different model systems, representing molecules of different symmetries, and quantum dynamics simulations to study the difference in the spectra. The results suggest that such pulse trains are well suited to capture the key features associated with the electronic coherence.

Place, publisher, year, edition, pages
2022. Vol. 9, no 3, article id 034101
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:su:diva-207427DOI: 10.1063/4.0000146ISI: 000816955900001PubMedID: 35774244Scopus ID: 2-s2.0-85133653483OAI: oai:DiVA.org:su-207427DiVA, id: diva2:1684608
Available from: 2022-07-27 Created: 2022-07-27 Last updated: 2023-05-09Bibliographically approved
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2. Probing Nonadiabatic Dynamics with Soft X-ray Raman Spectroscopy
Open this publication in new window or tab >>Probing Nonadiabatic Dynamics with Soft X-ray Raman Spectroscopy
2023 (English)Licentiate thesis, comprehensive summary (Other academic)
Place, publisher, year, edition, pages
Stockholm University, 2023
National Category
Atom and Molecular Physics and Optics
Research subject
Chemical Physics
Identifiers
urn:nbn:se:su:diva-217036 (URN)
Presentation
2023-04-04, 13:00 (English)
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Supervisors
Available from: 2023-05-09 Created: 2023-05-09 Last updated: 2023-05-09Bibliographically approved

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Restaino, LorenzoJadoun, DeependraKowalewski, Markus

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