Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $\mathrm{XUV}$-$\mathrm{IR}$ regime

Lee, J. W.  L.; Tikhonov, D. S.; Chopra, P.; Maclot, S.; Steber, A. L.; Gruet, S.; Allum, F.; Boll, R.; Cheng, X.; Düsterer, S.; Erk, B.; Garg, D.; He, L.; Heathcote, D.; Johny, M.; Kazemi, M. M.; Köckert, H.; Lahl, J.; Lemmens, A. K.; Loru, D.; Mason, R.; Müller, E.; Mullins, T.; Olshin, P.; Passow, C.; Peschel, J.; Ramm, D.; Rompotis, D.; Schirmel, N.; Trippel, S.; Wiese, J.; Ziaee, F.; Bari, S.; Burt, M.; Küpper, J.; Rijs, A. M.; Rolles, D.; Techert, S.; Eng-Johnsson, P.; Brouard, M.; Vallance, C.; Manschwetus, B.; Schnell, M.

doi:10.1038/s41467-021-26193-z

Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $$\mathrm{XUV}$$-$$\mathrm{IR}$$ regime

Journal Article · Wed Oct 20 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-26193-z· OSTI ID:1904604

^[1]; ^[2]; Chopra, P. ^[2]; ^[3]; ^[4]; Gruet, S. ^[5]; Allum, F. ^[6]; ^[7]; Cheng, X. ^[5]; ^[5]; ^[5]; Garg, D. ^[8]; ^[9]; ^[6]; Johny, M. ^[10]; Kazemi, M. M. ^[5]; ^[6]; Lahl, J. ^[11]; Lemmens, A. K. ^[12]; Loru, D. ^[2] more »

Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); University of Oxford (United Kingdom); Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); Christian-Albrechts University, Kiel (Germany)
Lund University (Sweden); University of Gothenburg (Sweden)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); Christian-Albrechts University, Kiel (Germany); University of Hamburg (Germany)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany)
University of Oxford (United Kingdom)
European X-ray Free-Electron Laser (XFEL), Hamburg (Germany); European XFEL, Schenefeld (Germany)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); University of Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Univ. of Hamburg (Germany); Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany)
Lund University (Sweden)
Radboud University, Nijmegen (Netherlands); University of Amsterdam (Netherlands)
Saint Petersburg State Universtiy, Saint Petersburg (Russia)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); European XFEL, Schenefeld (Germany)
University of Hamburg (Germany); Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany)
Kansas State University, Manhattan, KS (United States)
Radboud University, Nijmegen (Netherlands); Vrije University, Amsterdam (Netherlands)
Deutsches Elektronen-Synchrotron DESY, Hamburg (Germany); Georg-August-University, Gottingen (Germany)

Polycyclic aromatic hydrocarbons (PAHs) play an important role in interstellar chemistry and are subject to high energy photons that can induce excitation, ionization, and fragmentation. Previous studies have demonstrated electronic relaxation of parent PAH monocations over 10–100 femtoseconds as a result of beyond-Born-Oppenheimer coupling between the electronic and nuclear dynamics. Here, we investigate three PAH molecules: fluorene, phenanthrene, and pyrene, using ultrafast XUV and IR laser pulses. Simultaneous measurements of the ion yields, ion momenta, and electron momenta as a function of laser pulse delay allow a detailed insight into the various molecular processes. We report relaxation times for the electronically excited PAH^*, PAH^+*and PAH^2+*states, and show the time-dependent conversion between fragmentation pathways. Additionally, using recoil-frame covariance analysis between ion images, we demonstrate that the dissociation of the PAH²⁺ions favors reaction pathways involving two-body breakup and/or loss of neutral fragments totaling an even number of carbon atoms.

View Accepted Manuscript (DOE)

Research Organization:: Kansas State University, Manhattan, KS (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); HORIZON 2020; Max Planck Society; Federal Ministry of Education and Research ( BMBF ); Marie Skłodowska-Curie Grant; German Research Foundation (DFG); Netherlands Organization for Scientific Research (NWO); Swedish Research Council; Swedish Foundation for Strategic Research; Engineering and Physical Sciences Research Council (EPSRC); National Science Foundation (NSF); Helmholtz Initiative and Networking Fund; Deutsches Elektronen-Synchrotron DESY

Grant/Contract Number:: FG02-86ER13491

OSTI ID:: 1904604

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Time-resolved relaxation and fragmentation of polycyclic aromatic hydrocarbons investigated in the ultrafast $$\mathrm{XUV}$$-$$\mathrm{IR}$$ regime

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