Molecular movie of ultrafast coherent rotational dynamics of OCS

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Autorschaft

  • Evangelos T. Karamatskos
  • Sebastian Raabe
  • Terry Mullins
  • Andrea Trabattoni
  • Philipp Stammer
  • Gildas Goldsztejn
  • Rasmus R. Johansen
  • Karol Długołecki
  • Henrik Stapelfeldt
  • Marc J.J. Vrakking
  • Sebastian Trippel
  • Arnaud Rouzée
  • Jochen Küpper

Externe Organisationen

  • Deutsches Elektronen-Synchrotron (DESY)
  • Universität Hamburg
  • Max-Born-Institut für Nichtlineare Optik und Kurzzeitspektroskopie (MBI)
  • Center for Free-Electron Laser Science (CFEL)
  • Aarhus University
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Aufsatznummer3364
FachzeitschriftNature Communications
Jahrgang10
Ausgabenummer1
Frühes Online-Datum29 Juli 2019
PublikationsstatusVeröffentlicht - 1 Dez. 2019
Extern publiziertJa

Abstract

Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.

ASJC Scopus Sachgebiete

Zitieren

Molecular movie of ultrafast coherent rotational dynamics of OCS. / Karamatskos, Evangelos T.; Raabe, Sebastian; Mullins, Terry et al.
in: Nature Communications, Jahrgang 10, Nr. 1, 3364, 01.12.2019.

Publikation: Beitrag in Fachzeitschrift › Artikel › Forschung › Peer-Review

Karamatskos, ET, Raabe, S, Mullins, T, Trabattoni, A, Stammer, P, Goldsztejn, G, Johansen, RR, Długołecki, K, Stapelfeldt, H, Vrakking, MJJ, Trippel, S, Rouzée, A & Küpper, J 2019, 'Molecular movie of ultrafast coherent rotational dynamics of OCS', Nature Communications, Jg. 10, Nr. 1, 3364. https://doi.org/10.1038/s41467-019-11122-y
Karamatskos, E. T., Raabe, S., Mullins, T., Trabattoni, A., Stammer, P., Goldsztejn, G., Johansen, R. R., Długołecki, K., Stapelfeldt, H., Vrakking, M. J. J., Trippel, S., Rouzée, A., & Küpper, J. (2019). Molecular movie of ultrafast coherent rotational dynamics of OCS. Nature Communications, 10(1), Artikel 3364. https://doi.org/10.1038/s41467-019-11122-y
Karamatskos ET, Raabe S, Mullins T, Trabattoni A, Stammer P, Goldsztejn G et al. Molecular movie of ultrafast coherent rotational dynamics of OCS. Nature Communications. 2019 Dez 1;10(1):3364. Epub 2019 Jul 29. doi: 10.1038/s41467-019-11122-y
Karamatskos, Evangelos T. ; Raabe, Sebastian ; Mullins, Terry et al. / Molecular movie of ultrafast coherent rotational dynamics of OCS. in: Nature Communications. 2019 ; Jahrgang 10, Nr. 1.
Download
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abstract = "Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schr{\"o}dinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.",
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T1 - Molecular movie of ultrafast coherent rotational dynamics of OCS

AU - Karamatskos, Evangelos T.

AU - Raabe, Sebastian

AU - Mullins, Terry

AU - Trabattoni, Andrea

AU - Stammer, Philipp

AU - Goldsztejn, Gildas

AU - Johansen, Rasmus R.

AU - Długołecki, Karol

AU - Stapelfeldt, Henrik

AU - Vrakking, Marc J.J.

AU - Trippel, Sebastian

AU - Rouzée, Arnaud

AU - Küpper, Jochen

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N2 - Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.

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