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Molecular movie of ultrafast coherent rotational dynamics of OCS

Author

Listed:
  • Evangelos T. Karamatskos

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • Sebastian Raabe

    (Max Born Institute)

  • Terry Mullins

    (Deutsches Elektronen-Synchrotron DESY)

  • Andrea Trabattoni

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • Philipp Stammer

    (Max Born Institute)

  • Gildas Goldsztejn

    (Max Born Institute)

  • Rasmus R. Johansen

    (Aarhus University)

  • Karol Długołecki

    (Deutsches Elektronen-Synchrotron DESY)

  • Henrik Stapelfeldt

    (Aarhus University)

  • Marc J. J. Vrakking

    (Max Born Institute)

  • Sebastian Trippel

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg)

  • Arnaud Rouzée

    (Max Born Institute)

  • Jochen Küpper

    (Deutsches Elektronen-Synchrotron DESY
    Universität Hamburg
    Universität Hamburg)

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.

Suggested Citation

  • Evangelos T. Karamatskos & Sebastian Raabe & Terry Mullins & Andrea Trabattoni & Philipp Stammer & Gildas Goldsztejn & Rasmus R. Johansen & Karol Długołecki & Henrik Stapelfeldt & Marc J. J. Vrakking , 2019. "Molecular movie of ultrafast coherent rotational dynamics of OCS," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11122-y
    DOI: 10.1038/s41467-019-11122-y
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    Cited by:

    1. Terry Mullins & Evangelos T. Karamatskos & Joss Wiese & Jolijn Onvlee & Arnaud Rouzée & Andrey Yachmenev & Sebastian Trippel & Jochen Küpper, 2022. "Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    2. Kiana Baumgärtner & Marvin Reuner & Christian Metzger & Dmytro Kutnyakhov & Michael Heber & Federico Pressacco & Chul-Hee Min & Thiago R. F. Peixoto & Mario Reiser & Chan Kim & Wei Lu & Roman Shayduk , 2022. "Ultrafast orbital tomography of a pentacene film using time-resolved momentum microscopy at a FEL," Nature Communications, Nature, vol. 13(1), pages 1-7, December.

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