Molecular movie of ultrafast coherent rotational dynamics of OCS

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 () and Jochen Küpper ()
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Evangelos T. Karamatskos: Deutsches Elektronen-Synchrotron DESY
Sebastian Raabe: Max Born Institute
Terry Mullins: Deutsches Elektronen-Synchrotron DESY
Andrea Trabattoni: Deutsches Elektronen-Synchrotron DESY
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
Arnaud Rouzée: Max Born Institute
Jochen Küpper: Deutsches Elektronen-Synchrotron DESY

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11122-y

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