Molecular movie of ultrafast coherent rotational dynamics of OCS

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaperJournal articleResearchpeer-review

  • Evangelos T. Karamatskos, DESY Photon Science, Universitat Hamburg
  • ,
  • Sebastian Raabe, Max Born Institute, 12489 Berlin
  • ,
  • Terry Mullins, DESY Photon Science
  • ,
  • Andrea Trabattoni, DESY Photon Science, Universitat Hamburg
  • ,
  • Philipp Stammer, Max Born Institute, 12489 Berlin
  • ,
  • Gildas Goldsztejn, Max Born Institute, 12489 Berlin
  • ,
  • Rasmus R. Johansen
  • ,
  • Karol Długołecki, DESY Photon Science
  • ,
  • Henrik Stapelfeldt
  • Marc J.J. Vrakking, Max Born Institute, 12489 Berlin
  • ,
  • Sebastian Trippel, DESY Photon Science, Universitat Hamburg
  • ,
  • Arnaud Rouzée, Max Born Institute, 12489 Berlin
  • ,
  • Jochen Küpper, DESY Photon Science, Universitat Hamburg

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.

Original languageEnglish
Article number3364
JournalNature Communications
Volume10
Issue1
ISSN2041-1723
DOIs
Publication statusPublished - Dec 2019

See relations at Aarhus University Citationformats

ID: 161135379