Journal
NATURE COMMUNICATIONS
Volume 10, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-11122-y
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Funding
- Deutsche Forschungsgemeinschaft (DFG) [SPP1840, KU 1527/3, RO 4577/4]
- Cluster of Excellence Center for Ultrafast Imaging (CUI) of the Deutsche Forschungsgemeinschaft (DFG) [EXC 1074, 194651731]
- Cluster of Excellence Advanced Imaging of Matter (AIM) of the Deutsche Forschungsgemeinschaft (DFG) [EXC 2056, 390715994]
- European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) through the Advanced Grant DropletControl [ERC-320459]
- European Research Council under the European Union's Seventh Framework Programme (FP7/2007-2013) through the Consolidator Grant COMOTION [ERC-614507]
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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, < cos(2)theta(2D)> = 0.96 (< cos(2)theta > = 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 Schrodinger 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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