Molecular quantum control landscapes in von Neumann time-frequency phase space

Recently we introduced the von Neumann representation as a joint time-frequency description for femtosecond laser pulses and suggested its use as a basis for pulse shaping experiments. Here we use the von Neumann basis to represent multidimensional molecular control landscapes, providing insight int...

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Veröffentlicht in:The Journal of chemical physics 2010-10, Vol.133 (16), p.164510-164510-8
Hauptverfasser: Ruetzel, Stefan, Stolzenberger, Christoph, Fechner, Susanne, Dimler, Frank, Brixner, Tobias, Tannor, David J.
Format: Artikel
Sprache:eng
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Zusammenfassung:Recently we introduced the von Neumann representation as a joint time-frequency description for femtosecond laser pulses and suggested its use as a basis for pulse shaping experiments. Here we use the von Neumann basis to represent multidimensional molecular control landscapes, providing insight into the molecular dynamics. We present three kinds of time-frequency phase space scanning procedures based on the von Neumann formalism: variation of intensity, time-frequency phase space position, and/or the relative phase of single subpulses. The shaped pulses produced are characterized via Fourier-transform spectral interferometry. Quantum control is demonstrated on the laser dye IR140 elucidating a time-frequency pump-dump mechanism.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.3495950