Phase Sensitive Control of Vibronic Guest-Host Interaction: Br-2 in Ar Matrix

作者：Ibrahim Heide; Hejjas Monika; Fushitani Mizuho; Schwentner Nikolaus^*

来源：Journal of Physical Chemistry A, 2009, 113(26): 7439-7450.

DOI：10.1021/jp900287m

Vibronic progressions are programmed into a pulse shaper which converts them via the inherent Fourier transformation into a train of femtosecond pulses in time domain for chromophore excitation. Double Pulse results agree with phase-sensitive wave packet superposition from a Michelson interferometer which delivers coherence times with high reliability. Spectral resolution of 1 nm and a spacing of around 4 nm within the 20 nm envelope centered at 590 nm delivers a train of seven phase-controlled 40 fs subpulses separated by 250 fs. Combs adjusted to the zero phonon lines (ZPL) and phonon sidebands (PSB) of the B state vibronic progression are reproduced in the chromophore for a coherent subpulse accumulation. B state ZPL wave packet dynamics dominates in pump-probe spectra due to its coherence despite an overwhelming but incoherent A state contribution in absorption. PSB comb accumulation is also phase sensitive and demonstrates coherence within several 100 matrix degrees of freedom in the vicinity.

• 出版日期2009-7-2