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Issue 17, 2005
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Pump–probe spectroscopy with phase-locked pulses in the condensed phase: decoherence and control of vibrational wavepackets

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Abstract

Electronic and vibrational coherences of Cl2 embedded in solid Ar are investigated by exciting to the B state with a phase-locked pulse pair from an unbalanced Michelson interferometer, where the chirp difference matches the B state anharmonicity. Recording the A′ → X fluorescence after relaxation is compared to probing to charge transfer states by a third pulse. The three-pulse experiment delivers more details on the decoherence processes. The signal modulation due to phase tuning up to the third vibrational round-trip time indicates that the electronic coherence in the B ← X transition is preserved for more than 660 fs in the solid Ar environment where many body electronic interactions take place. Vibrational coherence lasts longer than 3 ps according to the observed half revival of the wavepacket. Control of the coupling between wavepacket motion and lattice oscillation is demonstrated by tuning the relative phase between the phase-locked pulses, preparing wavepackets predominantly composed of either zero-phonon lines or phonon side bands.

Graphical abstract: Pump–probe spectroscopy with phase-locked pulses in the condensed phase: decoherence and control of vibrational wavepackets

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Article information


Submitted
28 Jun 2005
Accepted
22 Jul 2005
First published
01 Aug 2005

Phys. Chem. Chem. Phys., 2005,7, 3143-3149
Article type
Paper

Pump–probe spectroscopy with phase-locked pulses in the condensed phase: decoherence and control of vibrational wavepackets

M. Fushitani, M. Bargheer, M. Gühr and N. Schwentner, Phys. Chem. Chem. Phys., 2005, 7, 3143
DOI: 10.1039/B509153E

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