Abstract
We present a quantum control scheme which realizes suppression of the intramolecular vibrational energy redistribution (IVR). In this scheme, we utilize effective decomposition brought by intense CW‐laser fields, which enables to exclude the doorway state coupled to background manifolds. In doing so, we introduce a helper state and make it optically coupled with the doorway state through the intense CW‐laser field. We have applied the present scheme to both the Bixon‐Jortner model and the SCCl2 model system.
Highlights
In coherent laser control of molecular vibrations, the key feature is manipulation of vibrational coherence
One of the typical dissipative processes is intramolecular vibrational energy redistribution (IVR), which is characterized as irreversible population flow from the doorway state to the background manifolds [1,2,3,4,5]
The suppression of IVR is theoretically confirmed under a strong resonant CW-laser excitation, in which total population is trapped on the initial and doorway states, and it rapidly oscillates between those two states [6]
Summary
In coherent laser control of molecular vibrations, the key feature is manipulation of vibrational coherence Dissipative processes such as dephasing and population decay have been considered as formidable obstacles. It is reported that the IVR can be restricted by the laser field, in which the frequency is swept [7, 8] This phenomena is explained by the concept of adiabatic passages and the population is locked on the doorway state during the chirp pulse. In those approaches, only the suppression of IVR is considered, and there is no concept of controlling the population dynamics which escape from the IVR. Additional laser would interfere with those existing “population locking” or “IVRsuppression” fields
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