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Interference between overlapping resonances: a route to coherent control of resonance lifetimes and photofragmentdistributions in the weak-field limit

Alberto Vela

Published Jul 6, 2015• 0 citations
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A weak-field coherent control scheme is applied in order to enhance the decay lifetime of a superposition of overlapping resonance states. The scheme uses a pump laser field consisting of two pulses delayed in time, each of them exciting a different energy at which several resonances of the Ne–Br 2 (B) complex overlap. Simultaneous excitation of these two energies induces interference between the overlapping resonances, which causes an enhancement of the lifetime of the superposition created. By variation of the delay time between the pulses, the mechanism of resonance interference can be controlled and optimized to achieve a maximum lifetime enhancement. The optimal delay time between pulses leading to maximum superposition lifetime can be quantitatively predicted with a simple law. The effect of the interference mechanism on the lifetime enhancement is investigated. It is found that interference induces a transfer of amplitude between the different resonances back and forth, which delays significantly the natural resonance decay, increasing the global lifetime of the superposition. Due to the simplicity of the control scheme, a wide applicability is envisioned.

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The lifetime of a resonance state overlapping with a second resonance is shown to be strongly enhanced (by a factor of 3) by combining two pump pulses to simultaneously excite the two resonances. Such an enhancement is produced by interference effects occurring between the two coherently excited overlapping resonances. A high degree of control on the intensity of interference, and thus on the resonance lifetime enhancement, is found to be achieved by varying the delay time between the pulses and their relative intensities.

The Journal of Physical Chemistry Letters•Jul 9, 2012•27 citations
A weak-field coherent control scheme is applied in order to enhance the decay lifetime of a superposition of overlapping resonance states. The scheme uses a pump laser field consisting of two pulses delayed in time, each of them exciting a different energy at which several resonances of the Ne–Br 2 (B) complex overlap. Simultaneous excitation of these two energies induces interference between the overlapping resonances, which causes an enhancement of the lifetime of the superposition created. By variation of the delay time between the pulses, the mechanism of resonance interference can be controlled and optimized to achieve a maximum lifetime enhancement. The optimal delay time between pulses leading to maximum superposition lifetime can be quantitatively predicted with a simple law. The effect of the interference mechanism on the lifetime enhancement is investigated. It is found that interference induces a transfer of amplitude between the different resonances back and forth, which delays significantly the natural resonance decay, increasing the global lifetime of the superposition. Due to the simplicity of the control scheme, a wide applicability is envisioned.
The enhancement of the resonance lifetime that occurs upon interference of two overlapping resonances excited coherently by two pulses with delayed time has been investigated as a function of the pulse temporal width and the delay time between the pulses. A general law predicting quantitatively the optimal delay time that maximizes the lifetime enhancement of the two resonances has been established in terms of the pulse width and of the lifetimes of both resonances when they are excited isolatedly. The specific form of the law and all the results found can be closely related to the characteristic features of the mechanism of interference between the overlapping resonances, providing a detailed understanding on how the mechanism operates. The proposed law is envisioned as a useful tool to design experimental strategies to control the resonance lifetime.
The lifetime of a resonance state overlapping with a second resonance is shown to be strongly enhanced (by a factor of 3) by combining two pump pulses to simultaneously excite the two resonances. Such an enhancement is produced by interference effects occurring between the two coherently excited overlapping resonances. A high degree of control on the intensity of interference, and thus on the resonance lifetime enhancement, is found to be achieved by varying the delay time between the pulses and their relative intensities.