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The Journal of Chemical Physics

Selective coherent control of the lifetime of a resonance state with laser pulses

Alberto García-Vela

Published Oct 4, 2013• 7 citations
Publisher

Abstract

It is shown that new possibilities for control of the lifetime of a system in a resonance state emerge when the density of resonances overlapping and interfering with the target resonance increases. When using a control scheme combining two pump laser pulses, it is found that increasing the density of resonance states overlapping with the target one increases the selectivity of the scheme applied, and leads to achieve a remarkably higher degree of control. Lifetime enhancements by factors up to 20 are obtained when this selectivity is applied. The underlying reasons for such strong enhancements are analyzed and explained in the light of the equations of the model applied. Application of this strategy to control and enhance the lifetime of a system in excited states is envisioned.

DOI
10.1063/1.4823983

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It is shown that new possibilities for control of the lifetime of a system in a resonance state emerge when the density of resonances overlapping and interfering with the target resonance increases. When using a control scheme combining two pump laser pulses, it is found that increasing the density of resonance states overlapping with the target one increases the selectivity of the scheme applied, and leads to achieve a remarkably higher degree of control. Lifetime enhancements by factors up to 20 are obtained when this selectivity is applied. The underlying reasons for such strong enhancements are analyzed and explained in the light of the equations of the model applied. Application of this strategy to control and enhance the lifetime of a system in excited states is envisioned.
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 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 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.
Two simple schemes are presented for the selective population transfer in systems where the target state is degenerate with a second level. Both states are coupled with the ground state via a one photon resonance. The schemes use a combination of two laser pulses. The first pulse breaks the degeneracy of the levels by inducing a Stark shift. The second pulse is chirped across the new levels. The idea is illustrated by numerical simulations of the time-dependent Schr\"odinger equation for a four-level system. The efficient population transfer is explained using a dressed state representation. In conclusion, applications for molecules are suggested.
We study the nonlinear and resonant process of two-photon ionization of atoms (He and H) in a pump-probe scheme. The pump pulse prepares the quantum system in a superposition of the ground state and an excited bound state. By varying the phase difference between the pulses, we show how it is possible to coherently control the dressed-state population during the probe pulse. Our main result is that for certain laser parameters, the control over the dressed-state population leads to strong control of the ionization probability during the probe pulse. The effect arises due to one of the dressed states becoming stabilized against ionization. Contrasting effects from circular and linear polarized pulses demonstrate how such “bound states in the continuum” are sensitive to the degeneracy of the coupled continuum.