Coherent Control of Photofragment Distributions Using Laser Phase Modulation in the Weak-Field Limit

Garcı́a-Vela, A.; Henriksen, Niels Engholm

doi:10.1021/acs.jpclett.5b00129

Cited by 31 publications

(33 citation statements)

References 41 publications

(82 reference statements)

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“…For all the energy shifts Δ E , the transient populations of Figure show postpulse variations once the pulse applied is over (for t ≥ 100), as expected from previous results . The most interesting result is that the magnitude of the variations in the populations increases remarkably with increasing Δ E .…”

Section: Resultssupporting

confidence: 83%

“…The possibility of enhancing the degree of control achieved by laser phase modulation is an important aspect which was not addressed in the previous works . Such an enhancement is expected to be associated with specific ways of interference between the overlapping resonances .…”

Section: Introductionmentioning

confidence: 98%

“…It has been shown that when a superposition of nonorthogonal, interfering states, like overlapping resonances, is prepared, transient weak‐field phase control of the time‐dependent populations of some electronic states in different systems is possible during a postpulse time window . More recently, the first computational demonstration of coherent control of the transient state distribution of photodissociation fragments, based on pure phase modulation of the pump pulse in the weak‐field regime, was reported for a polyatomic molecule supporting overlapping resonances . Phase control effects on the transient fragment distribution were demonstrated by varying the chirp rate of the pump pulse applied, and such effects were found to persist for a long‐time window after the pulse is over.…”

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Enhancement of the degree of control of photofragment distributions by laser phase modulation

Garcı́a-Vela¹

2018

Int J of Quantum Chemistry

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The possibility of enhancing the degree of control of a transient photofragment distribution achieved by means of laser phase modulation is explored. Such a control is exerted through interference between overlapping resonances, which are populated in a superposition by the laser field. It is found that by varying the central frequency of the pump laser across the energy range of the resonance superposition created, the effects of laser phase modulation on the resonance interference mechanism change remarkably, causing significant variations on the photofragment distribution. Knowledge of these variations can be used to increase and optimize the control effects of the scheme applied. The results presented here show that the intensity of the phase modulation control effect on the fragment distribution can be increased by more than double. Thus, varying the laser carrier frequency as an additional control parameter makes the control scheme more efficient and flexible.

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Section: Resultssupporting

confidence: 83%

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

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Enhancement of the degree of control of photofragment distributions by laser phase modulation

Garcı́a-Vela¹

2018

Int J of Quantum Chemistry

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“…[24][25][26][27] Such control schemes are based on the finding 24 that the lifetime of a specific overlapping resonance state depends strongly on the amplitudes of the other overlapping resonances populated in the superposition. 30 Now, a most interesting question is whether one can also control the lifetime of an isolated (nonoverlapping) resonance state in the weak-field regime. Control of the intensity of the resonance interference allows one to control the resonance lifetime.…”

Section: Introductionmentioning

confidence: 99%

Quantum interference control of an isolated resonance lifetime in the weak-field limit

Garcı́a-Vela

2015

Phys. Chem. Chem. Phys.

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Resonance states play an important role in a large variety of physical and chemical processes. Thus, controlling the resonance behavior, and particularly a key property like the resonance lifetime, opens up the possibility of controlling those resonance mediated processes. While such a resonance control is possible by applying strong-field approaches, the development of flexible weak-field control schemes that do not alter significantly the system dynamics still remains a challenge. In this work, one such control scheme within the weak-field regime is proposed for the first time in order to modify the lifetime of an isolated resonance state. The basis of the scheme suggested is quantum interference between two pathways induced by laser fields, that pump wave packet amplitude to the target resonance under control. The simulations reported here show that the scheme allows for both enhancement and quenching of the resonance survival lifetime, being particularly flexible to achieve large lifetime enhancements. Control effects on the resonance lifetime take place only while the pulse is operating. In addition, the conditions required to generate the two interfering quantum pathways are found to be rather easy to meet for general systems, which makes the experimental implementation straightforward and implies the wide applicability of the control scheme.

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“…20 Control strategies have also been proposed to modify the product fragment state distributions produced by the decay of a superposition of resonances. [21][22][23][24] It would also be desirable to have available a flexible scheme to control the fragment state distributions produced by the decay of a single, isolated resonance state.…”

mentioning

confidence: 99%

Communication: Control of the fragment state distributions produced upon decay of an isolated resonance state

Garcı́a-Vela

2016

The Journal of Chemical Physics

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Control of the fragment state distributions produced upon decay of a resonance state is achieved by using a weak laser field consisting of two pulses with a varying time delay between them. It is shown that specific product fragment states can be significantly favored or quenched. The efficiency and flexibility of the control method are found to increase with increasing resonance width. The control scheme is completely independent of the specific system to which it is applied, which makes its applicability universal.

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Coherent Control of Photofragment Distributions Using Laser Phase Modulation in the Weak-Field Limit

Cited by 31 publications

References 41 publications

Enhancement of the degree of control of photofragment distributions by laser phase modulation

Enhancement of the degree of control of photofragment distributions by laser phase modulation

Quantum interference control of an isolated resonance lifetime in the weak-field limit

Communication: Control of the fragment state distributions produced upon decay of an isolated resonance state

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