Frontiers in Optics

Selective and Efficient Excitation of a Diatomic Molecule by a Train of Weak Ultrashort Pulses

Luı́s E. E. de Araujo

Published Jan 1, 2008• 0 citations

Abstract

I show that a train of weak ultrashort pulses can selectively and efficiently transfer population between electronic states of a diatomic molecule. Almost 100% transfer between the ground and an excited vibrational state is demonstrated.

DOI: 10.1364/fio.2008.fthp7

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Frontiers in Optics

Selective and Efficient Excitation of a Diatomic Molecule by a Train of Weak Ultrashort Pulses

Luı́s E. E. de Araujo

Published Jan 1, 2008• 0 citations

Publisher

Abstract

DOI: 10.1364/fio.2008.fthp7

Related papers

Selective and efficient excitation of diatomic molecules by an ultrashort pulse train

Luı́s E. E. de Araujo

In this paper, I discuss the selective and efficient vibrational population transfer between electronic states of diatomic molecules by a weak, ultrashort pulse train. The spectrum of each individual pulse in the train is wide enough to simultaneously excite several vibrational levels of the molecule. However, selectivity is achieved by mismatching the frequency comb, associated with the pulse train, to the excited vibrational levels. Efficiency results from the coherent accumulation of population from one pulse in the train to the next.In this paper, I discuss the selective and efficient vibrational population transfer between electronic states of diatomic molecules by a weak, ultrashort pulse train. The spectrum of each individual pulse in the train is wide enough to simultaneously excite several vibrational levels of the molecule. However, selectivity is achieved by mismatching the frequency comb, associated with the pulse train, to the excited vibrational levels. Efficiency results from the coherent accumulation of population from one pulse in the train to the next.

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An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.

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Summary form only given. We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. Light-induced potentials were also key to understanding APLIP (adiabatic passage by light induced potentials), where a wave packet is guided from one ground vibrational state to another. However, in the new process we show how to target specific vibrational states with strong short pulses. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.Summary form only given. We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. Light-induced potentials were also key to understanding APLIP (adiabatic passage by light induced potentials), where a wave packet is guided from one ground vibrational state to another. However, in the new process we show how to target specific vibrational states with strong short pulses. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.

Conference on Lasers and Electro-OpticsAug 29, 20051 citation

{\mathrm{K}}_{2}

molecule are shown.

Highly efficient and selective population transfer in NO molecules in the electronic ground state (

{\mathit{X}}^{2}

${\mathrm{\ensuremath{\Pi}}}_{1/2}$) from the vibrational level v''=0 to the level v''=6 is demonstrated. It shows, for the first time with pulsed lasers, that a rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counterintuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage.