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arXiv:quant-ph/0002023 · Physical Review A

Tailoring of vibrational state populations with light-induced potentials in molecules

Mirta Rodríguez, Kalle‐Antti Suominen, B. M. Garraway

Published Oct 19, 2000• 54 citations
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Abstract

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 and their vibrational eigenstates. 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.

DOI
10.1103/physreva.62.053413

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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.

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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 and their vibrational eigenstates. 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.
Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.
We show that the vibrational state tailoring method developed for molecular systems can be applied for cold atoms in optical lattices. The original method is based on a three-level model interacting with two strong laser pulses in a counterintuitive sequence [M. Rodriguez et al., Phys. Rev. A 62, 053413 (2000)]. Here we outline the conditions for achieving similar dynamics with single time-dependent potential surfaces. It is shown that guided switching between diabatic and adiabatic evolution has an essential role in this system. We also show that efficient and precise tailoring of motional states in optical lattices can be achieved, for instance, simply by superimposing two lattices and moving them with respect to each other.
In this paper we propose to control the bond length of a diatomic molecule and its vibrational coherent motion over arbitrary distances. The method requires (a) mixing a dissociative potential with bound electronic configurations in order to stabilize the continuum, and (b) manipulating the wave-packet transfer below the threshold of adiabatic passage. Using asymmetric pulses it is possible to implement sudden-adiabatic transitions to stop or induce the motion in the light-induced potential, controlling the nonadiabatic dynamics in a most efficient way.
We present the process of adiabatic passage by light-induced potentials for transferring a wave packet from one molecular potential to the displaced ground vibrational state of another. The process uses a counterintuitive sequence of light pulses to couple three molecular states. It shares many features with the process of stimulated Raman adiabatic passage, such as high efficiency and insensitivity to pulse parameters. However, in the former there is no two-photon resonance, and the main mechanism for the transport of the wave packet is a light-induced potential.
We discover a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the sign of the slope of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses. As an example, we show how the scheme can be applied to population inversion in Na2.