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Conference on Lasers and Electro-Optics

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

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

Published Aug 29, 2005• 1 citation
Publisher

Abstract

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.

DOI
10.1109/iqec.2000.907778

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

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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.
This paper describes an investigation into the process of adiabatic passage by light-induced potentials (APLIP), which was previously suggested as a method for employing two strong picosecond laser pulses to transfer the population between two electronic states. We have extended earlier numerical studies in order to assess the feasibility of an experimental implementation of the APLIP concept. APLIP has been modeled in a three-level model system based on Na2 with chirped pulses, using laser parameters available from a typical chirped pulse amplified Ti:sapphire laser. The model showed that the APLIP process remains essentially unchanged for chirped pulses of equal magnitude and the opposite, or equal and positive sign of chirp as compared to the transform-limited case. We also examined the case of additional electronic states by introduction of a fourth state that lies close to the "target," i.e., final, state. The investigation showed that there are circumstances in which a significant fraction of the population gets transferred to this state which will disrupt the APLIP process. However, by switching to this fourth state as the target state in an experiment, good transfer efficiency is recovered. The results of the extension of the original APLIP modeling to chirped pulses and additional electronic states indicate that an APLIP experimental realization should be feasible in Na2.
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.
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 demonstrate numerically the conditions where a wave packet adiabatic passage method yields optimal results for selective excitation of a vibrational level on excited electronic states in molecules. In a recent contribution Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)] introduced the method of adiabatic passage by light-induced potentials (APLIP). Here we test and analyze the robustness of the APLIP process under realistic conditions for exciting the ground vibrational state of the Na2{\mathrm{Na}}_{2}Na2​ molecule to the ground vibrational level of the excited ${}^{1}{\ensuremath{\Sigma}}_{g}(4s)$ state. The spatial and temporal adiabaticity of the process assures the conservation of the vibrational quantum number during the passage and leads to the remarkable robustness of the method, which at some extent prevents the usual rotating-wave approximation to be employed.