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The Journal of Chemical Physics

Analysis of adiabatic passage by light-induced potentials with chirped laser pulses in three- and four-level diatomic systems

E. Heesel, B. M. Garraway, J. P. Marangos

Published Jan 10, 2006• 16 citations

Abstract

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.

DOI: 10.1063/1.2150435

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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.

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.

Adiabatic passage induced by chirped laser pulses in three-level $\ensuremath{\Lambda}$ systems is investigated. Two different strategies for efficient population transfer (equal and opposite sign of the chirp) are analyzed. The role of detuning, crucial for the attempt to reduce the population of the intermediate state, is demonstrated. The scheme of adiabatic passage by laser pulses with chirps of different sign is not symmetric with respect to the sign of the one-photon detuning. Blue detuning results in a smaller transient population of the intermediate state than does red detuning. The results are explained on the basis of dressed states. Numerical results for a fully off-resonant adiabatic passage scheme, based on two pulses with the same sign of the chirps, are also considered. The robustness of the schemes in terms of the Rabi frequency, chirp rate, detuning, and time delay of the pulses is explored.

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

{\mathrm{Na}}_{2}

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.

We have numerically explored the feasibility and the mechanism of population transfer to the excited E (1)Σ(g) electronic state of Li(2) from the v=0 level of the ground electronic state X (1)Σ(g) using the A (1)Σ(u) state as an intermediate. In this system, the use of transform limited pulses with a frequency difference greater than the maximum Rabi frequency does not produce population transfer when all possible radiative couplings are taken into account. We have employed two synchronous pulses far detuned from the allowed transition frequencies, mainly with the lower frequency pulse positively chirped, and both pulses coupling the successive pair of states, X-A and A-E. The adiabaticity of the process has been investigated by a generalized Floquet calculation in the basis of 12 field dressed molecular states, and the results have been compared with those obtained from the full solution of time dependent Schrödinger equation. The conventional representation of the process in terms of three (or four) adiabatic potentials is not valid. It has been found that for cases of almost complete population transfer in full calculations with the conservation of the vibrational quantum number, adiabatic passage is attained with the 12 state Floquet model but not with the six state model. The agreement between the full calculations and the 12 state Floquet calculations is generally good when the transfer is adiabatic. Another characteristic feature of this work is the gaining of control over the vibrational state preparation in the final electronic state by careful tuning of the laser parameters as well as the chirp rate sign. This causes time dependent changes in the adiabatic potentials and nonadiabatic transfers can be made to occur between them.