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Frontiers in Optics

Coherent Control of Ultra-Cold Molecules

Christiane P. Koch

Published Jan 1, 2008• 0 citations
Publisher

Abstract

Based on the example of short-pulse photoassociation, I will discuss how ultra-cold matter may be merged with coherent control. The concept of ‘shaping’ the photoassociation dynamics yields larger molecule formation rates and better final-state control.
DOI
10.1364/ls.2008.lwe2

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The paper investigates cold molecules formation in the photoassociation of two cold atoms by a strong laser pulse applied at short interatomic distances, which lead to a molecular dynamics taking place in the light-induced (adiabatic) potentials. A two electronic states model in the cesium dimer is used to analyse the effects of this strong coupling regime and to show specific results: i) acceleration of the ground state population to the inner zone due to a non-impulsive regime of coupling at short and intermediate interatomic distances; ii) formation of cold molecules in strongly bound levels of the ground state, where the population at the end of the pulse is much bigger than the population photoassociated in bound levels of the excited state; iii) the final momentum distribution of the ground state wavepacket keeping the signatures of the maxima in the initial wavefunction continuum. It is shown that the topology of the light-induced potentials plays an important role in dynamics.
This paper investigates the formation of cold molecules in the photoassociation of two cold atoms by a strong laser pulse applied at short interatomic distances, which lead to molecular dynamics taking place in the light-induced (adiabatic) potentials. A two-electronic-state model in the caesium dimer is used to analyse the effects of this strong coupling regime and to show specific results: (i) acceleration of the ground-state population to the inner zone due to a non-impulsive regime of coupling at short and intermediate interatomic distances, (ii) formation of cold molecules in strongly bound levels of the ground state, where the population at the end of the pulse is much bigger than the population photoassociated in bound levels of the excited state, and (iii) the final momentum distribution of the ground-state wavepacket keeping the signatures of the maxima in the initial wavefunction continuum. It is shown that the topology of the light-induced potentials plays an important role in dynamics.
Enhancement of the production of cold molecules via photoassociation is considered for the Cs2{\mathrm{Cs}}_{2}Cs2​ system. The employment of chirped picosecond pulses is proposed and studied theoretically. The analysis is based on the ability to achieve impulsive excitation which is given by the ultracold initial conditions where the nuclei are effectively stationary during the interaction with a field. The appropriate theoretical framework is the coordinate-dependent two-level system. Matching the pulse parameters to the potentials and initial conditions results in full Rabi cycling between the electronic potentials. By chirping the laser pulse, adiabatic transfer leading to the population inversion from the ground to the excited state is possible in a broad and tunable range of internuclear distance. Numerical simulations based on solving the time-dependent Schr\"odinger equation (TDSE) were performed. The simulation of the photoassociation of Cs2{\mathrm{Cs}}_{2}Cs2​ from the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ to the excited ${0}_{g}^{\ensuremath{-}}$ state under ultracold conditions verifies the qualitative picture. The ability to control the population transfer is employed to optimize molecular formation. Transfer of population to the excited ${0}_{g}^{\ensuremath{-}}$ surface leaves a void in the nuclear density of the ground ${}^{3}{\ensuremath{\Sigma}}_{u}^{+}$ surface. This void is either filled by thermal motion or by quantum ``pressure'' and it is the rate-determining step in the photoassociation. The spontaneous-emission process leading to cold-molecules is simulated by including an optical potential in the TDSE. Consequently, the rate of cold molecule formation in a pulsed mode is found to be larger than that obtained in a continuous-wave mode.