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The Journal of Chemical Physics

Efficient spatial separation for chiral molecules via optically induced forces

Jian-Jian Cheng

Published Jul 18, 2024• 3 citations

Abstract

We investigate an efficient spatial enantioseparation method of chiral molecules in cyclic three-level systems coupled with three optical fields using optically induced forces. When the overall phase differs by π between two enantiomers, significant variations in the magnitude and direction of the optically induced forces are observed. The manipulation of the center of mass of chiral molecules in optical fields can be achieved through the induced gauge force, primarily generated from the variations in the chirality-dependent scalar potentials created by the three inhomogeneous laser fields. By appropriately configuring the system, we can completely separate the slow spatial and fast inner dynamics, making instantaneous eigenstates of the inner Hamiltonian independent of the transverse profiles of the laser beams. Compared to previous methods, which required adiabatic conditions to be satisfied, the proposed method overcomes the limitations of the adiabatic approximation by utilizing a specific system configuration. This allows for increased flexibility in the transverse profiles of the laser beams and relaxes the constraints on the velocity of chiral molecules, leading to significantly greater spatial separations achievable across a broader range of parameters.

DOI: 10.1063/5.0207903

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Recently, several laser schemes have been proposed to separate racemic mixtures of enantiomers by splitting a molecular beam into subbeams consisting of molecules of definite chirality [Y. Li, C. Bruder, and C. P. Sun, Phys. Rev. Lett. 99, 130403 (2007); X. Li and M. Shapiro, J. Chem. Phys. 132, 194315 (2010)]. These ideas rely on laser-induced effective gauge potentials in an adiabatic basis which lead to a chirality dependent force on the center-of-mass. However, the effect of molecular rotation has been neglected in these studies. Accounting for the full molecular quantum state we find that the potentials from the adiabatic dressed state approach cannot be recovered once the molecular orientation dynamics is included, even in the rotational ground state. This affects substantially the ability to perform enantioseparation in the above mentioned setups.

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A highly efficient method for optical or microwave detection and separation of left- and right-handed chiral molecules is proposed. The method utilizes a closed-loop three-state system in which the population dynamics depends on the phases of the three couplings. Because of the different signs of the coupling between two of the states for the opposite chiralities the population dynamics is chirality dependent. By using the "shortcuts to adiabaticity" concept applied to the stimulated Raman adiabatic passage technique, one can achieve 100% contrast between the two enantiomers in the population of a particular state. It can be probed by light-induced fluorescence for large ensembles or through resonantly enhanced multiphoton ionization for single molecules.

The Stern-Gerlach effect is well known as spin-dependent splitting of a beam of atoms with magnetic moments by a magnetic-field gradient. Here, we show that an induced gauge potential may lead to a similar effect for chiral molecules. In the presence of three inhomogeneous light fields, the center of mass of a three-level chiral molecule is subject to an optically induced gauge potential, and the internal dynamics of the molecule can be described as an adiabatic evolution in the reduced pseudospin subspace of the two lowest energy levels. We demonstrate numerically that such an induced gauge potential can lead to observable pseudospin-dependent and chirality-dependent generalized Stern-Gerlach effects for mixed left- and right-handed chiral molecules under realistic conditions.