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The Journal of Chemical Physics

Communications: Spatial separation of enantiomers by coherent optical means

Xuan Li, Moshe Shapiro

Published Jan 22, 2010• 22 citations
Publisher

Abstract

We show that it is possible to spatially separate a ("racemic") mixture of left-handed and right-handed chiral molecules using optically induced forces. The separation is affected by the irradiation of the racemic mixture with three spatially inhomogeneous and partially overlapping cw laser fields, giving rise to enantiomeric and vibrational dependent light-induced forces. Two experimental arrangements, one consisting of placing the racemate in 1 mK optical trap, the second composed of a tightly skimmed molecular beam of the racemic mixture, forming one arm of a four-sided cavity, are numerically tested by performing quantum wave packet propagation and classical trajectories. Both the classical and the quantum simulations show an essentially perfect spatial separation between enantiomers of several vibrational states.

DOI
10.1063/1.3298585

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We show that it is possible to spatially separate a ("racemic") mixture of left-handed and right-handed chiral molecules using optically induced forces. The separation is affected by the irradiation of the racemic mixture with three spatially inhomogeneous and partially overlapping cw laser fields, giving rise to enantiomeric and vibrational dependent light-induced forces. Two experimental arrangements, one consisting of placing the racemate in 1 mK optical trap, the second composed of a tightly skimmed molecular beam of the racemic mixture, forming one arm of a four-sided cavity, are numerically tested by performing quantum wave packet propagation and classical trajectories. Both the classical and the quantum simulations show an essentially perfect spatial separation between enantiomers of several vibrational states.
Abstract In this paper, we show the possibility of spatially separating two opposite enantiomers of chiral molecules, using an optical dipole potential. Because of the broken mirror symmetry of effective potential, chiral molecules have a cyclic three-level Δ-configuration structure. Irradiation of these molecules with three femtosecond laser pulses gives rise to an enantiomer-dependent optical force. Interestingly, considerable differences in the direction of the force felt by the enantiomers have been shown to cause the chirality-dependent optical dipole potential which stably captures only one enantiomeric form. Moreover, the proposed scheme provides a complete control over what kind of molecules, the left- or right-handed ones, can be selectively trapped. Note that we have analyzed the optical force, and specifically the trapping effect, by considering the full interaction Hamiltonian, including both rotating and counter-rotating terms.
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.
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.
Controlling the internal quantum states of chiral molecules for a selected enantiomer has a wide range of fundamental applications. Using tailored microwave fields, a chosen rotational state can be enriched for a selected enantiomer, even starting from a racemic mixture. This enables rapid switching between samples of different enantiomers in a given state, holding great promise, for instance, for measuring parity violation in chiral molecules. Achieving full enantiomer-specific state transfer is a key requirement for this and many other applications. Although theoretically feasible, achieving the required experimental conditions seemed unrealistic. Here, we realize near-ideal conditions, overcoming both the limitations of thermal population and spatial degeneracy in rotational states. Our results show that 96% state-specific enantiomeric purity can be obtained from a racemic mixture, in an approach that is universally applicable to all chiral molecules of C1 symmetry.
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.