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arXiv:2406.15978 · The Journal of Physical Chemistry Letters

Enantiomer-Specific Pumping of Chiral Molecules

Fen Zou, Yong Li, Peng Zhang

Published Oct 14, 2024• 3 citations
arXivHTMLPDF

Abstract

Enantiomer-specific state transfer (ESST), which involves transferring enantiomers with different handedness of a chiral molecule into different-energy internal states, is a challenging yet significant task. Previous ESST methods are based on dynamic processes and thus require the preparation of initial states and precise control of microwave operation times. We propose a novel ESST approach, called enantiomer-specific pumping (ESP), which is based on a dissipative process and thereby eliminates the need for these two technical requirements. This approach utilizes a special microwave-induced dark state that appears exclusively for the enantiomer with a specific handedness. Specifically, in ESP, the enantiomer lacking the dark state can be pumped out of the subspace of relevant internal states, while the enantiomer with the dark state maintains a finite probability within this subspace, offering high efficiency in ESST. Notably, ESP facilitates enantiodetection without the need for enantiopure samples as reference.

DOI
10.1021/acs.jpclett.4c02139

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Enantiomer-specific state transfer (ESST), which involves transferring enantiomers with different handedness of a chiral molecule into different-energy internal states, is a challenging yet significant task. Previous ESST methods are based on dynamic processes and thus require the preparation of initial states and precise control of microwave operation times. We propose a novel ESST approach, called enantiomer-specific pumping (ESP), which is based on a dissipative process and thereby eliminates the need for these two technical requirements. This approach utilizes a special microwave-induced dark state that appears exclusively for the enantiomer with a specific handedness. Specifically, in ESP, the enantiomer lacking the dark state can be pumped out of the subspace of relevant internal states, while the enantiomer with the dark state maintains a finite probability within this subspace, offering high efficiency in ESST. Notably, ESP facilitates enantiodetection without the need for enantiopure samples as reference.
Enantiomer-specific pumping of chiral molecules in high-JJJ rotational states
Enantiomer-specific state transfer (ESST) based on electric-dipole transitions has attracted considerable interest in the studies of manipulating molecules with electromagnetic fields. It also holds promise as a powerful tool for enantiomer detection and separation. To date, experimental demonstrations of ESST have focused mainly on molecules in the lowest rotational angular-momentum states, namely, J=0J=0J=0 and J=1J=1J=1. Realistic molecular samples, however, may contain appreciable populations in higher-JJJ rotational states, making it desirable to develop ESST schemes applicable to such states. Nevertheless, one cannot derive such schemes via a simple and straightforward extension of existing low-JJJ schemes, because higher-JJJ manifolds contain more magnetic sub-levels and involve more complicated networks of electric-dipole transitions. Here, we propose an ESST scheme for chiral molecules involving the J=1J=1J=1 and J=2J=2J=2 rotational states. Specifically, our scheme is based on enantiomer-specific pumping driven by three linearly polarized microwave fields and one laser beam. Under this scheme, one enantiomer is pumped into an enantiomer-specific dark state within a sub manifold with J=1,2J=1,2J=1,2, whereas the other enantiomer is dissipatively pumped out of this manifold. Our strategy can be extended to systems involving rotational states with even higher angular momenta.
We propose a streamlined method of fast enantiomer-specific state transfer (ESST) of chiral molecules in cyclic three-level systems. Such three-level enantiomers are chirality-dependent systems driven by one of the three Rabi frequencies differing with a sign for the left- and right-handed chiral molecules. When the Hamiltonian of the three-level chiral molecules possesses the specific SU(2) algebraic structure, the populations transferred to the two excited states are shown to be exchanged between the left- and right-handed chiral molecules if they are initially prepared in their ground states. By employing unitary SU(2) transformation and inversely engineering time-dependent Hamiltonians with designed Rabi frequencies, we can make the left- and right-handed chiral molecules evolve respectively to different excited states from their initial ground states simultaneously. Thus a fast ESST is achieved.
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.
Using a microwave-regime cyclic three-state configuration, enantiomer-selective state transfer (ESST) is carried out through two-path interference between a direct one-photon coupling and an effective two-photon coupling. A phase difference of $\ensuremath{\pi}$ in the one-photon process between the two enantiomers makes the interference constructive for one enantiomer but destructive for the other. Therefore only one enantiomer is excited into a higher rotational state, while the other remains in the ground state. The scheme allows flexibility in the pulse waveforms and the time order of the two paths. We simulate the scheme for a sample of cyclohexylmethanol (C7H14O{\mathrm{C}}_{7}{\mathrm{H}}_{14}\mathrm{O}C7​H14​O) molecules. The simulation results show that robust high-fidelity ESST can be obtained when experimental concerns are considered. Finally, we propose to employ the ESST scheme to implement enantioseparation and determine enantiomeric excesses.
An interesting method of fast enantio-specific state transfer (ESST) is proposed for cyclic three-level systems of chiral molecules. We show that the fast population transfer via shortcut to adiabaticity can be accomplished for the cyclic three-level system of a general (chiral) molecule with invariant-based inverse engineering of the coupling strengths. By choosing appropriate parameters, the two enantiomers, which are initially prepared in their ground states in the three-level systems, will evolve respectively along their enantio-selective shortcut-to-adiabaticity paths to different-energy final states simultaneously, thereby achieving the fast ESST.
Enantiospecific state transfer of chiral molecules is extremely important because enantiomers coexist in many biologically active compounds and play significantly different physiological, pharmacological, and biological roles. The inherently strong electric-dipole optical approaches based on the cyclic three-level model of chiral molecules have been extensively discussed. But, for the cases of large chiral molecules and/or chiral molecules of low asymmetry, the four-level model with two sub-loops is more realistic to describe the molecules. Based on the four-level model, we propose a pump-control approach to realize the highly efficient enantiospecific state transfer. In our approach, two pump pulses are applied to generate molecular coherence between the ground state and the first excited state of our working model. According to the coherence of the molecules, we adjust the phase and pulse area of the control pulse, then we obtain the highly efficient enantiospecific state transfer in the first excited working state. In addition, we further optimize the fraction of enantiopure samples by adjusting the area of the two pump pulses.