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Optics Express

Discrimination of enantiomers through quantum interference and quantum Zeno effect

Jin‐Lei Wu, Yan Wang, Shi‐Lei Su, Yan Xia, Yongyuan Jiang, Jie Song

Published Oct 12, 2020• 26 citations
Publisher

Abstract

Quantum optical methods have great potential for highly efficient discrimination of chiral molecules. We propose quantum interference-based schemes of enantio-discrimination under microwave regime among molecular rotational states. The quantum interference between field-driven one- and two-photon transitions of two higher states is designed to be constructive for one enantiomer but destructive for the other, since a certain transition dipole moment can be set to change sign with enantiomers. Therefore, two enantiomers can evolve into entirely different states from the same ground state. Through strengthening the constructive interference, the quantum Zeno effect is found in one enantiomer and then its excitation is suppressed, which also enables the enantio-discrimination. We simulate the schemes for differentiating between S and R enantiomers of 1, 2-propanediol (C 3 H 8 O 2 ) molecules. With the analysis of the phase sensitivity to microwave fields and the effect of energy relaxations, the highly efficient enantio-discrimination of the 1, 2-propanediol molecules may be achieved.

DOI
10.1364/oe.404089

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Quantum optical methods have great potential for highly efficient discrimination of chiral molecules. We propose quantum interference-based schemes of enantio-discrimination under microwave regime among molecular rotational states. The quantum interference between field-driven one- and two-photon transitions of two higher states is designed to be constructive for one enantiomer but destructive for the other, since a certain transition dipole moment can be set to change sign with enantiomers. Therefore, two enantiomers can evolve into entirely different states from the same ground state. Through strengthening the constructive interference, the quantum Zeno effect is found in one enantiomer and then its excitation is suppressed, which also enables the enantio-discrimination. We simulate the schemes for differentiating between S and R enantiomers of 1, 2-propanediol (C 3 H 8 O 2 ) molecules. With the analysis of the phase sensitivity to microwave fields and the effect of energy relaxations, the highly efficient enantio-discrimination of the 1, 2-propanediol molecules may be achieved.
Chiral discrimination that is efficient at detecting tiny amounts of chiral substances, especially at the single-molecule level, is in great demand. Here, we propose a single-shot nondestructive quantum sensing method addressing such an issue. Our scheme consists of two steps. In the first step, the two enantiomers are prepared in different rotational states via microwave enantio-specific state transfer. Then, chiral discrimination is transferred to quantum hypothesis testing. In the second step, we for the first time introduce a nondestructive quantum-state detection technique assisted with a microwave resonator for chiral discrimination, through which the molecular chirality is determined by the sign of the output signals. Using a typical chiral molecule, 1,2-propanediol, and an experimentally feasible model based on spherical Fabry–Pérot cavity, we show that the molecular chirality of slowly moving enantiopure gaseous samples with 10 2 –10 3 molecules can be highly credibly distinguished in a single-shot detection. By further trapping chiral molecules, it is promising to achieve chiral discrimination at the single-molecule level by using our approach.
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.
We propose to discriminate chiral molecules by combining one- and two-photon processes in a closed-loop configuration. The one-photon-coupling intrinsic $\ensuremath{\pi}$-phase difference between two enantiomers leads to their different superposition states, which is then followed by a two-photon process through three-mode parallel paths (3MPPs), enabling the discrimination of enantiomers by inducing their entirely different population distributions. The 3MPPs are constructed by ``chosen paths,'' a method of shortcuts to adiabaticity, exhibiting a fast two-photon process. As an example, we propose to perform the scheme in 1,2-propanediol molecules, which show relatively robust and highly efficient results under considering the experimental issues concerning unwanted transitions, imperfect initial state, pulse shaping, control errors, and the effect of energy relaxations. The present work may provide help for laboratory researchers in a robust separation of chiral molecules.
Abstract We theoretically study enantioselective state transfer (ESST) in a reduced four-level rotational model of a chiral molecule. The cyclic three-level description is reliable only when the microwave bandwidth remains well below the detunings to nearby dipole-allowed rotational transitions. When the bandwidth becomes comparable to the detuning of the nearest relevant additional state, this state can participate in the dynamics, requiring a four-level description. Using a constrained multiobjective quantum optimal-control method, we design microwave control fields in the narrow-band three-level and broadband four-level regimes. The resulting optimized fields achieve final discrimination degrees above 0.999 under four-level propagation in both regimes, while direct four-level optimization permits shorter-duration control by explicitly accounting for transient fourth-state participation. To reveal the underlying coherent mechanism, the transition amplitudes are decomposed into even- and odd- a pathway groups. The even- a contribution is common to the two enantiomers, whereas the odd- a contribution changes sign, resulting in constructive interference for one enantiomer and destructive interference for the other. Lindblad simulations further show that the four-level optimized control fields exhibit enhanced robustness against rotational relaxation owing to their shorter control durations. These results show that broadband four-level optimization can enable faster ESST with improved robustness against dissipative relaxation while preserving the even/odd- a pathway-interference mechanism.
A novel optical method for distinguishing chiral molecules is proposed and validated within a quantum simulator employing a trapped-ion qudit. This approach correlates the sign disparity of the dipole moment of chiral molecules with distinct cyclic evolution trajectories, yielding the unity population contrast induced by the different non-Abelian holonomies corresponding to the chirality. Harnessing the principles of holonomic quantum computation (HQC), our method achieves highly efficient, non-adiabatic, and robust detection and separation of chiral molecules. Demonstrated in a trapped ion quantum simulator, this scheme achieves nearly 100% contrast between the two enantiomers in the population of a specific state, showcasing its resilience to the noise inherent in the driving field.
We propose a method for enantio-detection of chiral molecules based on a cavity-molecule system, where the left- and right-handed molecules are coupled with a cavity and two classical light fields to form cyclic three-level models. Via the cavity-assisted three-photon processes based on the cyclic three-level model, photons are generated continuously in the cavity even in the absence of external driving to the cavity. However, the photonic fields generated from the three-photon processes of left- and right-handed molecules differ with the phase difference π according to the inherent properties of electric-dipole transition moments of enantiomers. This provides a potential way to detect the enantiomeric excess of chiral mixture by monitoring the output field of the cavity.