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arXiv:1910.00763 · Physical Review A

Robust and highly efficient discrimination of chiral molecules through three-mode parallel paths

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

Published Oct 21, 2019• 52 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.100.043413

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We propose to discriminate chiral molecules by combining one- and two-photon processes in a closed-loop configuration. The one-photon-coupling intrinsic \ensuremathπ\ensuremath{\pi}\ensuremathπ-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.
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.
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.
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 introduce a method for the detection of chiral molecules using sequences of three pulses driving a closed-loop three-state quantum system. The left- and right-handed enantiomers have identical optical properties (transition frequencies and transition dipole moments) with the only difference being the sign of one of the couplings. We identify 12 different sequences of resonant pulses for which chiral resolution with perfect contrast occurs. In all of them, the first and third pulses are $\ensuremath{\pi}/2$ pulses and the middle pulse is a $\ensuremath{\pi}$ pulse. In addition, one of the three pulses must have a phase shift of $\ensuremath{\pi}/2$ with respect to the other two. The simplicity of the proposed chiral resolution technique allows for straightforward extensions to more efficient and more robust implementations by replacing the single $\ensuremath{\pi}/2$ and $\ensuremath{\pi}$ pulses by composite pulses. We present specific examples of chiral resolution by composite pulses which compensate errors in the pulse areas and the detuning of the driving fields.
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.
Abstract A protocol to distinguish chiral molecules with the help of a cyclic three‐level structure is proposed. Non‐resonant microwave pules are applied to drive the transition of chiral molecules from their ground states to dressed‐states with different eigenenergies, which induce a large energy split in the levels of left‐handed molecules. This dynamics helps to realize a chirality‐selective transition, where only the right‐handed molecules can be excited to the higher levels. By utilizing the SU(2)‐transformation‐based shortcuts to adiabaticity method and the systematic‐error‐sensitivity nullified optimal control method, systematic‐error‐resistant control pulses to realize maximal population difference between molecules with different chirality are designed. Numerical simulations show that the protocol is also insensitive to random noise and energy relaxation. Therefore, the protocol may provide a promising approach for rapid and robust chiral discrimination.