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arXiv:2310.02498 · The Journal of Physical Chemistry Letters

Single-Shot Nondestructive Quantum Sensing for Gaseous Samples with Hundreds of Chiral Molecules

Chong Ye, Yifan Sun, Yong Li, Xiangdong Zhang

Published Jul 21, 2023• 15 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1021/acs.jpclett.3c01622

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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.
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.
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.
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.
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.
The measurement of circular dichroism (CD) has widely been exploited to distinguish the different enantiomers of chiral structures. It has been applied to natural materials (e.g., molecules) as well as to artificial materials (e.g., nanophotonic structures). However, especially for chiral molecules the signal level is very low and increasing the signal-to-noise ratio is of paramount importance to either shorten the necessary measurement time or to lower the minimum detectable molecule concentration. As one solution to this problem, we propose here to use quantum states of light in CD sensing to reduce the noise below the shot noise level encountered when using coherent states of light. Through a multiparameter estimation approach, we identify the ultimate quantum limit of the precision in CD sensing, allowing for general schemes including additional ancillary modes. We show that the ultimate quantum limit can be achieved by various optimal schemes. These include using a pair of Fock-state probes in a direct sensing configuration and pairs of twin beams in an ancilla-assisted sensing configuration, for both of which photon number-resolved detection is shown to be the optimal measurement. These optimal schemes offer a significant quantum enhancement even in the presence of some additional system loss. The near optimality of a scheme using a single twin beam in a direct sensing configuration is also shown for cases where the actual CD signal is very small. Alternative optimal schemes involving single-photon sources and detectors are also proposed. This work paves the way for further investigations of quantum metrological techniques in chirality sensing.
We present a novel approach to chiral discrimination using gate-based quantum processors, addressing a key challenge in adapting conventional control techniques using modern quantum computing. Schemes such as stimulated rapid adiabatic passage and shortcuts to adiabaticity have shown strong potential for enantiomer discrimination; however, their reliance on analog and continuous-time control makes them incompatible with digital gate-based quantum computing architectures. Here, we adapt these protocols for quantum computers by discretizing their Gaussian-shaped pulses through Trotterization. We simulate the chiral molecule 1,2-propanediol and experimentally validate this gate-based implementation on IBM quantum hardware. Our results demonstrate that this approach is a viable foundation for advancing chiral discrimination protocols, preparing the way for quantum-level manipulation of molecular chirality on accessible quantum architectures.