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Enantio-discrimination via the cavity-assisted three-photon process

Yu-Yuan Chen, Chong Ye, Yong Li

Published Jan 17, 2021• 1 citation
OpenAlex

Abstract

We propose a theoretical method for enantio-discrimination of chiral molecules based on a cavity-molecules system, which consists of a cavity without external driving and an ensemble of chiral mixture (containing left- and right- handed molecules) confined in the cavity. The molecules in the chiral mixture are modeled as cyclic three-level models coupled with the quantized cavity field and two classical light fields. Via the cavity-assisted three-photon process based on the cyclic three-level model, the intracavity photons are generated continuously though there is no external driving to the cavity, and the fields of the photons generated from the the left- and right- handed molecules differ with the phase difference \pi. This provides a potential way to detect the enantiomeric excess of chiral mixture by monitoring the output field of the cavity.

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We propose a theoretical method for enantio-discrimination of chiral molecules based on a cavity-molecules system, which consists of a cavity without external driving and an ensemble of chiral mixture (containing left- and right- handed molecules) confined in the cavity. The molecules in the chiral mixture are modeled as cyclic three-level models coupled with the quantized cavity field and two classical light fields. Via the cavity-assisted three-photon process based on the cyclic three-level model, the intracavity photons are generated continuously though there is no external driving to the cavity, and the fields of the photons generated from the the left- and right- handed molecules differ with the phase difference \pi. This provides a potential way to detect the enantiomeric excess of chiral mixture by monitoring the output field of the cavity.
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.
We propose an enantiodetection method of chiral molecules in a cavity with an external drive. The chiral molecules are coupled with a quantized cavity field and two classical light fields to form the cyclic three-level systems. The chirality-dependent cavity-assisted three-photon process in the three-level systems leads to the generation of intracavity photons. Simultaneously, the drive field also results in a chirality-independent process of the generation of intracavity photons. Based on the interference between the intracavity photons generated from these two processes, one can detect the enantiomeric excess of chiral mixture via monitoring the transmission rate of the drive field. It is also shown that our method can work in the single-molecule weak-coupling region and in the absence of additional enantiopure samples. These advantages make it offer promising applications in enantiodetection of chiral molecules.
We propose a theoretical method for enantio-discrimination based on the light deflection effect in four-level models of chiral molecules. This four-level model consists of a cyclic three-level subsystem coupled by three strong driving fields and an auxiliary level connected to the cyclic three-level subsystem by a weak probe field. It is shown that the induced refractive index for the weak probe field is chirality-dependent. Thus, it will lead to chirality-dependent light deflection when the intensities of two of the three strong driving fields are spatially inhomogeneous. As a result, the deflection angle of the weak probe light can be utilized to detect the chirality of pure enantiomers and enantiomeric excess of the chiral mixture. Therefore, our method may act as a tool for enantio-discrimination.
We investigate enantiodetection for both a single cyclic three-level chiral molecule and finite ensembles of such molecules by monitoring the steady-state intracavity photon number in a cavity-QED platform. Our scheme exploits the intrinsic global πππ-phase difference between opposite enantiomers to engineer destructive and/or constructive interference pathways, enabling a direct readout of enantiomeric excess with an error below 5%5\%5%. To capture mesoscopic many-molecule effects beyond mean field while avoiding brute-force master-equation simulations, we employ a generalized discrete truncated Wigner approximation, which is well suited for systems with many yet finite molecules. These results pave the way for implementing enantiodetection in realistic quantum-optical settings.
We propose a method to realize enantiodiscrimination of chiral molecules based on quantum correlation function in a driven cavity-molecule system, where the chiral molecule is coupled with a quantized cavity field and two classical light fields to form a cyclic three-level model. According to the inherent properties of electric-dipole transition moments of chiral molecules, there is a π-phase difference in the overall phase of the cyclic three-level model for the left- and right-handed chiral molecules. Thus, the correlation function depends on this overall phase and is chirality-dependent. The analytical and numerical results indicate that the left- and right-handed chiral molecules can be discriminated by detecting quantum correlation function. Our work opens up a promising route to discriminate molecular chirality, which is an extremely important task in pharmacology and biochemistry.
Developing effective methods to measure the enantiomeric excess of the chiral mixture is one of the major topics in chiral molecular researches, yet remains challenging. Enantiodetection method via two-dimensional (2D) spectroscopy based on a four level model, containing a cyclic three-level system (CTLS), of chiral molecules was recently proposed and demonstrated, yet with a strict condition of the one-photon resonance (where three driving fields are exactly resonantly coupled to the three electric-dipole transitions, respectively) in the CTLS and narrowband probe pulse assumption. Here, we extend the 2D spectroscopy method to more general experimental conditions, with three-photon resonance (where the sum of the two smaller frequencies among the three driving fields equals to the third one) and broadband probe pulse. Our method remains effective on enantiodetection with the help of experimental techniques, such as the chop detection method, which is used to eliminate the influence of the other redundant levels existing in the real system of chiral molecules. Under these more general conditions, the enantiomeric excess of the chiral mixture is estimated by taking an easily available standard sample (usually the racemic mixture) as the reference.