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arXiv:1909.06923 · The Journal of Chemical Physics

Enantio-discrimination via light deflection effect

Yu-Yuan Chen, Chong Ye, Quansheng Zhang, Yong Li

Published May 27, 2020• 27 citations
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Abstract

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.

DOI
10.1063/5.0008157

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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 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.
Determination of enantiomeric excess is important and remains challenging. We propose theoretically a spectroscopic method for this issue based on the chirality-dependent ac Stark effects in cyclic three-level models under the three-photon resonance condition. The enantiomeric excess of the chiral mixture is determined by comparing the amplitudes of the two ac Stark peaks chosen in the Fourier transform spectrum of the induced polarizations, which are (approximately) proportional to the number of molecules of the two enantiomers, respectively. In contrast to current spectroscopic methods based on the interference between the electric and (usually weak) magnetic dipole transition moments and/or with the need for enantiopure samples, our method involves only electric dipole transitions and does not require the enantiopure samples. Therefore, it will give strong chiral signals and can be applied to the determination of enantiomeric excess for chiral molecules whose enantiopure samples are still challenging to achieve.
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.
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.
Developing effective methods to measure the enantiomeric excess of chiral mixtures is one of the major topics in chiral molecular research but remains challenging. An 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, but with a strict condition of one-photon resonance (where three driving fields are exactly resonantly coupled to the three electric dipole transitions) in the CTLS and narrow-band 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 the third one) and a 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 that exist 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.