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Physical Review A

Enantioselective switch on responses of dissipative chiral molecules

Chong Ye, Xiaowei Mu, Yifan Sun, Libin Fu, Xiangdong Zhang

Published Feb 20, 2024• 0 citations
Publisher

Abstract

Enantiodetection is an important and challenging task across natural sciences. The cyclic three-level models of chiral molecules provided possibilities to obtain the ultimate limit of the enantioselectivities in purely electric dipole effects, yielding an emerging frontier in enantiodetection. However, the generated enantioselectivities were usually severely reduced in the strong decoherence region, failing most of the related chiroptical methods. Here, we propose enantioselective switches of molecular responses by well designing the electromagnetic fields based on the dissipative cyclic three-level model of chiral molecules and provide a chiroptical method of enantiodetection. In our switches, the steady-state responses are turned on for the selected enantiomer and simultaneously turned off for its mirror image, which corresponds to the ultimate limit of enantioselectivities. The switches can survive in the strong decoherence regions, and so does the suggested chiroptical method of enantiodetection. Our results give more insight into answering whether the enantioselective responses of light based on the cyclic three-level model can survive in the strong decoherence region and thus have a potential impact on further research.

DOI
10.1103/physreva.109.023114

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Enantiodetection is an important and challenging task across natural sciences. The cyclic three-level models of chiral molecules provided possibilities to obtain the ultimate limit of the enantioselectivities in purely electric dipole effects, yielding an emerging frontier in enantiodetection. However, the generated enantioselectivities were usually severely reduced in the strong decoherence region, failing most of the related chiroptical methods. Here, we propose enantioselective switches of molecular responses by well designing the electromagnetic fields based on the dissipative cyclic three-level model of chiral molecules and provide a chiroptical method of enantiodetection. In our switches, the steady-state responses are turned on for the selected enantiomer and simultaneously turned off for its mirror image, which corresponds to the ultimate limit of enantioselectivities. The switches can survive in the strong decoherence regions, and so does the suggested chiroptical method of enantiodetection. Our results give more insight into answering whether the enantioselective responses of light based on the cyclic three-level model can survive in the strong decoherence region and thus have a potential impact on further research.
Enantiodetection is an important and challenging task across natural science. Nowadays, some chiroptical methods of enantiodetection based on decoherence-free cyclic three-level models of chiral molecules can reach the ultimate limit of the enantioselectivities in the molecular responses. They are thus more efficient than traditional chiroptical methods. However, decoherence is inevitable and can severely reduce enantioselectivities in these advanced chiroptical methods, so they only work well in the weak decoherence region. Here, we propose an enantioselective switch on the radiation of dissipative chiral molecules and develop a novel chiroptical method of enantiodetection working well in all decoherence regions. In our scheme, radiation is turned on for the selected enantiomer and simultaneously turned off for its mirror image by designing the electromagnetic fields well based on dissipative cyclic three-level models. The enantiomeric excess of a chiral mixture is determined by comparing its emissions in two cases, where the radiations of two enantiomers are turned off respectively. The corresponding enantioselectivities reach the ultimate limit in all decoherence regions, offering our scheme advantages over other chiroptical methods in enantiodetection. Our work potentially constitutes the starting point for developing more efficient chiroptical techniques for enantiodection in all decoherence regions.
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 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.
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.
Two molecules are enantiomers if they are nonsuperimposable mirror images of each other. Electric dipole-allowed cyclic transitions |1⟩ → |2⟩ → |3⟩ → |1⟩ obey the symmetry relation O R = − O S, where O R, S = (μ 21 R, S E 21 )(μ 13 R, S E 13 )(μ 32 R, S E 32 ) and R and S label the two enantiomers. Herein, we generalize the concept of topological frequency conversion to an ensemble of enantiomers. We show that, within a rotating-frame, the pumping power between fields of frequency ω 1 and ω 2 is sensitive to enantiomeric excess, P 2 → 1 = ℏ[ω 1 ω 2 C L R /(2π)]( N R – N S ), where N i is the number of enantiomers i and C L R is an enantiomer-dependent Chern number. Connections with chiroptical microwave spectroscopy are made. Our work provides an underexplored and fertile connection between topological physics and molecular chirality.
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.