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arXiv:2301.06005 · New Journal of Physics

Optical-pumping enantio-conversion of chiral mixtures in presence of tunneling between chiral states

Fen Zou, Chong Ye, Yong Li

Published Dec 1, 2023• 2 citations
arXivHTMLPDF

Abstract

Abstract Enantio-conversion of chiral mixtures, converting the mixtures composed of left- and right-handed chiral molecules into the homochiral ensembles, has become an important research topic in chemical and biological fields. In previous studies on enantio-conversion, the tunneling interaction between the left- and right-handed chiral states was often neglected. However, for certain chiral molecules, this tunneling interaction is significant and cannot be ignored. Here we propose a scheme for enantio-conversion of chiral mixtures through optical pumping based on a four-level model of chiral molecules, comprising two chiral ground states and two achiral excited states, with a tunneling interaction between the chiral states. Under one-photon large detuning and two-photon resonance conditions, one of the achiral excited states is eliminated adiabatically. By well designing the detuning and coupling strengths of the electromagnetic fields, the tunneling interaction between two chiral states and the interaction between one of the chiral states and the remaining achiral excited state can be eliminated. Consequently, one chiral state remains unchanged, while the other can be excited to an achiral excited state, establishing chiral-state-selective excitations. By numerically calculating the populations of two chiral ground states and the enantiomeric excess, we observe that high-efficiency enantio-conversion is achieved under the combined effects of system dissipation and chiral-state-selective excitations.

DOI
10.1088/1367-2630/ad121e

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Abstract Enantio-conversion of chiral mixtures, converting the mixtures composed of left- and right-handed chiral molecules into the homochiral ensembles, has become an important research topic in chemical and biological fields. In previous studies on enantio-conversion, the tunneling interaction between the left- and right-handed chiral states was often neglected. However, for certain chiral molecules, this tunneling interaction is significant and cannot be ignored. Here we propose a scheme for enantio-conversion of chiral mixtures through optical pumping based on a four-level model of chiral molecules, comprising two chiral ground states and two achiral excited states, with a tunneling interaction between the chiral states. Under one-photon large detuning and two-photon resonance conditions, one of the achiral excited states is eliminated adiabatically. By well designing the detuning and coupling strengths of the electromagnetic fields, the tunneling interaction between two chiral states and the interaction between one of the chiral states and the remaining achiral excited state can be eliminated. Consequently, one chiral state remains unchanged, while the other can be excited to an achiral excited state, establishing chiral-state-selective excitations. By numerically calculating the populations of two chiral ground states and the enantiomeric excess, we observe that high-efficiency enantio-conversion is achieved under the combined effects of system dissipation and chiral-state-selective excitations.
Enantio-conversion with the help of electromagnetic fields is an essential issue due to the chirality dependence of many chemical, biological, and pharmaceutical processes. Here, we propose a method for this issue based on a five-level double-$\mathrm{\ensuremath{\Delta}}$ model of chiral molecules. By utilizing the breaking of left-right symmetry in two $\mathrm{\ensuremath{\Delta}}$-type substructures, we can establish chiral-state-selective excitations with one chiral ground state being excited to an achiral excited state and the other one being undisturbed. In the meanwhile, the achiral excited state will relax to two chiral ground states. The two effects simultaneously acting on chiral mixtures can convert molecules of different chiralities to ones of the same chirality, i.e., enantio-conversion via optical pumping. We numerically show that highly efficient enantio-conversion can be achieved. Our method works in the appearance of decoherences and without the precise control of pulse durations (pulse areas) or pulse shapes. These advantages offer it promising features in promoting the future exploration of enantio-conversion.
Abstract Laser-assisted enantio-conversion is an ambitious issue related to chiral molecules in atomic, molecular, and optical physics. The theoretical laser-distillation method was proposed to realize enantio-conversion based on a four-level double-Δ model of two degenerated chiral ground states and two achiral excited states. Here, we re-investigate and improve the laser-distillation method so that a chiral mixture can be converted to an enantiopure sample of the desired chirality, i.e. complete enantio-conversion, which has not been discussed in previous theoretical works on the laser-distillation method. Since the undesired chirality may be inefficient, or even cause serious side effects in pharmacology, our work provides an important improvement to the original theoretical works on laser-assisted enantio-conversion.
We propose an interesting method for the fast enantioconversion of chiral mixtures, leveraging a modified four-level double-Δ model that operates entirely through coherent interactions. By simplifying the model to an effective two-level system, we eliminate the need for intermediate achiral excited states and their associated time-consuming relaxation steps. This approach accelerates enantioconversion by directly evolving the two chiral ground states through population transfer, offering a more efficient alternative to traditional methods such as laser distillation. Our method, which obviates the need for precise pulse shape control, enables highly efficient enantiomeric conversion on the microsecond timescale. This improvement is particularly beneficial in experimental conditions with limited operational time or short enantiomeric lifetimes, making it a powerful tool for enantioconversion of chiral mixtures.
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 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.
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.