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arXiv:1911.07376 · Physical Review Research

Fast enantioconversion of chiral mixtures based on a four-level double- Δ model

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

Published Jul 14, 2020• 26 citations
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Abstract

The authors propose a fast method for enantioconversion based on a four-level double-$\mathrm{\ensuremath{\Delta}}$ model. By designing the applied electromagnetic fields, the four-level double-$\mathrm{\ensuremath{\Delta}}$ model can be simplified to two effective two-level sub-systems. Upon this, after three coherent operations, the initial chiral mixture can be converted to the enantiopure sample

DOI
10.1103/physrevresearch.2.033064

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The authors propose a fast method for enantioconversion based on a four-level double-\ensuremathΔ\mathrm{\ensuremath{\Delta}}\ensuremathΔ model. By designing the applied electromagnetic fields, the four-level double-\ensuremathΔ\mathrm{\ensuremath{\Delta}}\ensuremathΔ model can be simplified to two effective two-level sub-systems. Upon this, after three coherent operations, the initial chiral mixture can be converted to the enantiopure sample
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.
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.
Enantiospecific state transfer of chiral molecules is extremely important because enantiomers coexist in many biologically active compounds and play significantly different physiological, pharmacological, and biological roles. The inherently strong electric-dipole optical approaches based on the cyclic three-level model of chiral molecules have been extensively discussed. But, for the cases of large chiral molecules and/or chiral molecules of low asymmetry, the four-level model with two sub-loops is more realistic to describe the molecules. Based on the four-level model, we propose a pump-control approach to realize the highly efficient enantiospecific state transfer. In our approach, two pump pulses are applied to generate molecular coherence between the ground state and the first excited state of our working model. According to the coherence of the molecules, we adjust the phase and pulse area of the control pulse, then we obtain the highly efficient enantiospecific state transfer in the first excited working state. In addition, we further optimize the fraction of enantiopure samples by adjusting the area of the two pump pulses.
We study the enantiospecific state transfer for gaseous symmetric-top chiral molecules by constructing a four-level model. This model is formed by coupling the electric dipole transitions among four appropriate rovibrational states with three electromagnetic fields. It includes two cyclic three-level substructures, where the overall phases of the coupling strengths differ by $\ensuremath{\pi}$ with enantiomers and reflect the chirality dependence of the molecules. Based on this four-level model, two dynamic ways are proposed to achieve the approximately perfect enantiospecific state transfer for gaseous symmetric-top chiral molecules when all the molecules are initially in the ground state of the system.
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.
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.