Enantioselective Quantum Optical Effects in Chiral Molecules

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 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.

Physical Review AFeb 20, 20240 citations

Chiral quantum optics

Peter Lodahl, Sahand Mahmoodian, Søren Stobbe +5 more

arXiv:1608.00446NatureJan 1, 20171,631 citations

Chiral quantum optics with giant atoms

Ariadna Soro Álvarez, Anton Frisk Kockum

Bulletin of the American Physical SocietyMar 17, 20210 citations

Enantioselective switch on radiations of dissipative chiral molecules

Ye, Chong, Mu, Xiaowei, Yifan Sun +2 more

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.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.

arXiv:2211.15112Nov 28, 20220 citations

Laser-driven coherent manipulation of molecular chirality

Ioannis Thanopulos, Emmanuel Paspalakis, Z. Kis

Chemical Physics LettersApr 29, 200424 citations

Cyclic three-level-pulse-area theorem for enantioselective state transfer of chiral molecules

Yu Guo, Xun Gong, Songshan Ma +1 more

We derive a pulse-area theorem for a single-loop cyclic three-level system without applying the rotating-wave approximation while explicitly taking into account the time delays of control fields. This corresponds to an archetypal model for exploring enantioselective state transfer (ESST) in chiral molecules driven by three linearly polarized microwave pulses. By dividing the closed-loop excitation into two separate stages, we obtain both amplitude and phase conditions of three control fields to generate high fidelity of ESST. As a proof of principle, we apply this pulse-area theorem to cyclohexylmethanol molecules, for which three rotational states are connected by $a$ -type, $b$ -type, and $c$ -type components of the transition dipole moments in both center-frequency-resonant and -detuned conditions. Our results show that two enantiomers with opposite handedness can be transferred to different target states by designing three microwave pulses that satisfy the amplitude and phase conditions at the transition frequencies. The corresponding control schemes are robust against the time delays between the two stages. We suggest that the two control fields used in the second stage should be applied simultaneously for practical applications. This work contributes an alternative pulse-area theorem to the field of quantum control, which has the potential to determine the chirality of enantiomers in a mixture.We derive a pulse-area theorem for a single-loop cyclic three-level system without applying the rotating-wave approximation while explicitly taking into account the time delays of control fields. This corresponds to an archetypal model for exploring enantioselective state transfer (ESST) in chiral molecules driven by three linearly polarized microwave pulses. By dividing the closed-loop excitation into two separate stages, we obtain both amplitude and phase conditions of three control fields to generate high fidelity of ESST. As a proof of principle, we apply this pulse-area theorem to cyclohexylmethanol molecules, for which three rotational states are connected by $a$-type, $b$-type, and $c$-type components of the transition dipole moments in both center-frequency-resonant and -detuned conditions. Our results show that two enantiomers with opposite handedness can be transferred to different target states by designing three microwave pulses that satisfy the amplitude and phase conditions at the transition frequencies. The corresponding control schemes are robust against the time delays between the two stages. We suggest that the two control fields used in the second stage should be applied simultaneously for practical applications. This work contributes an alternative pulse-area theorem to the field of quantum control, which has the potential to determine the chirality of enantiomers in a mixture.

arXiv:2110.09031Physical Review AJan 3, 202231 citations

a

-type,

b

-type, and

c

-type components of the transition dipole moments in both center-frequency-resonant and -detuned conditions. Our results show that two enantiomers with opposite handedness can be transferred to different target states by designing three microwave pulses that satisfy the amplitude and phase conditions at the transition frequencies. The corresponding control schemes are robust against the time delays between the two stages. We suggest that the two control fields used in the second stage should be applied simultaneously for practical applications. This work contributes an alternative pulse-area theorem to the field of quantum control, which has the potential to determine the chirality of enantiomers in a mixture.