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arXiv:0712.3722 · Physical Review A

Dynamic method to distinguish between left- and right-handed chiral molecules

Yong Li, Christoph Bruder

Published Jan 18, 2008• 69 citations
arXivHTMLPDF

Abstract

We study quantum systems with broken symmetry that can be modeled as cyclic three-level atoms with coexisting one- and two-photon transitions. They can be selectively optically excited to any state. As an example, we show that left- and right-handed chiral molecules starting in the same initial states can evolve into different final states by a purely dynamic transfer process. That means that left- and right-handed molecules can be distinguished purely dynamically.

DOI
10.1103/physreva.77.015403

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We study quantum systems with broken symmetry that can be modeled as cyclic three-level atoms with coexisting one- and two-photon transitions. They can be selectively optically excited to any state. As an example, we show that left- and right-handed chiral molecules starting in the same initial states can evolve into different final states by a purely dynamic transfer process. That means that left- and right-handed molecules can be distinguished purely dynamically.
We propose a streamlined method of fast enantiomer-specific state transfer (ESST) of chiral molecules in cyclic three-level systems. Such three-level enantiomers are chirality-dependent systems driven by one of the three Rabi frequencies differing with a sign for the left- and right-handed chiral molecules. When the Hamiltonian of the three-level chiral molecules possesses the specific SU(2) algebraic structure, the populations transferred to the two excited states are shown to be exchanged between the left- and right-handed chiral molecules if they are initially prepared in their ground states. By employing unitary SU(2) transformation and inversely engineering time-dependent Hamiltonians with designed Rabi frequencies, we can make the left- and right-handed chiral molecules evolve respectively to different excited states from their initial ground states simultaneously. Thus a fast ESST is achieved.
The optical bistability (OB) and multistability (OM) in chiral molecules are investigated by placing the sample into a unidirectional ring cavity. Because of broken mirror symmetry of the effective potential, the chiral molecules have a cyclic three-level Δ-configuration structure, in which one- and two-photon transitions can coexist. We find that the OB is achievable in this system on exact one-, two- and three-photon resonance conditions but absent in the three-level Λ-type system under the two-photon resonance. Moreover, the OM and the switching between OB and OM are also realized by choosing parameters properly. Interestingly, the left- and right-handed chiral molecules exhibit different bistable and multistable behaviors. It is shown that the threshold intensity of OB is strongly dependent on the percentage of the two enantiomers in the mixture. This provides an effective approach to probe molecular chirality and to determine enantiomer excess, which may find potential application in organic chemistry, pharmacology, biochemistry, etc..
Enantiomers are chiral molecules that exist in right-handed and left-handed conformations. Optical techniques of enantiomers' detection are widely employed to discriminate between left- and right-handed molecules. However, identical spectra of enantiomers make enantiomer detection a very challenging task. Here, we investigate the possibility of exploiting thermodynamic processes for enantiomer detection. In particular, we employ a quantum Otto cycle in which a chiral molecule described by a three-level system with cyclic optical transitions is considered a working medium. Each energy transition of the three-level system is coupled with an external laser drive. We find that the left- and right-handed enantiomers operate as a quantum heat engine and a thermal accelerator, respectively, when the overall phase is the control parameter. In addition, both enantiomers act as heat engines by keeping the overall phase constant and using the laser drives' detuning as the control parameter during the cycle. However, the molecules can still be distinguished because both cases' extracted work and efficiency are quantitatively very different. Accordingly, the left- and right-handed molecules can be distinguished by evaluating the work distribution in the Otto cycle.
A highly efficient method for optical or microwave detection and separation of left- and right-handed chiral molecules is proposed. The method utilizes a closed-loop three-state system in which the population dynamics depends on the phases of the three couplings. Because of the different signs of the coupling between two of the states for the opposite chiralities the population dynamics is chirality dependent. By using the "shortcuts to adiabaticity" concept applied to the stimulated Raman adiabatic passage technique, one can achieve 100% contrast between the two enantiomers in the population of a particular state. It can be probed by light-induced fluorescence for large ensembles or through resonantly enhanced multiphoton ionization for single molecules.
We propose an accurate and convenient method to achieve 100% discrimination of chiral molecules with Lewis-Riesenfeld invariance. By reversely designing the pulse scheme of handed resolution, we obtain the parameters of the three-level Hamiltonians to achieve this goal. For the same initial state, we can completely transfer its population to one energy level for left-handed molecules, while transferring it to another energy level for right-handed molecules. Moreover, this method can be further optimized when errors exist, and it shows that the optimal method is more robust against these errors than the counterdiabatic and original invariant-based shortcut schemes. This provides an effective, accurate, and robust method to distinguish the handedness of molecules.