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arXiv:1202.2693 · Physical Review A

Multistate transitions and quantum oscillations of optical activity

Celia Blanco, David Hochberg

Published Feb 10, 2012• 1 citation
arXivHTMLPDF

Abstract

We consider the effects of multistate transitions on the tunneling racemization of chiral molecules. This requires going beyond simple two-state models of enantiomers and to include transitions within a multiple-level quantum-mechanical system. We derive an effective two-level description which accounts for transitions from the enantiomers to an arbitrary number of excited states as an application of the Weisskopf-Wigner approximation scheme. Modifications to the optical activity from these additional states are considered in general terms under the assumption of CPT invariance and then under $T$ invariance. Some formal dynamical analogies between enantiomers and the neutral $K$-meson system are discussed.

DOI
10.1103/physreva.85.022114

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We consider the effects of multistate transitions on the tunneling racemization of chiral molecules. This requires going beyond simple two-state models of enantiomers and to include transitions within a multiple-level quantum-mechanical system. We derive an effective two-level description which accounts for transitions from the enantiomers to an arbitrary number of excited states as an application of the Weisskopf-Wigner approximation scheme. Modifications to the optical activity from these additional states are considered in general terms under the assumption of CPT invariance and then under TTT invariance. Some formal dynamical analogies between enantiomers and the neutral KKK-meson system are discussed.
We study in the framework of the Schrodinger equation the effect of intermolecular interactions on the tunneling racemization of the active molecule. The active molecule is assumed as a two-level system and the left-right isomerism is viewed in terms of a double-bottomed harmonic potential well. The active molecule is assumed to be embedded in a gas, liquid or solid, submitted to a perturbing potential U created by the molecules of the sample. In our model we take into account the difference of energy E due to the weak interactions between the left (L) and right (R) configurations. We have shown that when E is equal to zero the system cannot be optically stable: the optical activity tends asymptotically to zero in the case of dilute gases or compressed gases and liquids or oscillates periodically around zero when the molecules are isolated or submitted to a static potential. Only when E is different of zero the system can be optically stable depending on the strength parameters of the potential U and on the magnitude of the spontaneous tunneling.
Controlling the internal quantum states of chiral molecules for a selected enantiomer has a wide range of fundamental applications. Using tailored microwave fields, a chosen rotational state can be enriched for a selected enantiomer, even starting from a racemic mixture. This enables rapid switching between samples of different enantiomers in a given state, holding great promise, for instance, for measuring parity violation in chiral molecules. Achieving full enantiomer-specific state transfer is a key requirement for this and many other applications. Although theoretically feasible, achieving the required experimental conditions seemed unrealistic. Here, we realize near-ideal conditions, overcoming both the limitations of thermal population and spatial degeneracy in rotational states. Our results show that 96% state-specific enantiomeric purity can be obtained from a racemic mixture, in an approach that is universally applicable to all chiral molecules of C1 symmetry.
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..
This is the second in a series of three papers on nonlinear resonance effects in multilevel quantum systems in which quantum-mechanical systems are considered that are under the influence of any number of classically described driving fields (well defined in amplitude and phase) and are in weak contact with a thermal reservoir, such that relaxation may be described by means of phenomenological decay constants. In the first paper, referred to as I, a projection-operator formalism was developed for separating the equation of motion for the density operator into a part which may be treated by conventional time-dependent perturbation techniques and another part which, because it would give rise to secular terms using a time-dependent perturbation theory, must be treated by more exact means. In this paper three applications of the formalism developed in I are considered. The first application is to a system in which a multiple-quantum transition is taking place between two levels of the system which contains many levels between the two levels under consideration. In particular, the transition probability is calculated for these two levels, which are not directly connected by matrix elements of the interaction but are connected indirectly through intermediate states. The next application considered is the Raman effect in a four-level system. As a final application of the formalism developed in I an expression is derived for the magnetization M+(t)=Mx(t)+iMy(t){M}_{+}(t)={M}_{x}(t)+i{M}_{y}(t)M+​(t)=Mx​(t)+iMy​(t) of a system of NNN noninteracting spins under the influence of a static field in the zzz direction and an arbitrary number of rf fields in the xxx direction. As in I, a phenomenological form is assumed for the relaxation in all of these applications. It is shown in this problem that fields which are not involved in directly causing transitions in this system give rise to frequency shifts in the resonance conditions, which are accounted for in this treatment in a very natural and straightforward manner. For these fields, the rotating as well as the counter-rotating fields give shifts in the resonance condition.
In this review, the concepts of quantum tunneling and parity violation are introduced in the context of chiral molecules. A particle moving in a double well potential provides a good model to study the behavior of chiral molecules, where the left well and right well represent the L and R enantiomers, respectively. If the model considers the quantum behavior of matter, the concept of quantum tunneling emerges, giving place to stereomutation dynamics between left- and right-handed chiral molecules. Parity-violating interactions, like the electroweak one, can be also considered, making possible the existence of an energy difference between the L and R enantiomers, the so-called parity-violating energy difference (PVED). Here we provide a brief account of some theoretical methods usually employed to calculate this PVED, also commenting on relevant experiments devoted to experimentally detect the aforementioned PVED in chiral molecules. Finally, we comment on some ways of solving the so-called Hund’s paradox, with emphasis on mean-field theory and decoherence.
Based on cyclic three-level systems of chiral molecules, we propose two methods to realize highly efficient inner-state enantioseparations of a chiral mixture with the two enantiomers initially prepared in their ground states. Our methods work in the region where the evolutions of the two enantiomers can be described by their corresponding effective two-level models, simultaneously. The approximately 100100%100-efficiency inner-state enantioseparations can be realized when the probability occupying the ground state of one enantiomer becomes zero by experiencing half-integer periods of its corresponding on-resonance Rabi oscillation and the other one stays always in the ground state approximately, under the conditions that the two enantiomers are governed by the effective on-resonance and large-detuning two-level models, respectively. Alternatively, the exactly 100100%100-efficiency inner-state enantioseparation can be obtained when the probability occupying the ground state of one enantiomer becomes zero by experiencing half-integer periods of its corresponding on-resonance Rabi oscillation and in the meanwhile that of the other one becomes 1 by experiencing integer periods of its corresponding detuned Rabi oscillation, respectively.