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The Journal of Chemical Physics

Dissipative geometric phase and decoherence in parity-violating chiral molecules

Anaís Dorta-Urra, H.C. Peñate-Rodríguez, Pedro Bargueño, Germán A. Rojas-Lorenzo, Salvador Miret-Artés

Published May 3, 2012• 17 citations
Publisher

Abstract

Within a generalized Langevin framework for open quantum systems, the cyclic evolution of a two-level system is analyzed in terms of the geometric phase extended to dissipative systems for Ohmic friction. This proposal is applied to the dynamics of chiral molecules where the tunneling and parity violating effects are competing. The effect of different system-bath coupling functions in the dissipated energy is shown to be crucial to understand the behavior of the geometric phase as well as the decoherence displayed by the corresponding interference patterns.

DOI
10.1063/1.4707735

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Within a generalized Langevin framework for open quantum systems, the cyclic evolution of a two-level system is analyzed in terms of the geometric phase extended to dissipative systems for Ohmic friction. This proposal is applied to the dynamics of chiral molecules where the tunneling and parity violating effects are competing. The effect of different system-bath coupling functions in the dissipated energy is shown to be crucial to understand the behavior of the geometric phase as well as the decoherence displayed by the corresponding interference patterns.
Geometric phases are foundational to isolated quantum systems, yet their thermodynamic role in open systems remains unrevealed Developing a dissipative adiabatic perturbation expansion, we discover a Berry-phase-induced chiral work difference that survives decoherence. This chirality evolves from an interferometric thermodynamic Aharonov-Bohm effect in the unitary regime to a fringe-free signal in the dissipative regime. We illustrate this framework in a two-level system and assess its experimental feasibility. Our findings clarify the role of quantum geometry in the geometric formulation of thermodynamics.
A Langevin canonical framework for a chiral two-level system coupled to a bath of harmonic oscillators is used within a coupling scheme different from the well-known spin-boson model to study the quantum stochastic resonance for chiral molecules. This process refers to the amplification of the response to an external periodic signal at a certain value of the noise strength, being a cooperative effect of friction, noise, and periodic driving occurring in a bistable system. Furthermore, from this stochastic dynamics within the Markovian regime and Ohmic friction, the competing process between tunneling and the parity violating energy difference present in this type of chiral systems plays a fundamental role. This mechanism is finally proposed to observe the so-far elusive parity-violating energy difference in chiral molecules.
Dissipative and stochastic effects in the geometric phase of a qubit are taken into account using a geometrical description of the corresponding open-system dynamics within a canonical Langevin framework based on a Caldeira-Leggett-like Hamiltonian. By extending the Hopf fibration ${S}^{3}\ensuremath{\rightarrow}{S}^{2}$ to include such effects, the exact geometric phase for a dissipative qubit is obtained, whereas numerical calculations are used to include finite-temperature effects on it.
Based on a generic quantum open system model, we study the geometric nature of decoherence by defining a complex-valued geometric phase through stochastic pure states describing nonunitary, noncyclic, and nonadiabatic evolutions. The ensemble average of the complex geometric phases for the pure stochastic states yields a conventional geometric phase together with an amplitude factor. We show that the decoherence process described by the decaying amplitude can be a geometric quantity independent of the system's dynamics. It is a remarkable fact that the geometric phase of a quantum system can serve as an ideal realization of quantum gates due to its robustness against dynamical errors; however, in this paper we show that, for some open quantum systems, a desirable geometric phase may be accompanied by an unwanted robust geometric decoherence factor. Two exactly solvable models are studied to demonstrate that, while the decoherence is a purely dynamical effect for a dephasing two-level model, the decoherence in a dissipative two-level model can be a geometric process. Finally, we show that such a geometric decoherence effect may be eliminated by a nonperturbative control scheme.
We describe the decoherence process induced on a two-level quantum system in direct interaction with a nonequilibrium environment. The nonequilibrium feature is represented by a nonstationary random function corresponding to the fluctuating transition frequency between two quantum states coupled to the surroundings. In this framework, we compute the decoherence factors which have a characteristic ``dip'' related to the initial phases of the bath modes. We therefore study different types of environments, namely, ohmic and supraohmic. These environments present different decoherence time scales than the thermal environment we used to study. As a consequence, we compute analytically and numerically the nonunitary geometric phase for the qubit in a quasicyclic evolution under the presence of these particular nonequilibrium environments. We show in which cases decoherence effects could, in principle, be controlled in order to perform a measurement of the geometric phase using standard procedures.
The decoherence of a two-state tunneling molecule, such as a chiral molecule or ammonia, due to collisions with a buffer gas is analyzed in terms of a succession of quantum states of the molecule satisfying the conditions for a consistent family of histories. With $\ensuremath{\hbar}\ensuremath{\omega}$ the separation in energy of the levels in the isolated molecule and $\ensuremath{\gamma}$ a decoherence rate proportional to the rate of collisions, we find for $\ensuremath{\gamma}\ensuremath{\gg}\ensuremath{\omega}$ (strong decoherence) a consistent family in which the molecule flips randomly back and forth between the left- and right-handed chiral states in a stationary Markov process. For $\ensuremath{\gamma}<\ensuremath{\omega}$ there is a family in which the molecule oscillates continuously between the different chiral states, but with occasional random changes of phase, at a frequency that goes to zero at a phase transition $\ensuremath{\gamma}=\ensuremath{\omega}$. This transition is similar to the behavior of the inversion frequency of ammonia with increasing pressure, but will be difficult to observe in chiral molecules such as D2{}_{2}2​S2{}_{2}2​. There are additional consistent families both for $\ensuremath{\gamma}>\ensuremath{\omega}$ and for $\ensuremath{\gamma}<\ensuremath{\omega}$. In addition, we relate the speed with which chiral information is transferred to the environment to the rate of decrease of complementary types of information (e.g., parity information) remaining in the molecule itself.