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Quantum Studies Mathematics and Foundations

Linear response theory for open quantum systems within the framework of the ABL formalism

Masashi Ban

Published Feb 23, 2015• 15 citations
Publisher
DOI
10.1007/s40509-015-0034-x

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The formalism of linear response theory can be extended to encompass physical situations where an open quantum system evolves toward a nonequilibrium steady state. Here, we use the framework put forward by Konopik and Lutz [] to go beyond unitary perturbations of the dynamics. Considering an open system comprised of two coupled quantum harmonic oscillators, we study the system's response to unitary perturbations, affecting the Hamiltonian dynamics, as well as nonunitary perturbations, affecting the properties of the environment, e.g., its temperature and squeezing. We show that linear response, combined with a quantum probing approach, can effectively provide valuable quantitative information about the perturbation and characteristics of the environment, even in cases of nonunitary dynamics. Published by the American Physical Society 2024
Single-Molecule Magnets (SMMs) exhibit slow magnetic relaxation as a result of axial magnetic anisotropy inhibiting spin-phonon transitions. In order to establish a direct link between physical observables and the microscopic theory of magnetic relaxation, we here develop and numerically implement a first-principles linear-response theory for open quantum systems that provides access to the complex a.c. magnetic susceptibility in the presence of an oscillating a.c. magnetic field. Once combined with density functional theory and multiconfigurational electronic structure simulations, this formalism is applied in a fully first-principles fashion to three cyanido-bridged Ln/Y-based coordination polymers with general formula {LnxIII^{III}_xxIII​ Y1−xIII^{III}_{1-x}1−xIII​ [Co(CN)6_66​]}, where Ln = Yb (1), Tb (2), and Dy (3). The method is able to reproduce the low-temperature direct relaxation process and its field dependence, as well as the high-temperature Orbach relaxation regime for all the investigated compounds. These results demonstrate the feasibility of ab initio simulations of magnetic a.c.susceptibility in lanthanide-based SMMs and support the potential of further development of ab initio open quantum systems methods towards the completion of a magnetization dynamics theory.
Dynamical maps are the principal subject of the open system theory. Formally, the dynamical map of a given open quantum system is a density matrix transformation that takes any initial state and sends it to the state at a later time. Physically, it encapsulates the system’s evolution due to coupling with its environment. Hence, the theory provides a flexible and accurate framework for computing expectation values of open system observables. However, expectation values-or more generally, single-time correlation functions-capture only the simplest aspects of a quantum system’s dynamics. A complete characterization of the dynamics requires access to multi-time correlation functions as well: phenomena like detailed balance, linear and non-linear response, non-equilibrium transport in general, or even sequential measurements of system observables are all described in terms of multi-time correlations. For closed systems, such correlations are well-defined, even though knowledge of the system’s state alone is insufficient to determine them fully. In contrast, the standard dynamical map formalism for open systems does not account for multi-time correlations, as it is fundamentally limited to describing state evolution. Here, we extend the scope of open quantum system theory by developing a systematic perturbation theory for computing multi-time correlation functions.