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In this paper, we present an extended dissipaton equation of motion for studying the dynamics of electronic impurity systems. Compared with the original theoretical formalism, the quadratic couplings are introduced into the Hamiltonian accounting for the interaction between the impurity and its surrounding environment. By exploiting the quadratic fermionic dissipaton algebra, the proposed extended dissipaton equation of motion offers a powerful tool for studying the dynamical behaviors of electronic impurity systems, particularly in situations where nonequilibrium and strongly correlated effects play significant roles. Numerical demonstrations are carried out to investigate the temperature dependence of the Kondo resonance in the Kondo impurity model.
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http://dx.doi.org/10.1063/5.0155585 | DOI Listing |
J Chem Phys
June 2025
Hefei National Research Center for Physical Sciences at the Microscale and Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
Understanding the effects of vibrations in electron transfer (ET) dynamics and optical spectroscopies is essential to precisely interpret the role of decoherence, especially for systems embedded in solvents. In this work, we study the correlated Duschinsky and solvent effects on ET and spectroscopy. Exploited is a novel extended dissipaton-equation-of-motion approach, which is an exact and non-Markovian, non-perturbative method for quadratic system-bath couplings.
View Article and Find Full Text PDFJ Chem Theory Comput
April 2025
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
In this paper, we present the extended dissipaton theory, including the dissipaton-equation-of-motion formalism and the equivalent dissipaton-embedded quantum master equation. These are exact, non-Markovian, and nonperturbative theories, capable of handling not only linear but also quadratic environmental couplings. These scenarios are prevalent in a variety of strongly correlated electronic systems, including mesoscopic nanodevices and superconductors.
View Article and Find Full Text PDFJ Chem Phys
October 2024
Department of Chemistry, University of Rochester, 120 Trustee Road, Rochester, New York 14627, USA.
We investigate the quantum dynamics of a spin coupling to a bath of independent spins via the dissipaton equation of motion (DEOM) approach. The bath, characterized by a continuous spectral density function, is composed of spins that are independent level systems described by the su(2) Lie algebra, representing an environment with a large magnitude of anharmonicity. Based on the previous work by Suarez and Silbey [J.
View Article and Find Full Text PDFJ Chem Phys
July 2024
Department of Chemistry, School of Science and Research Center for Industries of the Future, Westlake University, Hangzhou, Zhejiang 310024, China.
Fermi's golden rule (FGR) offers an empirical framework for understanding the dynamics of spin-lattice relaxation in magnetic molecules, encompassing mechanisms like direct (one-phonon) and Raman (two-phonon) processes. These principles effectively model experimental longitudinal relaxation rates, denoted as T1-1. However, under scenarios of increased coupling strength and nonlinear spin-lattice interactions, FGR's applicability may diminish.
View Article and Find Full Text PDFJ Chem Phys
July 2023
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui 230026, China.
In this paper, we present an extended dissipaton equation of motion for studying the dynamics of electronic impurity systems. Compared with the original theoretical formalism, the quadratic couplings are introduced into the Hamiltonian accounting for the interaction between the impurity and its surrounding environment. By exploiting the quadratic fermionic dissipaton algebra, the proposed extended dissipaton equation of motion offers a powerful tool for studying the dynamical behaviors of electronic impurity systems, particularly in situations where nonequilibrium and strongly correlated effects play significant roles.
View Article and Find Full Text PDF