Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

The Journal of Physical Chemistry B

Combining Lindblad Master Equation and Surface Hopping to Evolve Distributions of Quantum Particles

Yi-Siang Wang, Parmeet Nijjar, Xin Zhou, Denys I. Bondar, Oleg V. Prezhdo

Published May 4, 2020• 25 citations
Publisher

Abstract

Motivated by the need to study nonequilibrium evolutions of many-electron systems at the atomistic ab initio level, as they occur in modern devices and applications, we developed a quantum dynamics approach bridging master equations and surface hopping (SH). The Lindblad master equation (LME) allows us to propagate efficiently ensembles of particles, while SH provides nonperturbative evaluation of transition rates that evolve in time and depend explicitly on nuclear geometry. We implemented the LME-SH technique within real-time time-dependent density functional theory using global flux SH, and we demonstrated its efficiency and utility by modeling metallic films, in which charge-phonon dynamics was studied experimentally and showed an unexpectedly strong dependence on adhesion layers. The LME-SH approach provides a general framework for modeling efficiently quantum dynamics in a broad range of complex many-electron condensed-matter and nanoscale systems.

DOI
10.1021/acs.jpcb.0c03030

Related papers

Surface hopping with a manifold of electronic states. II. Application to the many-body Anderson-Holstein model

Wenjie Dou, Abraham Nitzan, Joseph Eli Subotnik

We investigate a simple surface hopping (SH) approach for modeling a single impurity level coupled to a single phonon and an electronic (metal) bath (i.e., the Anderson-Holstein model). The phonon degree of freedom is treated classically with motion along--and hops between--diabatic potential energy surfaces. The hopping rate is determined by the dynamics of the electronic bath (which are treated implicitly). For the case of one electronic bath, in the limit of small coupling to the bath, SH recovers phonon relaxation to thermal equilibrium and yields the correct impurity electron population (as compared with numerical renormalization group). For the case of out of equilibrium dynamics, SH current-voltage (I-V) curve is compared with the quantum master equation (QME) over a range of parameters, spanning the quantum region to the classical region. In the limit of large temperature, SH and QME agree. Furthermore, we can show that, in the limit of low temperature, the QME agrees with real-time path integral calculations. As such, the simple procedure described here should be useful in many other contexts.

The Journal of Chemical Physics•Feb 25, 2015•60 citations

Open quantum-classical systems: A hybrid MASH master equation

Kasra Asnaashari, Jeremy O. Richardson

We propose a method which combines the quantum-classical mapping approach to surface hopping (MASH) with the dissipative quantum dynamics of the Lindblad master equation. Like conventional surface-hopping methods, our approach is based on classical trajectories coupled to the dynamics of a quantum subsystem. However, instead of evolving the subsystem wavefunction according to the time-dependent Schrödinger equation, we use stochastic quantum trajectories derived from secular Redfield theory. This enables the simulation of open quantum systems coupled simultaneously to Markovian quantum baths and anharmonic non-Markovian classical degrees of freedom. Applications to the spin--boson model and to the cavity-enhanced fluorescence of an electronically nonadiabatic molecule show excellent agreement with fully quantum-mechanical benchmarks.

quant-pharXiv:2511.05282•The Journal of Chemical Physics•Nov 10, 2025•2 citations

Quantum-Classical Master Equation Dynamics: An Analysis of Decoherence and Surface-hopping Techniques

Robbie Grunwald

In this thesis quantum-classical dynamics is applied to the study of quantum condensed phase processes. This approach is based on the quantum-classical Liouville equation where the dynamics of a small subset of the degrees of freedom are treated quantum mechanically while the remaining degrees of freedom are treated by classical mechanics to a good approximation. We use this approach as it is computationally tractable, and the resulting equation of motion accurately accounts for the quantum and classical dynamics, as well as the coupling between these two components of the system. \n\nBy recasting the quantum-classical Liouville equation into the form of a generalized master equation we investigate connections to surface-hopping. The link between these approaches is decoherence arising from interaction of the subsystem with the environment. We derive an evolution equation for the subsystem which contains terms accounting for the effects of the environment. One of these terms involves a memory kernel that accounts for the coherent dynamics. If this term decays rapidly, a Markovian approximation can be made. By lifting the resulting subsystem master equation into the full phase space, we obtain a Markovian master equation that prescribes surface-hopping-like dynamics. Our analysis outlines the conditions under which such a description is valid.\n\nNext, we consider the calculation of the rate constant for a quantum mechanical barrier crossing process. Starting from the reactive-flux autocorrelation function, we derive a quantum-classical expression for the rate kernel. This expression involves quantum-classical evolution of a species operator averaged over the initial quantum equilibrium structure of the system making it possible to compute the rate constant via computer simulation. Using a simple model for a proton transfer reaction we compare the results of the rate calculation obtained by quantum-classical Liouville dynamics with that of master equation dynamics. The master equation provides a good approximation to the full quantum-classical Liouville calculation for our model and a more stable algorithm results due to the elimination of oscillating phase factors in the simulation. \n\nFinally, we make use of the theoretical framework established in this thesis to analyze some aspects of decoherence used in popular surface-hopping techniques.

•Jan 19, 2009•0 citations

Complex non-Hermitian Potentials and Real-Time Time-Dependent Density Functional Theory: A Master Equation Approach

Justin E. Elenewski, Yanxiang Zhao, Hanning Chen

The simulation of quantum transport in a realistic, many-particle system is a nontrivial problem with no quantitatively satisfactory solution. While real-time propagation has the potential to overcome the shortcomings of conventional transport methods, this approach is prone to finite size effects that are associated with modeling an open system on a closed spatial domain. Using a master equation framework, we exploit an equivalence between the superoperators coupling an open system to external particle reservoirs and non-Hermitian terms defined at the periphery of a quantum device. By taking the mean-field limit, the equation of motion for the single-particle reduced density matrix becomes equivalent to real-time time-dependent density functional theory in the presence of imaginary source and sink potentials. This method may be used to converge nonequilibrium steady states for a many-body quantum system using a previously reported constraint algorithm.

arXiv:1510.04308•Oct 14, 2015•0 citations

Quantum Master Equations: Tips and Tricks for Quantum Optics, Quantum Computing, and Beyond

Francesco Campaioli, Jared H. Cole, Harini Hapuarachchi

Quantum master equations are an invaluable tool to model the dynamics of a plethora of microscopic systems, ranging from quantum optics and quantum information processing to energy and charge transport, electronic and nuclear spin resonance, photochemistry, and more. This tutorial offers a concise and pedagogical introduction to quantum master equations, accessible to a broad, cross-disciplinary audience. The reader is guided through the basics of quantum dynamics with hands-on examples that increase in complexity. The tutorial covers essential methods such as the use of the Lindblad master equation, Redfield relaxation, and Floquet theory, as well as techniques such as Suzuki-Trotter expansion and numerical approaches for sparse solvers. These methods are illustrated with code snippets implemented in and other languages, which can be used as a starting point for generalization and more sophisticated implementations. Published by the American Physical Society 2024

arXiv:2303.16449•PRX Quantum•Jun 10, 2024•89 citations

Lindbladian dynamics with loss of quantum jumps

Yu-Guo Liu, Shu Chen

The Lindblad master equation (LME) describing the Markovian dynamics of the quantum open system can be understood as the evolution of the effective non-Hermitian Hamiltonian balanced with random quantum jumps. Here we investigate the balance-breaking dynamics by partly eliminating jumps from postselection experiments. To describe this dynamics, a nonlinear Lindblad master equation (NLME) is derived from the quantum trajectory method. However, the NLME shows significant advantages in analytical analysis over the quantum trajectory method. Using the NLME, we classify the dynamics into two classes. In the trivial class, the process of reducing jumps is completely equivalent to weakening the coupling from the environment. In contrast, the nontrivial class presents more complex dynamics. We study a prototypical model within this class and demonstrate the existence of the postselected skin effect whose steady state is characterized by the accumulation of particles on one side. The steady-state distribution can be fitted by a scale-invariant tanh function which is different from the uniform distribution of LME. Furthermore, the NLME can give a reasonable framework for studying the interplay and competition between the non-Hermitian Hamiltonians and dissipative terms. We show this by capturing the characteristics of the trajectory-averaged entanglement entropy influenced by non-Hermitian skin effect and Zeno effect in the model of postselected skin effect.

arXiv:2405.11812•Physical review. B./Physical review. B•Jan 7, 2025•12 citations
Motivated by the need to study nonequilibrium evolutions of many-electron systems at the atomistic ab initio level, as they occur in modern devices and applications, we developed a quantum dynamics approach bridging master equations and surface hopping (SH). The Lindblad master equation (LME) allows us to propagate efficiently ensembles of particles, while SH provides nonperturbative evaluation of transition rates that evolve in time and depend explicitly on nuclear geometry. We implemented the LME-SH technique within real-time time-dependent density functional theory using global flux SH, and we demonstrated its efficiency and utility by modeling metallic films, in which charge-phonon dynamics was studied experimentally and showed an unexpectedly strong dependence on adhesion layers. The LME-SH approach provides a general framework for modeling efficiently quantum dynamics in a broad range of complex many-electron condensed-matter and nanoscale systems.
We investigate a simple surface hopping (SH) approach for modeling a single impurity level coupled to a single phonon and an electronic (metal) bath (i.e., the Anderson-Holstein model). The phonon degree of freedom is treated classically with motion along--and hops between--diabatic potential energy surfaces. The hopping rate is determined by the dynamics of the electronic bath (which are treated implicitly). For the case of one electronic bath, in the limit of small coupling to the bath, SH recovers phonon relaxation to thermal equilibrium and yields the correct impurity electron population (as compared with numerical renormalization group). For the case of out of equilibrium dynamics, SH current-voltage (I-V) curve is compared with the quantum master equation (QME) over a range of parameters, spanning the quantum region to the classical region. In the limit of large temperature, SH and QME agree. Furthermore, we can show that, in the limit of low temperature, the QME agrees with real-time path integral calculations. As such, the simple procedure described here should be useful in many other contexts.
We propose a method which combines the quantum-classical mapping approach to surface hopping (MASH) with the dissipative quantum dynamics of the Lindblad master equation. Like conventional surface-hopping methods, our approach is based on classical trajectories coupled to the dynamics of a quantum subsystem. However, instead of evolving the subsystem wavefunction according to the time-dependent Schrödinger equation, we use stochastic quantum trajectories derived from secular Redfield theory. This enables the simulation of open quantum systems coupled simultaneously to Markovian quantum baths and anharmonic non-Markovian classical degrees of freedom. Applications to the spin--boson model and to the cavity-enhanced fluorescence of an electronically nonadiabatic molecule show excellent agreement with fully quantum-mechanical benchmarks.
In this thesis quantum-classical dynamics is applied to the study of quantum condensed phase processes. This approach is based on the quantum-classical Liouville equation where the dynamics of a small subset of the degrees of freedom are treated quantum mechanically while the remaining degrees of freedom are treated by classical mechanics to a good approximation. We use this approach as it is computationally tractable, and the resulting equation of motion accurately accounts for the quantum and classical dynamics, as well as the coupling between these two components of the system. \n\nBy recasting the quantum-classical Liouville equation into the form of a generalized master equation we investigate connections to surface-hopping. The link between these approaches is decoherence arising from interaction of the subsystem with the environment. We derive an evolution equation for the subsystem which contains terms accounting for the effects of the environment. One of these terms involves a memory kernel that accounts for the coherent dynamics. If this term decays rapidly, a Markovian approximation can be made. By lifting the resulting subsystem master equation into the full phase space, we obtain a Markovian master equation that prescribes surface-hopping-like dynamics. Our analysis outlines the conditions under which such a description is valid.\n\nNext, we consider the calculation of the rate constant for a quantum mechanical barrier crossing process. Starting from the reactive-flux autocorrelation function, we derive a quantum-classical expression for the rate kernel. This expression involves quantum-classical evolution of a species operator averaged over the initial quantum equilibrium structure of the system making it possible to compute the rate constant via computer simulation. Using a simple model for a proton transfer reaction we compare the results of the rate calculation obtained by quantum-classical Liouville dynamics with that of master equation dynamics. The master equation provides a good approximation to the full quantum-classical Liouville calculation for our model and a more stable algorithm results due to the elimination of oscillating phase factors in the simulation. \n\nFinally, we make use of the theoretical framework established in this thesis to analyze some aspects of decoherence used in popular surface-hopping techniques.
The simulation of quantum transport in a realistic, many-particle system is a nontrivial problem with no quantitatively satisfactory solution. While real-time propagation has the potential to overcome the shortcomings of conventional transport methods, this approach is prone to finite size effects that are associated with modeling an open system on a closed spatial domain. Using a master equation framework, we exploit an equivalence between the superoperators coupling an open system to external particle reservoirs and non-Hermitian terms defined at the periphery of a quantum device. By taking the mean-field limit, the equation of motion for the single-particle reduced density matrix becomes equivalent to real-time time-dependent density functional theory in the presence of imaginary source and sink potentials. This method may be used to converge nonequilibrium steady states for a many-body quantum system using a previously reported constraint algorithm.
Quantum master equations are an invaluable tool to model the dynamics of a plethora of microscopic systems, ranging from quantum optics and quantum information processing to energy and charge transport, electronic and nuclear spin resonance, photochemistry, and more. This tutorial offers a concise and pedagogical introduction to quantum master equations, accessible to a broad, cross-disciplinary audience. The reader is guided through the basics of quantum dynamics with hands-on examples that increase in complexity. The tutorial covers essential methods such as the use of the Lindblad master equation, Redfield relaxation, and Floquet theory, as well as techniques such as Suzuki-Trotter expansion and numerical approaches for sparse solvers. These methods are illustrated with code snippets implemented in and other languages, which can be used as a starting point for generalization and more sophisticated implementations. Published by the American Physical Society 2024
The Lindblad master equation (LME) describing the Markovian dynamics of the quantum open system can be understood as the evolution of the effective non-Hermitian Hamiltonian balanced with random quantum jumps. Here we investigate the balance-breaking dynamics by partly eliminating jumps from postselection experiments. To describe this dynamics, a nonlinear Lindblad master equation (NLME) is derived from the quantum trajectory method. However, the NLME shows significant advantages in analytical analysis over the quantum trajectory method. Using the NLME, we classify the dynamics into two classes. In the trivial class, the process of reducing jumps is completely equivalent to weakening the coupling from the environment. In contrast, the nontrivial class presents more complex dynamics. We study a prototypical model within this class and demonstrate the existence of the postselected skin effect whose steady state is characterized by the accumulation of particles on one side. The steady-state distribution can be fitted by a scale-invariant tanh function which is different from the uniform distribution of LME. Furthermore, the NLME can give a reasonable framework for studying the interplay and competition between the non-Hermitian Hamiltonians and dissipative terms. We show this by capturing the characteristics of the trajectory-averaged entanglement entropy influenced by non-Hermitian skin effect and Zeno effect in the model of postselected skin effect.