Related papers: Unified Formulation of Phase Space Mapping Approac…
We show that a novel, general phase space mapping Hamiltonian for nonadiabatic systems, which is reminiscent of the renowned Meyer-Miller mapping Hamiltonian, involves a commutator variable matrix rather than the conventional…
We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…
Mixed-quantum-classical molecular dynamics simulation implies an effective measurement on the electronic states owing to continuously tracking the atomic forces.Based on this insight, we propose a quantum trajectory mean-field approach for…
We propose a new unified theoretical framework to construct equivalent representations of the multi-state Hamiltonian operator and present several approaches for the mapping onto the Cartesian phase space. After mapping an F-dimensional…
Reliable trajectory-based nonadiabatic quantum dynamics methods at the atomic level are critical for understanding many important processes in real systems. The paper reports latest progress of nonadiabatic field (NaF), a conceptually novel…
A single-loop scenario is proposed to realize nonadiabatic geometric quantum computation. Conventionally, a so-called multi-loop approach is used to remove the dynamical phase accumulated in the operation process for geometric quantum…
Chemical relaxation phenomena, including photochemistry and electron transfer processes, form a vigorous area of research in which nonadiabatic dynamics plays a fundamental role. Here, we show that for nonadiabatic dynamics with two…
We report recent progress on the phase space formulation of quantum mechanics with coordinate-momentum variables, focusing more on new theory of (weighted) constraint coordinate-momentum phase space for discrete-variable quantum systems.…
This work identifies geometric effects on dynamics due to nonadiabatic couplings in Born Oppenheimer systems and provides a systematic method for deriving corrections to mixed quantum-classical methods. Specifically, an exact path integral…
We describe a path-integral approach for including nuclear quantum effects in non-adiabatic chemical dynamics simulations. For a general physical system with multiple electronic energy levels, a corresponding isomorphic Hamiltonian is…
The celebrated Meyer-Miller mapping model has been a useful approach for generating practical trajectory-based nonadiabatic dynamics methods. It is generally assumed that the zero-point-energy (ZPE) parameter is positive. The constraint…
In this paper, we derive universal nonadiabatic passages in a general $M+N$-dimensional discrete system, where $M$ and $N$ denote the degrees of freedom for the assistant and working subspaces, respectively, that could be separated by…
We address the nonadiabatic quantum dynamics of macrosystems with several coupled electronic states, taking into account the possibility of multi-state conical intersections. The general situation of an arbitrary number of states and…
The geometric phase stands as a foundational concept in quantum physics, revealing deep connections between geometric structures and quantum dynamical evolution. Unlike dynamical phases, geometric phases exhibit intrinsic resilience to…
On-the-fly quantum nonadiabatic dynamics for large systems greatly benefits from the adiabatic representation readily available from the electronic structure programs. However, frequently occurring in this representation conical…
Nonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be carried out in a practical manner using…
In this article we show how Ehrenfest mean field theory can be made both a more accurate and efficient method to treat nonadiabatic quantum dynamics by combining it with the generalized quantum master equation framework. The resulting mean…
The theoretical investigation of non-adiabatic processes is hampered by the complexity of the coupled electron-nuclear dynamics beyond the Born-Oppenheimer approximation. Classically, the simulation of such reactions is limited by the…
We develop a unified quantum geometric framework to understand reactive quantum dynamics. The critical roles of the quantum geometry of adiabatic electronic states in both adiabatic and non-adiabatic quantum dynamics are unveiled. A…
We present the formulation of the problem of the coherent dynamics of quantum mechanical two-level systems in the adiabatic region in terms of the differential geometry of plane curves. We show that there is a natural plane curve…