Related papers: Nonadiabatic semiclassical dynamics in the mixed q…
A first principles quantum formalism to describe the non-adiabatic dynamics of electrons and nuclei based on a second quantization representation (SQR) of the electronic motion combined with the usual representation of the nuclear…
A symmetrical quasiclassical (SQC) dynamics approach based on the Li-Miller (LM) mapping Hamiltonian (SQC-LM) was employed to describe nonadiabatic dynamics. In principle, the different initial sampling procedures may be applied in the…
We derive an exact, continuous-variable path integral (PI) representation of the canonical partition function for electronically nonadiabatic systems. Utilizing the Stock-Thoss (ST) mapping for an N-level system, matrix elements of the…
A common strategy to simulate mixed quantum-classical dynamics is by propagating classical trajectories with mapping variables, often using the Meyer-Miller-Stock-Thoss (MMST) Hamiltonian or the related spin-mapping approach. When mapping…
The combined quantum electron-nuclear dynamics is often associated with the Born-Huang expansion of the molecular wave function and the appearance of nonadiabatic effects as a perturbation. On the other hand, native multicomponent…
We present a semiclassical quantization condition, i.e., quantum-classical correspondence, for steady states of nonadiabatic systems consisting of fast and slow degrees of freedom (DOFs) by extending Gutzwiller's trace formula to a…
We propose to measure the importance of spin-orbit couplings (SOCs) in the nonadiabatic molecular quantum dynamics rigorously with quantum fidelity. To make the criterion practical, quantum fidelity is estimated efficiently with the…
One of the open challenges in quantum computing is to find meaningful and practical methods to leverage quantum computation to accelerate classical machine learning workflows. A ubiquitous problem in machine learning workflows is sampling…
We developed a general theoretical approach and a user-ready computer code that permit to study the dynamics of collisional energy transfer and ro-vibrational energy exchange in complex molecule-molecule collisions. The method is a mixture…
Quantum simulation has begun to penetrate the field of quantum chemistry in hopes of efficiently calculating ground state energies and approximating real-time evolution. With modern research highlighting nonadiabatic dynamics, tunably…
Quantum computation is an attractive front for many problems that are intractable for computers today. One such problem is nonadiabatic quantum molecular dynamics, where quantized internal states coupling to parameterized modes result in a…
The mapping approach addresses the mismatch between the continuous nuclear phase space and discrete electronic states by creating an extended, fully continuous phase space using a set of harmonic oscillators to encode the populations and…
Dynamical mean-field theory (DMFT) is a cornerstone technique for studying strongly correlated electronic systems. However, each DMFT step is computationally demanding, and many iterations can be required to achieve convergence. Here, we…
The use of mid-circuit measurement and qubit reset within quantum programs has been introduced recently and several applications demonstrated that perform conditional branching based on these measurements. In this work, we go a step further…
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…
Diabatization of the molecular Hamiltonian is a standard approach to removing the singularities of nonadiabatic couplings at conical intersections of adiabatic potential energy surfaces. In general, it is impossible to eliminate the…
We introduce a new path integral Monte Carlo method for investigating nonadiabatic systems in thermal equilibrium and demonstrate an approach to reducing stochastic error. We derive a general path integral expression for the partition…
In order to alleviate the computational costs of fully quantum nonadiabatic dynamics, we present a mixed quantum-classical (MQC) particle method based on the theory of Koopman wavefunctions. Although conventional MQC models often suffer…
Nonadiabatic dynamical processes are one of the most important quantum mechanical phenomena in chemical, materials, biological, and environmental molecular systems, where the coupling between different electronic states is either inherent…
A method for carrying out semiclassical initial value representation calculations using first-principles molecular dynamics (FP-SC-IVR) is presented. This method can extract the full vibrational power spectrum of carbon dioxide from a…