相关论文: State Dependent Ring Polymer Molecular Dynamics fo…

We recently obtained a quantum-Boltzmann-conserving classical dynamics by making a single change to the derivation of the `Classical Wigner' approximation. Here, we show that the further approximation of this `Matsubara dynamics' gives rise…

Accurate simulation of the non-adiabatic dynamics of molecules in excited electronic states is key to understanding molecular photo-physical processes. Here we present a novel method, based on a semiclassical approximation, that is as…

We extend our previous symmetrized path-integral molecular dynamics approach to calculate tunneling splittings of molecules in rotationally excited states. In this new formalism, the system is rigorously projected onto selected rotational…

To fully understand, analyze, and determine the behavior of dynamical systems, it is crucial to identify their intrinsic modal coordinates. In nonlinear dynamical systems, this task is challenging as the modal transformation based on the…

This report is concerned with the efficiency of numerical methods for simulating quantum spin systems, with the aim to implement an improved method for simulation of a time-dependent Hamiltonian that displays chirped pulses at a high…

The charge state dynamics of the nitrogen-vacancy (NV) center in diamond play a key role in a wide range of applications, yet remain imperfectly understood. Using single ps-pulses and pulse pairs, we quantitatively investigate the charge…

We address the calculation of microcanonical reaction rates for processes involving significant nuclear quantum effects using ring-polymer molecular dynamics (RPMD), both with and without electronically non-adiabatic transitions. After…

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…

The algebraic reformulation of molecular Quantum Electrodynamics (mQED) at finite temperatures is applied to Nuclear Magnetic Resonance (NMR) in order to provide a foundation for the reconstruction of much more detailed molecular…

In Part I [J. Chem. Phys. 138, 084108 (2013)] we derived a quantum transition-state theory by taking the t->0+ (short-time) limit of a new form of quantum flux-side time-correlation function containing a ring-polymer dividing surface. This…

We review a dynamical approach to non-equilibrium MD (D-NEMD). We show how, using a proper simulation setup, is possible to treat interesting cases in which the initial condition is a stationary non-equilibrium state produced by a suitable…

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…

We discuss nuclear dynamics at molecule-metal interfaces including non-equilibrium molecular junctions. Starting from the many-body states (pseudoparticle) formulation of the molecule-metal system in the molecular vibronic basis, we…

Ring polymers are prevalent in natural and engineered systems, including circular bacterial DNA, crown ethers for cation chelation, and mechanical nanoswitches. The morphology and dynamics of ring polymers are governed by the chemistry and…

We develop a semi-classical method to simulate the motion of atoms in a dissipative optical lattice. Our method treats the internal states of the atom quantum mechanically, including all nonadiabatic couplings, while position and momentum…

Path-integral-based molecular dynamics (MD) simulations are widely used for the calculation of numerically exact quantum Boltzmann properties and approximate dynamical quantities. A nearly universal feature of MD numerical integration…

We introduce a numerical method to simulate nonlinear open quantum dynamics of a particle in situations where its state undergoes significant expansion in phase space while generating small quantum features at the phase-space Planck scale.…

NMR is emerging as a valuable testbed for the investigation of foundational questions in quantum mechanics. The present paper outlines the preparation of a class of mixed states, called pseudo-pure states, that emulate pure quantum states…

Including quantum mechanical effects on the dynamics of nuclei in the condensed phase is challenging, because the complexity of exact methods grows exponentially with the number of quantum degrees of freedom. Efforts to circumvent these…

Molecular dynamics simulations were conducted to investigate the structural properties of melts of nonconcatenated ring polymers and compared to melts of linear polymers. The longest rings were composed of N=1600 monomers per chain which…