Related papers: An alternative derivation of ring-polymer molecula…
We introduce mapping-variable ring polymer molecular dynamics (MV-RPMD), a model dynamics for the direct simulation of multi-electron processes. An extension of the RPMD idea, this method is based on an exact, imaginary time path-integral…
Thermal rate constants and several kinetic isotope effects were evaluated for the OH + CH4 hydrogen abstraction reaction using two kinetics approaches, ring polymer molecular dynamics (RPMD), and variational transition state theory with…
A model is proposed for studying the reaction dynamics in complex quantum systems in which the complete mixing of states is hindered by an internal barrier. Such systems are often treated by the transition-state theory, also known in…
We develop a theory of quantum $T = 0$ phase transition (q-SMT) between metal and superconducting ground states in a two-dimensional metal with frozen-in spatial fluctuations $\delta\lambda(r)$ of the Cooper attraction constant. When…
Transition State Theory is a central cornerstone in reaction dynamics. Its key step is the identification of a dividing surface that is crossed only once by all reactive trajectories. This assumption is often badly violated, especially when…
Recently proposed non-adiabatic ring polymer molecular dynamics (NRPMD) approach has shown to provide accurate quantum dynamics by incorporating explicit electronic state descriptions and nuclear quantizations. Here, we present a rigorous…
In this thesis I generalize Ring Polymer Molecular Dynamics (RPMD) rate theory to electronically non-adiabatic systems, followed by application to two one-dimensional curve crossing models and a multidimensional spin-boson model.
Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction…
In principle, we should not need the time-dependent extension of density-functional theory (TDDFT) for excitations, and in particular not for Molecular Dynamics (MD) studies: the theorem by Hohenberg and Kohn teaches us that for any…
A practical method for finding free energy barriers for transitions in high-dimensional classical and quantum systems is presented and used to calculate the dissociative sticking probability of H2 on a metal surface within transition state…
We describe a path-integral molecular dynamics implementation of our recently developed golden-rule quantum transition-state theory (GR-QTST). The method is applied to compute the reaction rate in various models of electron transfer and…
Transition state theory (TST) is generalized for the nonequilibrium system with power-law distributions. The stochastic dynamics that gives rise to the power-law distributions for the reaction coordinate and momentum is modeled by the…
The predictions of the mode-coupling theory of the glass transition (MCT) for the tagged-particle density-correlation functions and the mean-squared displacement curves are compared quantitatively and in detail to results from Newtonian-…
The speed limit of quantum state transfer (QST) in a system of interacting particles is not only important for quantum information processing, but also directly linked to Lieb-Robinson-type bounds that are crucial for understanding various…
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…
We present a simple method for the calculation of reaction rates in the Fermi golden-rule limit, which accurately captures the effects of tunnelling and zero-point energy. The method is based on a modification of the recently proposed…
Ring polymer molecular dynamics (RPMD) has proven to be an accurate approach for calculating thermal rate coefficients of various chemical reactions. For wider application of this methodology, efficient ways to generate the underlying…
The accuracy of rate constants calculated using transition state theory depends crucially on the correct identification of a recrossing--free dividing surface. We show here that it is possible to define such optimal dividing surface in…
A new mean-field type theory is proposed to study order-disorder transitions (ODT) in block copolymers. The theory applies to both the weak segregation (WS) and the strong segregation (SS) regimes. A new energy functional is proposed…
Mode-coupling theory (MCT) is conjectured to be a mean-field description of dynamics of the structural glass transition and the replica theory to be its thermodynamic counterpart. However, the relationship between the two theories remains…