arXiv subjects

T. Uzer

Publications and source records attributed to T. Uzer.

26 records · Page 2Linked to original sources

arXiv2006

Identifying reactive trajectories using a moving transition state

A time-dependent no-recrossing dividing surface is shown to lead to a new criterion for identifying reactive trajectories well before they are evolved to infinite time. Numerical dynamics simulations of a dissipative anharmonic two-dimensional system confirm the efficiency of this approach. The results are compared to the standard fixed transition state dividing surface that is well-known to suffer from recrossings and therefore requires trajectories to be evolved over a long time interval before they can reliably be classified as reactive or non-reactive. The moving dividing surface can be used to identify reactive trajectories in harmonic or moderately anharmonic systems with considerably lower numerical effort or even without any simulation at all.

cond-mat.stat-mech↗

arXiv2005

Stochastic Transition States: Reaction Geometry amidst Noise

Classical transition state theory (TST) is the cornerstone of reaction rate theory. It postulates a partition of phase space into reactant and product regions, which are separated by a dividing surface that reactive trajectories must cross. In order not to overestimate the reaction rate, the dynamics must be free of recrossings of the dividing surface. This no-recrossing rule is difficult (and sometimes impossible) to enforce, however, when a chemical reaction takes place in a fluctuating environment such as a liquid. High-accuracy approximations to the rate are well known when the solvent forces are treated using stochastic representations, though again, exact no-recrossing surfaces have not been available. To generalize the exact limit of TST to reactive systems driven by noise, we introduce a time-dependent dividing surface that is stochastically moving in phase space such that it is crossed once and only once by each transition path.

cond-mat.stat-mech↗

arXiv2005

The Transition State in a Noisy Environment

Transition State Theory overestimates reaction rates in solution because conventional dividing surfaces between reagents and products are crossed many times by the same reactive trajectory. We describe a recipe for constructing a time-dependent dividing surface free of such recrossings in the presence of noise. The no-recrossing limit of Transition State Theory thus becomes generally available for the description of reactions in a fluctuating environment.

cond-mat.stat-mech↗

arXiv2004

Semiclassical ionization dynamics of the hydrogen molecular ion in an electric field of arbitrary orientation

Quasi-static models of barrier suppression have played a major role in our understanding of the ionization of atoms and molecules in strong laser fields. Despite their success, in the case of diatomic molecules these studies have so far been restricted to fields aligned with the molecular axis. In this paper we investigate the locations and heights of the potential barriers in the hydrogen molecular ion in an electric field of arbitrary orientation. We find that the barriers undergo bifurcations as the external field strength and direction are varied. This phenomenon represents an unexpected level of intricacy even on this most elementary level of the dynamics. We describe the dynamics of tunnelling ionization through the barriers semiclassically and use our results to shed new light on the success of a recent theory of molecular tunnelling ionization as well as earlier theories that restrict the electric field to be aligned with the molecular axis.

physics.atom-ph↗

arXiv2002

Time-frequency analysis of chaotic systems

We describe a method for analyzing the phase space structures of Hamiltonian systems. This method is based on a time-frequency decomposition of a trajectory using wavelets. The ridges of the time-frequency landscape of a trajectory, also called instantaneous frequencies, enable us to analyze the phase space structures. In particular, this method detects resonance trappings and transitions and allows a characterization of the notion of weak and strong chaos. We illustrate the method with the trajectories of the standard map and the hydrogen atom in crossed magnetic and elliptically polarized microwave fields.

nlin.CD↗

arXiv2002

Thresholds to Chaos and Ionization for the Hydrogen Atom in Rotating Fields

We analyze the classical phase space of the hydrogen atom in crossed magnetic and circularly polarized microwave fields in the high frequency regime, using the Chirikov resonance overlap criterion and the renormalization map. These methods are used to compute thresholds to large scale chaos and to ionization. The effect of the magnetic field is a strong stabilization of a set of invariant tori which bound the trajectories and prevent stochastic ionization. In order to ionize, larger amplitudes of the microwave field are necessary in the presence of a magnetic field.

nlin.CD↗

arXiv2002

Stochastic ionization through noble tori: Renormalization results

We find that chaos in the stochastic ionization problem develops through the break-up of a sequence of noble tori. In addition to being very accurate, our method of choice, the renormalization map, is ideally suited for analyzing properties at criticality. Our computations of chaos thresholds agree closely with the widely used empirical Chirikov criterion.

nlin.CD↗

arXiv1998

Quantum-classical correspondence in the hydrogen atom in weak external fields

The complex processes leading to the collisional population of ultra-long-lived Rydberg states with very high angular momentum can be explained surprisingly well using classical mechanics. In this article, we explain the reason behind this striking agreement between classical theory and experiment by showing that the classical and quantum dynamics of Rydberg electrons in weak, slowly varying external fields agree beyond the mandates of Ehrenfest's Theorem. In particular, we show that the expectation values of angular momentum and Runge-Lenz vectors in hydrogenic eigenstates obey exactly the same perturbative equations of motion as the time averages of the corresponding classical variables. By time averaging the quantum dynamics over a Kepler period, we extend this special quantum-classical equivalence to Rydberg wave packets relatively well localized in energy. Finally, the perturbative equations hold well also for external fields beyond the Inglis-Teller limit, and in the case of elliptic states, which yield the appropriate quasi-classical initial conditions, the matching with classical mechanics is complete.

physics.atom-ph↗