arXiv subjects

Johannes Reiff

Publications and source records attributed to Johannes Reiff.

12 recordsLinked to original sources

arXiv2022

Transition state theory characterizes thin film macrospin dynamics driven by an oscillatory magnetic field: Inertial effects

Understanding the magnetization switching process in ferromagnetic thin films is essential for many technological applications. We investigate the effects of periodic driving via magnetic fields on a macrospin system under explicit consideration of inertial dynamics. This is usually achieved by extending the Landau-Lifshitz-Gilbert equation with a term including the second time derivative of the magnetization. The dynamics of the magnetization switching can then be characterized by its switching rate. We apply methods from transition state theory for driven systems to resolve the rate of magnetization switching in this general case. In doing so, we find that magnetization exhibits resonance-like behavior under certain driving conditions, and it can be affected strongly by the system's relaxation rate.

cond-mat.mtrl-sci↗

arXiv2022

Mean first-passage times for solvated LiCN isomerization at intermediate to high temperatures

The behavior of a particle in a solvent has been framed using stochastic dynamics since the early theory of Kramers. A particle in a chemical reaction reacts slower in a diluted solvent because of the lack of energy transfer via collisions. The flux-over-population reaction rate constant rises with increasing density before falling again for very dense solvents. This Kramers turnover is observed in this paper at intermediate and high temperatures in the backward reaction of the LiNC $\rightleftharpoons$ LiCN isomerization via Langevin dynamics and mean first-passage times (MFPTs). It is in good agreement with the Pollak-Grabert-Hänggi (PGH) reaction rates at lower temperatures. Furthermore, we find a square root behavior of the reaction rate at high temperatures and have made direct comparisons of the methods in the intermediate- and high- temperature regimes; all suggesting increased ranges in accuracy of both the PGH and MFPT approaches.

physics.chem-ph↗

arXiv2021

On the stability of satellites at unstable libration points of sun-planet-moon systems

The five libration points of a sun-planet system are stable or unstable fixed positions at which satellites or asteroids can remain fixed relative to the two orbiting bodies. A moon orbiting around the planet causes a time-dependent perturbation on the system. Here, we address the sense in which invariant structure remains. We employ a transition state theory developed previously for periodically driven systems with a rank-1 saddle in the context of chemical reactions. We find that a satellite can be parked on a so-called time-periodic transition state trajectory -- which is an orbit restricted to the vicinity of the libration point L2 for infinitely long time -- and investigate the stability properties of that orbit.

astro-ph.EP↗

arXiv2021

Transition state dynamics of a driven magnetic free layer

Magnetization switching in ferromagnetic structures is an important process for technical applications such as data storage in spintronics, and therefore the determination of the corresponding switching rates becomes essential. We investigate a free-layer system in an oscillating external magnetic field resulting in an additional torque on the spin. The magnetization dynamics including inertial damping can be described by the phenomenological Gilbert equation. The magnetization switching between the two stable orientations on the sphere then requires the crossing of a potential region characterized by a moving rank-1 saddle. We adopt and apply recent extensions of transition state theory for driven systems to compute both the time-dependent and average switching rates of the activated spin system in the saddle region.

cond-mat.mtrl-sci↗

arXiv2021

Controlling reaction dynamics in chemical model systems through external driving

The rate of a chemical reaction can often be determined by the properties of a rank-1 saddle and the associated transition state separating reactants and products. We have found evidence that such rates can be controlled and even enhanced by external driving in at least one such system. Specifically, we analyze a reactive model in two degrees of freedom that has been used earlier to describe driven chemical reactions. Therein, changes in the external driving can lead to a local maximum of the decay rate constant or even to bifurcations of periodic trajectories on the normally hyperbolic invariant manifold (NHIM) corresponding to the transition state. Inspired by these bifurcations, we show that in this case, the dynamics on the NHIM can be connected to the geometry of reactive trajectories and to reaction probabilities of Maxwell-Boltzmann distributed reactant ensembles.

physics.chem-ph↗

arXiv2021

Dynamics and decay rates of a time-dependent two-saddle system

The framework of transition state theory (TST) provides a powerful way for analyzing the dynamics of physical and chemical reactions. While TST has already been successfully used to obtain reaction rates for systems with a single time-dependent saddle point, multiple driven saddles have proven challenging because of their fractal-like phase space structure. This paper presents the construction of an approximately recrossing-free dividing surface based on the normally hyperbolic invariant manifold in a time-dependent two-saddle model system. Based on this, multiple methods for obtaining instantaneous (time-resolved) decay rates of the underlying activated complex are presented and their results discussed.

physics.chem-ph↗

arXiv2021

Thermal decay rates of an activated complex in a driven model chemical reaction

Recent work has shown that in a non-thermal, multidimensional system, the trajectories in the activated complex possess different instantaneous and time-averaged reactant decay rates. Under dissipative dynamics, it is known that these trajectories, which are bound on the normally hyperbolic invariant manifold (NHIM), converge to a single trajectory over time. By subjecting these dissipative systems to thermal noise, we find fluctuations in the saddle-bound trajectories and their instantaneous decay rates. Averaging over these instantaneous rates results in the decay rate of the activated complex in a thermal system. We find, that the temperature dependence of the activated complex decay in a thermal system can be linked to the distribution of the phase space resolved decay rates on the NHIM in the non-dissipative case. By adjusting the external driving of the reaction, we show that it is possible to influence how the decay rate of the activated complex changes with rising temperature.

physics.chem-ph↗

arXiv2020

Influence of external driving on decays in the geometry of the LiCN isomerization

The framework of transition state theory relies on the determination of a geometric structure identifying reactivity. It replaces the laborious exercise of following many trajectories for a long time to provide chemical reaction rates and pathways. In this paper, recent advances in constructing this geometry even in time-dependent systems are applied to the LiCN $\rightleftharpoons$ LiNC isomerization reaction, driven by an external field. We obtain decay rates of the reactant population close to the transition state by exploiting local properties of the dynamics of trajectories in and close to it. We find that the external driving has a large influence on these decay rates when compared to the non-driven isomerization reaction. This, in turn, provides renewed evidence for the possibility of controlling chemical reactions, like this one, through external time-dependent fields.

physics.chem-ph↗

arXiv2020

Dynamics and bifurcations on the normally hyperbolic invariant manifold of a periodically driven system with rank-1 saddle

In chemical reactions, trajectories typically turn from reactants to products when crossing a dividing surface close to the normally hyperbolic invariant manifold (NHIM) given by the intersection of the stable and unstable manifolds of a rank-1 saddle. Trajectories started exactly on the NHIM in principle never leave this manifold when propagated forward or backward in time. This still holds for driven systems when the NHIM itself becomes time dependent. We investigate the dynamics on the NHIM for a periodically driven model system with two degrees of freedom by numerically stabilizing the motion. Using Poincaré surfaces of section we demonstrate the occurrence of structural changes of the dynamics, \emph{viz.}, bifurcations of periodic transition state (TS) trajectories when changing the amplitude and frequency of the external driving. In particular, periodic TS trajectories with the same period as the external driving but significantly different parameters---such as mean energy---compared to the ordinary TS trajectory can be created in a saddle-node bifurcation.

physics.chem-ph↗

arXiv2020

Phase-space resolved rates in driven multidimensional chemical reactions

Chemical reactions in multidimensional driven systems are typically described by a time-dependent rank-1 saddle associated with one reaction and several orthogonal coordinates (including the solvent bath). To investigate reactions in such systems, we develop a fast and robust method ---viz., local manifold analysis (LMA)--- for computing the instantaneous decay rate of reactants. Specifically, it computes the instantaneous decay rates along saddle-bound trajectories near the activated complex by exploiting local properties of the stable and unstable manifold associated with the normally hyperbolic invariant manifold (NHIM). The LMA method offers substantial reduction of numerical effort and increased reliability in comparison to direct ensemble integration. It provides an instantaneous flux that can be assigned to every point on the NHIM and which is associated with a trajectory ---regardless of whether it is periodic, quasi-periodic, or chaotic--- that is bound on the NHIM. The time average of these fluxes in the driven system corresponds to the average rate through a given local section containing the corresponding point on the NHIM. We find good agreement between the results of the LMA and direct ensemble integration obtained using numerically constructed, recrossing-free dividing surfaces.

physics.chem-ph↗

arXiv2019

Invariant Manifolds and Rate Constants in Driven Chemical Reactions

Reaction rates of chemical reactions under nonequilibrium conditions can be determined through the construction of the normally hyperbolic invariant manifold (NHIM) [and moving dividing surface (DS)] associated with the transition state trajectory. Here, we extend our recent methods by constructing points on the NHIM accurately even for multidimensional cases. We also advance the implementation of machine learning approaches to construct smooth versions of the NHIM from a known high-accuracy set of its points. That is, we expand on our earlier use of neural nets, and introduce the use of Gaussian process regression for the determination of the NHIM. Finally, we compare and contrast all of these methods for a challenging two-dimensional model barrier case so as to illustrate their accuracy and general applicability.

physics.chem-ph↗

arXiv2018

Realization of balanced gain and loss in a time-dependent four-mode Bose-Hubbard model

A quantum system exhibiting $\mathcal{PT}$ symmetry is a Bose-Einstein condensate in a double-well potential with balanced particle gain and loss, which is described in the mean-field limit by a Gross-Pitaevskii equation with a complex potential. A possible experimental realization of such a system by embedding it into a Hermitian time-dependent four-mode optical lattice was proposed by Kreibich et al. [Phys. Rev. A 87, 051601(R) (2013)], where additional potential wells act as reservoirs and particle exchange happens via tunneling. Since particle influx and outflux have to be controlled explicitly, a set of conditions on the potential parameters had to be derived. In contrast to previous work, our focus lies on a full many-body description beyond the mean-field approximation using a Bose-Hubbard model with time-dependent potentials. This gives rise to novel quantum effects, such that the differences between mean-field and many-body dynamics are of special interest. We further present stationary analytical solutions for the embedded wells in the mean-field limit, different approaches for the embedding into a many-body system, and a very efficient method for the evaluation of hopping terms to calculate exact Bose-Hubbard dynamics.

quant-ph↗