arXiv subjects

Jörg Main

Publications and source records attributed to Jörg Main.

At least 37 records · Page 2Linked to original sources

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

Balancing gain and loss in symmetrised multi-well potentials

Balanced gain and loss leads to stationary dynamics in open systems. This occurs naturally in PT-symmetric systems, where the imaginary part of the potential describing gain and loss is perfectly antisymmetric. While this case seems intuitive, stationary dynamics are also possible in asymmetric open systems. Open multi-well quantum systems can possess completely or partly real spectra if their Hamiltonian is symmetrised or semi-symmetrised, respectively. In contrast to similar concepts, symmetrisation allows for the description of physical multi-well potentials with gain and loss. A simple matrix model for the description of two and three-mode systems is used as an example, for which analytical symmetrised solutions are derived. It is explicitly shown how symmetrisation can be used to systematically find two-mode systems with a stable, stationary ground state and why only PT-symmetric two-mode systems can have stationary excited states.

quant-ph↗

arXiv2020

Classical and semiclassical description of Rydberg excitons in cuprous oxide

Experimental and theoretical investigations of excitons in cuprous oxide have revealed a significant fine-structure splitting of the excitonic Rydberg states caused by a strong impact of the valence band structure. We provide a semiclassical interpretation of that splitting by investigating the classical dynamics of the excitonic electron-hole pair beyond the hydrogen-like model. Considering the slow motion of Rydberg excitons in coordinate space compared to the fast dynamics of quasispin and hole spin we use an adiabatic approach and energy surfaces in momentum space for the computation of the exciton dynamics. We observe quasi-periodic motion on near-integrable tori. Semiclassical torus quantization yields the energy regions of the fine-structure splitting of $n$-manifolds in agreement with quantum mechanical computations.

cond-mat.mes-hall↗

arXiv2020

Second Harmonic Generation of cuprous oxide in magnetic fields

Recently Second Harmonic Generation (SHG) for the yellow exciton series in cuprous oxide has been demonstrated [J. Mund et al., Phys. Rev. B 98, 085203 (2018)]. Assuming perfect $O_{\mathrm{h}}$ symmetry, SHG is forbidden along certain high-symmetry axes. Perturbations can break this symmetry and forbidden transitions may become allowed. We investigate theoretically the effect of external magnetic fields on the yellow exciton lines of cuprous oxide. We identify two mechanisms by which an applied magnetic field can induce a second harmonic signal in a forbidden direction. First of all, a magnetic field by itself generally lifts the selection rules. In the Voigt configuration, an additional magneto-Stark electric field appears. This also induces certain SHG processes differing from those induced by the magnetic field alone. Complementary to the manuscript by A. Farenbruch et al. [Phys. Rev. B, submitted], we perform a full numerical diagonalization of the exciton Hamiltonian including the complex valence band structure. Numerical results are compared with experimental data.

cond-mat.mes-hall↗

arXiv2020

Green exciton series in cuprous oxide

We numerically investigate the odd parity states of the green exciton series in cuprous oxide. Taking into account the coupling to the yellow series and especially to the yellow continuum, the green excitons are quasi-bound resonances with a finite lifetime which cannot be described with Hermitian operators. To calculate their positions and linewidths, we use the method of complex-coordinate rotation, leading to a non-Hermitian complex eigenvalue problem. We find that the behavior of the dominant P states is very well approximated by a modified Rydberg formula using a negative quantum defect. The corresponding linewidths induced by the coupling to the yellow continuum decrease with the third power of the principal quantum number.

cond-mat.mtrl-sci↗

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↗

arXiv2020

Neural network approach for the dynamics on the normally hyperbolic invariant manifold of periodically driven systems

Chemical reactions in multidimensional systems are often described by a rank-1 saddle, whose stable and unstable manifolds intersect in the normally hyperbolic invariant manifold (NHIM). Trajectories started on the NHIM in principle never leave this manifold when propagated forward or backward in time. However, the numerical investigation of the dynamics on the NHIM is difficult because of the instability of the motion. We apply a neural network to describe time-dependent NHIMs and use this network to stabilize the motion on the NHIM for a periodically driven model system with two degrees of freedom. The method allows us to analyze the dynamics on the NHIM via Poincaré surfaces of section (PSOS) and to determine the transition state (TS) trajectory as a periodic orbit with the same periodicity as the driving saddle, viz. a fixed point of the PSOS surrounded by near-integrable tori. Based on Transition State Theory and a Floquet analysis of a periodic TS trajectory we compute the rate constant of the reaction with significantly reduced numerical effort compared to the propagation of a large trajectory ensemble.

physics.chem-ph↗

arXiv2019

Balanced gain and loss in spatially extended non-$\mathcal{PT}$-symmetric multi-well potentials

The experimental realization of balanced gain and loss in a quantum system has been a long standing goal in quantum mechanics since the introduction of the concept of $\mathcal{PT}$ symmetry and has only recently been achieved. In this paper we analyze balanced gain and loss in Gaussian multi-well potentials with either only gain or loss in each well. By means of symmetrization via matrix models we can construct asymmetric extended potentials with partially real or complex conjugate spectra. This will be demonstrated explicitly for double-well and triple-well systems. Such systems can be realized with Bose-Einstein condensates in optical trapping potentials in the presence of localized particle gain and loss. The usage of asymmetric potentials in the process is more versatile and is considered beneficial in real experimental implementations.

quant-ph↗

arXiv2019

Rydberg excitons in electric and magnetic fields obtained with the complex-coordinate-rotation method

The complete theoretical description of experimentally observed magnetoexcitons in cuprous oxide has been achieved by F. Schweiner et al [Phys. Rev. B 95, 035202 (2017)], using a complete basis set and taking into account the valence band structure and the cubic symmetry of the solid. Here, we extend these calculations by investigating numerically the autoionising resonances of cuprous oxide in electric fields and in parallel electric and magnetic fields oriented in [001] direction. To this aim we apply the complex-coordinate-rotation method. Complex resonance energies are computed by solving a non-Hermitian generalised eigenvalue problem, and absorption spectra are simulated by using relative oscillator strengths. The method allows us to investigate the influence of different electric and magnetic field strengths on the position, the lifetime, and the shape of resonances.

cond-mat.mtrl-sci↗

arXiv2019

Realization of $\mathcal{PT}$-symmetric and $\mathcal{PT}$-symmetry broken states in static optical lattice potentials

R. Labouvie et al. [Phys. Rev. Lett. 116, 235302 (2016)] have described an experiment with a weakly interacting Bose-Einstein condensate trapped in a one-dimensional optical lattice with localized loss created by a focused electron beam. We show that by setting suitable initial currents between neighboring sites it is possible to create $\mathcal{PT}$-symmetric quasi-stationary and $\mathcal{PT}$-symmetry broken decaying states in an embedded two-mode subsystem. This subsystem exhibits gain provided by the coupling to the reservoir sites and localized loss due to the electron beam, and shows the same dynamics as a non-Hermitian two-mode system with symmetric real and antisymmetric imaginary time-independent potentials, except for a proportionality factor in the chemical potential. We also show that there are three other equivalent scenarios, and that the presence of a localized loss term significantly reduces the size of the condensate required for the realization.

quant-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

Topological edge states in the Su-Schrieffer-Heeger model subject to balanced particle gain and loss

We investigate the Su-Schrieffer-Heeger model in presence of an injection and removal of particles, introduced via a master equation in Lindblad form. It is shown that the dynamics of the density matrix follows the predictions of calculations in which the gain and loss are modeled by complex $\mathcal{PT}$-symmetric potentials. In particular it is found that there is a clear distinction in the dynamics between the topologically different cases known from the stationary eigenstates.

quant-ph↗

arXiv2018

Topological invariants in dissipative extensions of the Su-Schrieffer-Heeger model

We investigate dissipative extensions of the Su-Schrieffer-Heeger model with regard to different approaches of modeling dissipation. In doing so, we use two distinct frameworks to describe the gain and loss of particles, one uses Lindblad operators within the scope of Lindblad master equations, the other uses complex potentials as an effective description of dissipation. The reservoirs are chosen in such a way that the non-Hermitian complex potentials are $\mathcal{PT}$-symmetric. From the effective theory we extract a state which has similar properties as the non-equilibrium steady state following from Lindblad master equations with respect to lattice site occupation. We find considerable similarities in the spectra of the effective Hamiltonian and the corresponding Liouvillean. Further, we generalize the concept of the Zak phase to the dissipative scenario in terms of the Lindblad description and relate it to the topological phases of the underlying Hermitian Hamiltonian.

quant-ph↗

arXiv2018

Magneto-Stark-effect of yellow excitons in cuprous oxide

We investigate and compare experimental and numerical excitonic spectra of the yellow series in cuprous oxide Cu$_2$O in the Voigt configuration and thus partially extend the results from Schweiner et al. [Phys. Rev. B 95, 035202 (2017)], who only considered the Faraday configuration. The main difference between the configurations is given by an additional effective electric field in the Voigt configuration, caused by the motion of the exciton through the magnetic field. This Magneto-Stark effect was already postulated by Gross et al. and Thomas et al. in 1961 [Sov. Phys. Solid State 3, 221 (1961); Phys. Rev. 124, 657 (1961)]. Group theoretical considerations show that the field most of all significantly increases the number of allowed lines by decreasing the symmetry of the system. This conclusion is supported by both the experimental and numerical data.

cond-mat.mtrl-sci↗

arXiv2018

Population transfer at exceptional points in spectra of the hydrogen atom in parallel electric and magnetic fields

We study the population transfer between resonance states for a time-dependent loop around exceptional points in spectra of the hydrogen atom in parallel electric and magnetic fields. Exceptional points are well-suited for population transfer mechanisms, since a closed loop around these in parameter space commutes eigenstates. We address the question how shape and duration of the dynamical parameter loop affects the transferred population, in order to optimize the latter. Since the full quantum dynamics of the expansion coefficients is time-consuming, we furthermore present an approximation method, based on a $2\times 2$ matrix.

quant-ph↗

arXiv2018

Using mixed many-body particle states to generate exact $\mathcal{PT}$-symmetry in a time-dependent four-well system

Bose-Einstein condensates with balanced gain and loss in a double-well potential have been shown to exhibit PT-symmetric states. As proposed by Kreibich et al [Phys. Rev. A 87, 051601(R) (2013)], in the mean-field limit the dynamical behaviour of this system, especially that of the PT-symmetric states, can be simulated by embedding it into a Hermitian four-well system with time-dependent parameters. In this paper we go beyond the mean-field approximation and investigate many-body effects in this system, which are in lowest order described by the single-particle density matrix. The conditions for PT symmetry in the single-particle density matrix cannot be completely fulfilled by using pure initial states. Here we show that it is mathematically possible to achieve exact PT symmetry in the four-well many-body system in the sense of the dynamical behaviour of the single-particle density matrix. In contrast to previous work, for this purpose, we use mixed initial states fulfilling certain constraints and use them to calculate the dynamics.

quant-ph↗