Hybrid quantum-classical modeling of quantum dot devices

The design of electrically driven quantum dot devices for quantum optical applications asks for modeling approaches combining classical device physics with quantum mechanics. We connect the well-established fields of semi-classical semiconductor transport theory and the theory of open quantum systems to meet this requirement. By coupling the van Roosbroeck system with a quantum master equation in Lindblad form, we introduce a new hybrid quantum-classical modeling approach, which provides a comprehensive description of quantum dot devices on multiple scales: It enables the calculation of quantum optical figures of merit and the spatially resolved simulation of the current flow in realistic semiconductor device geometries in a unified way. We construct the interface between both theories in such a way, that the resulting hybrid system obeys the fundamental axioms of (non-)equilibrium thermodynamics. We show that our approach guarantees the conservation of charge, consistency with the thermodynamic equilibrium and the second law of thermodynamics. The feasibility of the approach is demonstrated by numerical simulations of an electrically driven single-photon source based on a single quantum dot in the stationary and transient operation regime

First Class Constrained Systems and Twisting of Courant Algebroids by a Closed 4-form

We show that in analogy to the introduction of Poisson structures twisted by a closed 3-form by Park and Klimcik-Strobl, the study of three dimensional sigma models with Wess-Zumino term leads in a likewise way to twisting of Courant algebroid structures by closed 4-forms H. The presentation is kept pedagogical and accessible to physicists as well as to mathematicians, explaining in detail in particular the interplay of field transformations in a sigma model with the type of geometrical structures induced on a target. In fact, as we also show, even if one does not know the mathematical concept of a Courant algebroid, the study of a rather general class of 3-dimensional sigma models leads one to that notion by itself. Courant algebroids became of relevance for mathematical physics lately from several perspectives - like for example by means of using generalized complex structures in String Theory. One may expect that their twisting by the curvature H of some 3-form Ramond-Ramond gauge field will become of relevance as well.Comment: 25 pages, invited contribution to the Wolfgang Kummer memorial volum

Inverse Quantum Chemistry: Concepts and Strategies for Rational Compound Design

The rational design of molecules and materials is becoming more and more important. With the advent of powerful computer systems and sophisticated algorithms, quantum chemistry plays an important role in rational design. While traditional quantum chemical approaches predict the properties of a predefined molecular structure, the goal of inverse quantum chemistry is to find a structure featuring one or more desired properties. Herein, we review inverse quantum chemical approaches proposed so far and discuss their advantages as well as their weaknesses.Comment: 43 pages, 5 figure

Distribution functions and current-correlations in normal-metal--superconductor hetero-structures

We introduce electron-like and hole-like distribution functions, which determine the currents and the fluctuation spectra of the currents measured at a normal-conductor--superconductor hetero-structure. These distribution functions are expressed with the help of newly defined partial densities of states for hetero-structures. Voltage measurements using a weakly coupled contact on such a structure show the absence of a contact resistance to the superconducting reservoir and illustrate how the interface to the superconductor acts as an Andreev mirror. We also discuss the current-current correlations measured at two normal contacts and argue that the appearance of positive correlations is a purely mesoscopic effect, which vanishes in the limit of a large number of channels and in the average over an ensemble.Comment: 8 pages REVTeX, 1 figur

Applicability of Effective Pair Potentials for Active Brownian Particles

We have performed a case study investigating a recently proposed scheme to obtain an effective pair potential for active Brownian particles [Farage et al., Phys. Rev. E 91, 042310 (2015)]. Applying this scheme to the Lennard-Jones potential, numerical simulations of active Brownian particles are compared to simulations of passive Brownian particles interacting by the effective pair potential. Analyzing the static pair correlations, our results indicate a limited range of activity parameters (speed and orientational correlation time) for which we obtain quantitative, or even qualitative, agreement. Moreover, we find a qualitatively different behavior for the virial pressure even for small propulsion speeds. Combining these findings we conclude that beyond linear response active particles exhibit genuine non-equilibrium properties that cannot be captured by effective pair interaction alone

Gradient-Driven Molecule Construction: An Inverse Approach Applied to the Design of Small-Molecule Fixating Catalysts

Rational design of molecules and materials usually requires extensive screening of molecular structures for the desired property. The inverse approach to deduce a structure for a predefined property would be highly desirable, but is, unfortunately, not well-defined. However, feasible strategies for such an inverse design process may be successfully developed for specific purposes. We discuss options for calculating 'jacket' potentials that fulfill a predefined target requirement - a concept that we recently introduced [T. Weymuth, M. Reiher, MRS Proceediungs, 2013, 1524, DOI:10.1557/opl.2012.1764]. We consider the case of small-molecule activating transition metal catalysts. As a target requirement we choose the vanishing geometry gradients on all atoms of a subsystem consisting of a metal center binding the small molecule to be activated. The jacket potential can be represented within a full quantum model or by a sequence of approximations of which a field of electrostatic point charges is the simplest. In a second step, the jacket potential needs to be replaced by a chemically viable chelate-ligand structure for which the geometry gradients on all of its atoms are also required to vanish. In order to analyze the feasibility of this approach, we dissect a known dinitrogen-fixating catalyst to study possible design strategies that must eventually produce the known catalyst.Comment: 40 pages, 6 tables, 5 figure