arXiv subjects

Tobias Schäfer

Publications and source records attributed to Tobias Schäfer.

28 records · Page 2Linked to original sources

arXiv2018

Ab initio phase diagram of PbSe crystals calculated with the Random Phase Approximation

Understanding the phase behavior of semiconductor materials is important for applications in solid state physics and nanoscience. Accurate experimental data is often difficult to obtain due to strong kinetic effects. In this work, we calculate the temperature-pressure phase diagram of lead selenide (PbSe) using the random phase approximation (RPA), an accurate wavefunction based many-body technique. We consider three crystalline phases, the low pressure B1 phase (NaCl-type), the intermediate B33 phase (CrB-type), and the high pressure B2 phase (CsCl-type). The electronic contributions to the free energy (at T=0K) are calculated in the Born-Oppenheimer approximation using the RPA, whereas phononic contributions are computed in the quasi-harmonic approximation using DFT and the PBEsol functional. At room temperature, we find transition pressures of 4.6 +/- 0.3 GPa for the B1-B33 transition and 18.7 +/- 0.3 GPa for the B33-B2 transition, in good agreement with experiments. In contrast to the interpretation of recent experiments, we observe a negative Clapeyron slope for both transitions. Gibbs free energy differences between competing structures have small gradients close to coexistence, consistent with pronounced hysteresis observed in experiments. The phase diagram presented in this work can serve as a reference for future studies of PbSe and should prove useful in the development of accurate and efficient force fields.

physics.chem-ph↗

arXiv2018

Disorder control in crystalline GeSb2Te4 and its impact on characteristic length scales

Crystalline GeSb2Te4 (GST) is remarkable material, as it allows to continuously tune the electrical resistance by orders of magnitude without involving a phase transition or stoichiometric changes, just by altering the short-range order. While well-ordered specimen are metallic, increasing amounts of disorder can eventually lead to an insulating state with vanishing conductivity in the 0K limit, but a similar number of charge carriers. These observations make disordered GST one of the most promising candidates for the realization of a true Anderson insulator. While so far the low-temperature properties have mostly been studied in films of small grain size, here a sputter-deposition process is employed that enables preparation of a large variety of these GST states including metallic and truly insulating ones. By growing films of GST on mica substrates, biaxially textured samples with huge grain sizes are obtained. A series of these samples is employed for transport measurements, as their electron mean free path can be altered by a factor of 20. Yet, the mean free path always remains more than an order of magnitude smaller than the lateral grain size. This proves unequivocally that grain boundaries play a negligible role for electron scattering, while intragrain scattering, presumably by disordered vacancies, dominates. Most importantly, these findings underline that the Anderson insulating state as well as the system's evolution towards metallic conductivity are indeed intrinsic properties of the material.

cond-mat.mtrl-sci↗

arXiv2018

Laplace transformed MP2 for three dimensional periodic materials using stochastic orbitals in the plane wave basis and correlated sampling

We present an implementation and analysis of a stochastic high performance algorithm to calculate the correlation energy of three dimensional periodic systems in second-order Møller-Plesset perturbation theory (MP2). In particular we measure the scaling behavior of the sample variance and probe whether this stochastic approach is competitive if accuracies well below 1 meV per valence orbital are required, as it is necessary for calculations of adsorption, binding, or surface energies. The algorithm is based on the Laplace transformed MP2 (LTMP2) formulation in the plane wave basis. The time-dependent Hartree-Fock orbitals, appearing in the LTMP2 formulation, are stochastically rotated in the occupied and unoccupied Hilbert space. This avoids a full summation over all combinations of occupied and unoccupied orbitals, as inspired by the work of D. Neuhauser, E. Rabani, and R. Baer in J. Chem. Theory Comput. 9, 24 (2013). Additionally, correlated sampling is introduced, accelerating the statistical convergence significantly.

physics.chem-ph↗

arXiv2017

Analytic Interatomic Forces in the Random Phase Approximation

We discuss that in the random phase approximation (RPA) the first derivative of the energy with respect to the Green's function is the self-energy in the GW approximation. This relationship allows us to derive compact equations for the RPA interatomic forces. We also show that position dependent overlap operators are elegantly incorporated in the present framework. The RPA force equations have been implemented in the projector augmented wave formalism, and we present illustrative applications, including ab initio molecular dynamics simulations, the calculation of phonon dispersion relations for diamond and graphite, as well as structural relaxations for water on boron nitride. The present derivation establishes a concise framework for forces within perturbative approaches and is also applicable to more involved approximations for the correlation energy.

physics.chem-ph↗

arXiv2017

Quartic scaling MP2 for solids: A highly parallelized algorithm in the plane wave basis

We present a low-complexity algorithm to calculate the correlation energy of periodic systems in second-order Møller-Plesset perturbation theory (MP2). In contrast to previous approximation-free MP2 codes, our implementation possesses a quartic scaling, $\mathcal O (N^4)$, with respect to the system size $N$ and offers an almost ideal parallelization efficiency. The general issue that the correlation energy converges slowly with the number of basis functions is eased by an internal basis set extrapolation. The key concept to reduce the scaling is to eliminate all summations over virtual orbitals which can be elegantly achieved in the Laplace transformed MP2 (LTMP2) formulation using plane wave basis sets and Fast Fourier transforms. Analogously, this approach could allow to calculate second order screened exchange (SOSEX) as well as particle-hole ladder diagrams with a similar low complexity. Hence, the presented method can be considered as a step towards systematically improved correlation energies.

physics.chem-ph↗

arXiv2015

The instanton method and its numerical implementation in fluid mechanics

A precise characterization of structures occurring in turbulent fluid flows at high Reynolds numbers is one of the last open problems of classical physics. In this review we discuss recent developments related to the application of instanton methods to turbulence. Instantons are saddle point configurations of the underlying path integrals. They are equivalent to minimizers of the related Freidlin-Wentzell action and known to be able to characterize rare events in such systems. While there is an impressive body of work concerning their analytical description, this review focuses on the question on how to compute these minimizers numerically. In a short introduction we present the relevant mathematical and physical background before we discuss the stochastic Burgers equation in detail. We present algorithms to compute instantons numerically by an efficient solution of the corresponding Euler-Lagrange equations. A second focus is the discussion of a recently developed numerical filtering technique that allows to extract instantons from direct numerical simulations. In the following we present modifications of the algorithms to make them efficient when applied to two- or three-dimensional fluid dynamical problems. We illustrate these ideas using the two-dimensional Burgers equation and the three-dimensional Navier-Stokes equations.

physics.flu-dyn↗

arXiv2014

Relevance of instantons in Burgers turbulence

Instanton calculations are performed in the context of stationary Burgers turbulence to estimate the tails of the probability density function (PDF) of velocity gradients. These results are then compared to those obtained from massive direct numerical simulations (DNS) of the randomly forced Burgers equation. The instanton predictions are shown to agree with the DNS in a wide range of regimes, including those that are far from the limiting cases previously considered in the literature. These results settle the controversy of the relevance of the instanton approach for the prediction of the velocity gradient PDF tail exponents. They also demonstrate the usefulness of the instanton formalism in Burgers turbulence, and suggest that this approach may be applicable in other contexts, such as 2D and 3D turbulence in compressible and incompressible flows.

physics.flu-dyn↗

arXiv2014

Quickest detection in coupled systems

This work considers the problem of quickest detection of signals in a coupled system of $N$ sensors, which receive continuous sequential observations from the environment. It is assumed that the signals, which are modeled by general Itô processes, are coupled across sensors, but that their onset times may differ from sensor to sensor. Two main cases are considered; in the first one signal strengths are the same across sensors while in the second one they differ by a constant. The objective is the optimal detection of the first time at which any sensor in the system receives a signal. The problem is formulated as a stochastic optimization problem in which an extended minimal Kullback-Leibler divergence criterion is used as a measure of detection delay, with a constraint on the mean time to the first false alarm. The case in which the sensors employ cumulative sum (CUSUM) strategies is considered, and it is proved that the minimum of $N$ CUSUMs is asymptotically optimal as the mean time to the first false alarm increases without bound. In particular, in the case of equal signal strengths across sensors, it is seen that the difference in detection delay of the $N$-CUSUM stopping rule and the unknown optimal stopping scheme tends to a constant related to the number of sensors as the mean time to the first false alarm increases without bound. Alternatively, in the case of unequal signal strengths, it is seen that this difference tends to zero.

math.OC↗

arXiv2013

Arclength parametrized Hamilton's equations for the calculation of instantons

A method is presented to compute minimizers (instantons) of action functionals using arclength parametrization of Hamilton's equations. This method can be interpreted as a local variant of the geometric minimum action method (gMAM) introduced to compute minimizers of the Freidlin-Wentzell action functional that arises in the context of large deviation theory for stochastic differential equations. The method is particularly well-suited to calculate expectations dominated by noise-induced excursions from deterministically stable fixpoints. Its simplicity and computational efficiency are illustrated here using several examples: a finite-dimensional stochastic dynamical system (an Ornstein-Uhlenbeck model) and two models based on stochastic partial differential equations: the $ϕ^4$-model and the stochastically driven Burgers equation.

cond-mat.stat-mech↗

arXiv2012

Instanton filtering for the stochastic Burgers equation

We address the question whether one can identify instantons in direct numerical simulations of the stochastically driven Burgers equation. For this purpose, we first solve the instanton equations using the Chernykh-Stepanov method [Phys. Rev. E 64, 026306 (2001)]. These results are then compared to direct numerical simulations by introducing a filtering technique to extract prescribed rare events from massive data sets of realizations. Using this approach we can extract the entire time history of the instanton evolution which allows us to identify the different phases predicted by the direct method of Chernykh and Stepanov with remarkable agreement.

physics.flu-dyn↗