arXiv subjects

E. K. U. Gross

Publications and source records attributed to E. K. U. Gross.

At least 73 records · Page 4Linked to original sources

arXiv2015

Semiclassical analysis of the electron-nuclear coupling in electronic non-adiabatic processes

In the context of the exact factorization of the electron-nuclear wave function, the coupling between electrons and nuclei beyond the adiabatic regime is encoded (i) in the time-dependent vector and scalar potentials and (ii) in the electron-nuclear coupling operator. The former appear in the Schroedinger-like equation that drives the evolution of the nuclear degrees of freedom, whereas the latter is responsible for inducing non-adiabatic effects in the electronic evolution equation. As we have devoted previous studies to the analysis of the vector and scalar potentials, in this paper we focus on the properties of the electron-nuclear coupling operator, with the aim of describing a numerical procedure to approximate it within a semiclassical treatment of the nuclear dynamics.

physics.chem-ph↗

arXiv2015

Ab initio calculation of a Pb single layer on a Si substrate: two-dimensionality and superconductivity

We report on first principles calculations of superconductivity in a single layer of lead on a silicon substrate including a full treatment of phononic and RPA screened coulomb interactions within the parameter free framework of Density Functional Theory for superconductors. A thorough investigation shows that several approximations that are commonly valid in bulk systems fail in this constrained 2D geometry. The calculated critical temperature turns out to be much higher than the experimental value of 1.86K. We argue that the only plausible explanation for the experimental Tc suppression is the onset of fluctuations of the superconducting order parameter.

cond-mat.supr-con↗

arXiv2015

Ab Initio Theory of Superconductivity in a Magnetic Field I. : Spin Density Functional Theory For Superconductors and Eliashberg Equations

We present a first-principles approach to describe magnetic and superconducting systems and the phenomena of competition between these electronic effects. We develop a density functional theory: SpinSCDFT, by extending the Hohenberg-Kohn theorem and constructing the non-interacting Kohn- Sham system. An exchange-correlation functional for SpinSCDFT is derived from the Sham Schlüter connection between the SpinSCDFT Kohn-Sham and a self-energy in Eliashberg approximation. The reference Eliashberg equations for superconductors in the presence of magnetism are also derived and discussed.

cond-mat.supr-con↗

arXiv2015

Ab-Initio Theory of Superconductivity in a Magnetic Field II. : Numerical solution

We numerically investigate the Spin Density Functional theory for superconductors (SpinSCDFT) and the approximated exchange-correlation functional, derived and presented in the preceding paper I. As a test system we employ a free electron gas featuring an exchange-splitting, a phononic pairing field and a Coulomb repulsion. SpinSCDFT results are compared with Sarma, the Bardeen Cooper and Schrieffer theory and with an Eliashberg type of approach. We find that the spectrum of the superconducting Kohn-Sham SpinSCDFT system is not in agreement with the true quasi particle structure. Therefore, starting from the Dyson equation, we derive a scheme that allows to compute the many body excitations of the superconductor and represents the extension to superconductivity of the G0W0 method in band structure theory. This superconducting G0 W0 method vastly improves the predicted spectra.

cond-mat.supr-con↗

arXiv2015

The exact forces on classical nuclei in non-adiabatic charge transfer

The decomposition of electronic and nuclear motion presented in~[A. Abedi, N. T. Maitra, and E. K. U. Gross, Phys. Rev. Lett. 105, 123002 (2010)] yields a time-dependent potential that drives the nuclear motion and fully accounts for the coupling to the electronic subsystem. Here we show that propagation of an ensemble of independent classical nuclear trajectories on this exact potential yields dynamics that are essentially indistinguishable from the exact quantum dynamics for a model non-adiabatic charge transfer problem. We point out the importance of step and bump features in the exact potential that are critical in obtaining the correct splitting of the quasiclassical nuclear wave packet in space after it passes through an avoided crossing between two Born-Oppenheimer surfaces, and analyze their structure. Lastly, an analysis of the exact potentials in the context of trajectory surface hopping procedure is presented, including preliminary investigations of velocity-adjustment, and the force-induced decoherence effect.

physics.chem-ph↗

arXiv2015

High temperature superconductivity in sulfur and selenium hydrides at high pressure

Due to its low atomic mass hydrogen is the most promising element to search for high-temperature phononic superconductors. However, metallic phases of hydrogen are only expected at extreme pressures (400 GPa or higher). The measurement of a record superconducting critical temperature of 190 K in a hydrogen-sulfur compound at 200 GPa of pressure[1], shows that metallization of hydrogen can be reached at significantly lower pressure by inserting it in the matrix of other elements. In this work we re-investigate the phase diagram and the superconducting properties of the H-S system by means of minima hopping method for structure prediction and Density Functional theory for superconductors. We also show that Se-H has a similar phase diagram as its sulfur counterpart as well as high superconducting critical temperature. We predict SeH3 to exceed 120 K superconductivity at 100 GPa. We show that both SeH3 and SH3, due to the critical temperature and peculiar electronic structure, present rather unusual superconducting properties.

cond-mat.supr-con↗

arXiv2014

An efficient algorithm for time propagation within time-dependent density functional theory

An efficient algorithm for time propagation of the time-dependent Kohn-Sham equations is presented. The algorithm is based on dividing the Hamiltonian into small time steps and assuming that it is constant over these steps. This allows for the time-propagating Kohn-Sham wave function to be expanded in the instantaneous eigenstates of the Hamiltonian. The stability and efficiency of the algorithm are tested not just for non-magnetic but also for fully non-collinear magnetic systems. We show that even for delicate properties, like magnetization density, large time-step sizes can be used indicating the stability and efficiency of the algorithm.

physics.comp-ph↗

arXiv2014

Ab-initio theory of Iron based superconductors

We report the first-principles study of superconducting critical temperature and superconducting properties of Fe-based superconductors taking into account on the same footing phonon, charge and spin-fluctuation mediated Cooper pairing. We show that in FeSe this leads to a modulated s$\pm$ gap symmetry, and that the antiferromagnetic paramagnons are the leading mechanism for superconductivity in FeSe, overcoming the strong repulsive effect of both phonons and charge pairing.

cond-mat.supr-con↗

arXiv2014

Superconducting pairing mediated by spin-fluctuations from first principles

We present the derivation of an ab-initio and parameter free effective electron-electron interaction that goes beyond the screened RPA and accounts for superconducting pairing driven by spin-fluctuations. The construction is based on many body perturbation theory and relies on the approximation of the exchange-correlation part of the electronic self-energy within time dependent density functional theory. This effective interaction is included in an exchange correlation kernel for superconducting density functional theory, in order to achieve a completely parameter free superconducting gap equation. First results from applying the new functional to a simplified two-band electron gas model are consistent with experiments.

cond-mat.supr-con↗

arXiv2014

Enhancing and controlling single-atom high-harmonic generation spectra: a time-dependent density-functional scheme

High harmonic generation (HHG) provides a flexible framework for the development of coherent light sources in the extreme-ultraviolet and soft x-ray regimes. However it suffers from low conversion efficiencies as the control of the HHG spectral and temporal characteristics requires manipulating electron trajectories on attosecond time scale. The phase matching mechanism has been employed to selectively enhance specific quantum paths leading to HHG. A few important fundamental questions remain open, among those how much of the enhancement can be achieved by the single-emitter and what is the role of correlations (or the electronic structure) in the selectivity and control of HHG generation. Here we address those questions by examining computationally the possibility of optimizing the HHG spectrum of isolated Hydrogen and Helium atoms by shaping the slowly varying envelope of a 800 nm, 200-cycles long laser pulse. The spectra are computed with a fully quantum mechanical description, by explicitly computing the time-dependent dipole moment of the systems using a first-principles time-dependent density-functional approach (exact for the case of H). The sought optimization corresponds to the selective enhancement of single harmonics, which we find to be significant. This selectivity is entirely due to the single atom response, and not due to any propagation or phase-matching effect. In fact, this single-emitter enhancement adds to the phase-matching techniques to achieving even larger HHG enhancement factors. Moreover, we see that the electronic correlation plays a role in the determining the degree of optimization that can be obtained.

physics.optics↗

arXiv2014

Almost Exact Exchange At Almost No Cost

A recently developed semiclassical approximation to exchange in one dimension is shown to be almost exact, with essentially no computational cost. The variational stability of this approximation is tested, and its far greater accuracy relative to local density functional calculations demonstrated. Even a fully orbital-free potential-functional calculation (no orbitals of any kind) yields little error relative to exact exchange, for more than one orbital.

physics.chem-ph↗

arXiv2014

Controlling observables in time-dependent quantum transport

The theory of time-dependent quantum transport addresses the question: How do electrons flow through a junction under the influence of an external perturbation as time goes by? In this paper, we invert this question and search for a time-dependent bias such that the system behaves in a desired way. This can, for example, be an observable that is forced to follow a certain pattern or the minimization of an objective function which depends on the observables. Our system of choice consists of quantum dots coupled to normal or superconducting leads. We present results for junctions with normal leads where the current, the density or a molecular vibration is optimized to follow a given target pattern. For junctions with two superconducting leads, where the Josephson effect triggers the current to oscillate, we show how to suppress the Josephson oscillations by suitably tailoring the bias. In a second example involving superconductivity, we consider a Y shaped junction with two quantum dots coupled to one superconducting and two normal leads. This device is used as a Cooper pair splitter to create entangled electrons on the two quantum dots. We maximize the splitting efficiency with the help of an optimized bias.

cond-mat.mes-hall↗

arXiv2014

Laser induced ultrafast demagnetization: an \emph{ab-initio} perspective

Time-dependent density functional theory is implemented in an all electron solid-state code for the case of fully non-collinear spins. We use this to study laser induced demagnetization in Fe, Co and Ni. It is shown that this demagnetization is a two-step process: excitation of a fraction of electrons followed by spin-flip transitions of the remaining localized electrons. These results successfully explain several experimental features such as the time-lag between the start of the pulse and demagnetization and spin-flip excitations dominating the physics. We further show that it is possible to control the moment loss by tunable laser parameters like frequency, duration and intensity.

cond-mat.mtrl-sci↗

arXiv2014

First-principles study of superconducting Rare-earth doped CaFe2As2

We report a systematic and ab-initio electronic structure calculation of Ca0.75 M0.25 Fe2 As2 with M = Ca, Sr, Eu, La, Ce, Pr, Nd, Pm, Sm, Na, K, Rb. The recently reported experimentally observed structural trends in rare earths-doped CaFe2 As2 compounds are successfully predicted and a complete theoretical description of the pressure induced orthorhombic to collapsed tetragonal transition is given. We demonstrate that the transition pressure is reduced by electron doping and rises linearly with the ionic size of the dopants. We discuss the implications of our description for the realization of a superconducting phase.

cond-mat.supr-con↗

arXiv2014

Classical nuclear motion coupled to electronic non-adiabatic transitions

We present a detailed derivation and numerical tests of a new mixed quantum-classical scheme to deal with non-adiabatic processes. The method is presented as the zero-th order approximation to the exact coupled dynamics of electrons and nuclei offered by the factorization of the electron-nuclear wave function [A. Abedi, N. T. Maitra and E. K. U. Gross, Phys. Rev. Lett., 105 (2010)]. Numerical results are presented for a model system for non-adiabatic charge transfer in order to test the performance of the method and to validate the underlying approximations.

physics.chem-ph↗

arXiv2014

How to interpret the spectral density of the Keldysh nonequilibrium Green's function

This paper is devoted to the study and interpretation of the spectral function $\mathbf{A}(ω, T)$ of the Keldysh nonequilibrium Green's function. The spatial diagonal of the spectral function is often interpreted as a time-dependent local density of states. We show that this object can take negative values implying that a simple probability interpretation as a time-dependent density of states is not possible. The same issue also occurs for the Wigner function $P(x,p)$ where it is solved by taking the uncertainty principle into account. We follow the same path and incorporate the time-energy uncertainty relation to define a convoluted spectral function that allows for a probability interpretation. The usefulness of this quantity as a interpretative tool is demonstrated by visualizing the charge dynamics in a quantum dot coupled to superconducting leads.

cond-mat.mes-hall↗

arXiv2014

How to represent crystal structures for machine learning: towards fast prediction of electronic properties

High-throughput density-functional calculations of solids are extremely time consuming. As an alternative, we here propose a machine learning approach for the fast prediction of solid-state properties. To achieve this, LSDA calculations are used as training set. We focus on predicting metallic vs. insulating behavior, and on predicting the value of the density of electronic states at the Fermi energy. We find that conventional representations of the input data, such as the Coulomb matrix, are not suitable for the training of learning machines in the case of periodic solids. We propose a novel crystal structure representation for which learning and competitive prediction accuracies become possible within an unrestricted class of spd systems. Due to magnetic phenomena learning on d systems is found more difficult than in pure sp systems.

cond-mat.mtrl-sci↗

arXiv2014

The virial theorem and exact properties of density functionals for periodic systems

In the framework of density functional theory, scaling and the virial theorem are essential tools for deriving exact properties of density functionals. Preexisting mathematical difficulties in deriving the virial theorem via scaling for periodic systems are resolved via a particular scaling technique. This methodology is employed to derive universal properties of the exchange-correlation energy functional for periodic systems.

cond-mat.other↗