arXiv subjects

Carsten A. Ullrich

Publications and source records attributed to Carsten A. Ullrich.

At least 37 records · Page 2Linked to original sources

arXiv2019

Chirality and intrinsic dissipation of spin modes in two-dimensional electron liquids

We review recent theoretical and experimental developments concerning collective spin excitations in two-dimensional electron liquid (2DEL) systems, with particular emphasis on the interplay between many-body and spin-orbit effects, as well as the intrinsic dissipation due to the spin-Coulomb drag. Historically, the experimental realization of 2DELs in silicon inversion layers in the 60s and 70s created unprecedented opportunities to probe subtle quantum effects, culminating in the discovery of the quantum Hall effect. In the following years, high quality 2DELs were obtained in doped quantum wells made in typical semiconductors like GaAs or CdTe. These systems became important test beds for quantum many-body effects due to Coulomb interaction, spin dynamics, spin-orbit coupling, effects of applied magnetic fields, as well as dissipation mechanisms. Here we focus on the recent results involving chiral effects and intrinsic dissipation of collective spin modes: these are not only of fundamental interest but also important towards demonstrating new concepts in spintronics. Moreover, new realizations of 2DELs are emerging beyond traditional semiconductors, for instance in multilayer graphene, oxide interfaces, dichalcogenide monolayers, and many more. The concepts discussed in this review will be relevant also for these emerging systems.

cond-mat.mes-hall↗

arXiv2018

Density-functional theory for systems with noncollinear spin: orbital-dependent exchange-correlation functionals and their application to the Hubbard dimer

A new class of orbital-dependent exchange-correlation (xc) potentials for applications in noncollinear spin-density-functional theory is developed. Starting from the optimized effective potential (OEP) formalism for the exact exchange potential - generalized to the noncollinear case - correlation effects are added via a self-consistent procedure inspired by the Singwi-Tosi-Land-Sjolander (STLS) method. The orbital-dependent xc potentials are applied to the Hubbard dimer in uniform and noncollinear magnetic fields and compared to exact diagonalization and to the Bethe-ansatz local spin-density approximation. The STLS gives the overall best performance for total energies, densities and magnetizations, particularly in the weakly to moderately correlated regime.

cond-mat.mes-hall↗

arXiv2017

Direct extraction of excitation energies from ensemble density-functional theory

A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme avoids either the need to calculate many unoccupied levels as in time-dependent density functional theory (TDDFT) or the need for many self-consistent ensemble calculations. The symmetry-eigenstate Hartree-exchange (SEHX) approximation yields results comparable to standard TDDFT for atoms. With this formalism, SEHX yields approximate double-excitations, which are missed by adiabatic TDDFT.

physics.chem-ph↗

arXiv2017

Assessment of long-range-corrected exchange-correlation kernels for solids: accurate exciton binding energies via an empirically scaled Bootstrap kernel

In time-dependent density-functional theory, a family of exchange-correlation kernels, known as long-range-corrected (LRC) kernels, have shown promise in the calculation of excitonic effects in solids. We perform a systematic assessment of existing static LRC kernels (empirical LRC, Bootstrap, and jellium-with-a-gap model) for a range of semiconductors and insulators, focusing on optical spectra and exciton binding energies. We find that no LRC kernel is capable of simultaneously producing good optical spectra and quantitatively accurate exciton binding energies for both semiconductors and insulators. We propose a simple and universal, empirically scaled Bootstrap kernel which yields accurate exciton binding energies for all materials under consideration, with low computational cost.

cond-mat.mtrl-sci↗

arXiv2016

Spin precession and spin waves in a chiral electron gas: beyond Larmor's theorem

Larmor's theorem holds for magnetic systems that are invariant under spin rotation. In the presence of spin-orbit coupling this invariance is lost and Larmor's theorem is broken: for systems of interacting electrons, this gives rise to a subtle interplay between the spin-orbit coupling acting on individual single-particle states and Coulomb many-body effects. We consider a quasi-two-dimensional, partially spin-polarized electron gas in a semiconductor quantum well in the presence of Rashba and Dresselhaus spin-orbit coupling. Using a linear-response approach based on time-dependent density-functional theory, we calculate the dispersions of spin-flip waves. We obtain analytic results for small wave vectors and up to second order in the Rashba and Dresselhaus coupling strengths $α$ and $β$. Comparison with experimental data from inelastic light scattering allows us to extract $α$ and $β$ as well as the spin-wave stiffness very accurately. We find significant deviations from the local density approximation for spin-dependent electron systems.

cond-mat.mes-hall↗

arXiv2016

Excitons in solids from time-dependent density-functional theory: Assessing the Tamm-Dancoff approximation

Excitonic effects in solids can be calculated using the Bethe-Salpeter equation (BSE) or the Casida equation of time-dependent density-functional theory (TDDFT). In both methods, the Tamm-Dancoff approximation (TDA), which decouples excitations and de-excitations, is widely used to reduce computational cost. Here, we study the effect of the TDA on exciton binding energies of solids obtained from the Casida equation using long-range corrected (LRC) exchange-correlation kernels. We find that the TDA underestimates TDDFT-LRC exciton binding energies of semiconductors slightly, but those of insulators significantly (i.e., by more than 100%), and thus it is essential to solve the full Casida equation to describe strongly bound excitons. These findings are relevant in the ongoing search for accurate and efficient TDDFT approaches for excitons.

cond-mat.mtrl-sci↗

arXiv2016

The particle-hole map: formal derivation and numerical implementation

The particle-hole map (PHM) is a tool to visualize electronic excitations, based on representations in a canonical orbital transition space. Introduced as an alternative to the transition density matrix, the PHM has a simple probabilistic interpretation, indicating the origins and destinations of electrons and holes and, hence, the roles of different functional units of molecules during an excitation. We present a formal derivation of the PHM, starting from the particle-hole transition density matrix and projecting onto a set of single-particle orbitals. We implement the PHM using atom-centered localized basis sets and discuss the example of the molecular charge-transfer complex $\rm C_2H_4 - C_2F_4$.

physics.chem-ph↗

arXiv2015

The particle-hole map: a computational tool to visualize electronic excitations

We introduce the particle-hole map (PHM), a visualization tool to analyze electronic excitations in molecules in the time or frequency domain, to be used in conjunction with time-dependent density-functional theory (TDDFT) or other ab initio methods. The purpose of the PHM is to give detailed insight into electronic excitation processes which is not obtainable from local visualization methods such as transition densities, density differences, or natural transition orbitals. The PHM is defined as a nonlocal function of two spatial variables and provides information about the origins, destinations, and connections of charge fluctuations during an excitation process; it is particularly valuable to analyze charge-transfer excitonic processes. In contrast with the transition density matrix, the PHM has a statistical interpretation involving joint probabilities of individual states and their transitions, it satisfies several sum rules and exact conditions, and it is easier to read and interpret. We discuss and illustrate the properties of the PHM and give several examples and applications to excitations in one-dimensional model systems, in a hydrogen chain, and in a benzothiadiazole based molecule.

physics.chem-ph↗

arXiv2015

A simple screened exact-exchange approach for excitonic properties in solids

We present a screened exact-exchange (SXX) method for the efficient and accurate calculation of the optical properties of solids, where the screening is achieved through the zero-wavevector limit of the inverse dielectric function. The SXX approach can be viewed as a simplification of the Bethe-Salpeter equation (BSE) or, in the context of time-dependent density-functional theory, as a first step towards a new class of hybrid functionals for the optical properties of solids. SXX performs well for bound excitons and continuum spectra in both small-gap semiconductors and large-gap insulators, with a computational cost much lower than that of the BSE.

cond-mat.mtrl-sci↗

arXiv2014

Three- to two-dimensional crossover in time-dependent density-functional theory

Quasi-two-dimensional (2D) systems, such as an electron gas confined in a quantum well, are important model systems for many-body theories. Earlier studies of the crossover from 3D to 2D in ground-state density-functional theory showed that local and semilocal exchange-correlation functionals which are based on the 3D electron gas are appropriate for wide quantum wells, but eventually break down as the 2D limit is approached. We now consider the dynamical case and study the performance of various linear-response exchange kernels in time-dependent density-functional theory. We compare approximate local, semilocal and orbital-dependent exchange kernels, and analyze their performance for inter- and intrasubband plasmons as the quantum wells approach the 2D limit. 3D (semi)local exchange functionals are found to fail for quantum well widths comparable to the 2D Wigner-Seitz radius, which implies in practice that 3D local exchange remains valid in the quasi-2D dynamical regime for typical quantum well parameters, except for very low densities.

cond-mat.mes-hall↗

arXiv2014

Exact and approximate Kohn-Sham potentials in ensemble density-functional theory

We construct exact Kohn-Sham potentials for the ensemble density-functional theory (EDFT) from the ground and excited states of helium. The exchange-correlation (XC) potential is compared with the quasi-local-density approximation and both single determinant and symmetry eigenstate ghost-corrected exact exchange approximations. Symmetry eigenstate Hartree-exchange recovers distinctive features of the exact XC potential and is used to calculate the correlation potential. Unlike the exact case, excitation energies calculated from these approximations depend on ensemble weight, and it is shown that only the symmetry eigenstate method produces an ensemble derivative discontinuity. Differences in asymptotic and near-ground-state behavior of exact and approximate XC potentials are discussed in the context of producing accurate optical gaps.

physics.chem-ph↗

arXiv2014

Excitations and benchmark ensemble density functional theory for two electrons

A new method for extracting ensemble Kohn-Sham potentials from accurate excited state densities is applied to a variety of two electron systems, exploring the behavior of exact ensemble density functional theory. The issue of separating the Hartree energy and the choice of degenerate eigenstates is explored. A new approximation, spin eigenstate Hartree-exchange (SEHX), is derived. Exact conditions that are proven include the signs of the correlation energy components, the virial theorem for both exchange and correlation, and the asymptotic behavior of the potential for small weights of the excited states. Many energy components are given as a function of the weights for two electrons in a one-dimensional flat box, in a box with a large barrier to create charge transfer excitations, in a three-dimensional harmonic well (Hooke's atom), and for the He atom singlet-triplet ensemble, singlet-triplet-singlet ensemble, and triplet bi-ensemble.

physics.chem-ph↗

arXiv2014

A brief compendium of time-dependent density-functional theory

Time-dependent density-functional theory (TDDFT) is a formally exact approach to the time-dependent electronic many-body problem which is widely used for calculating excitation energies. We present a survey of the fundamental framework, practical aspects, and applications of TDDFT. This paper is mainly intended for non-experts (students or researchers in other areas) who would like to learn about the present state of TDDFT without going too deeply into formal details.

cond-mat.mtrl-sci↗

arXiv2013

Coulomb-driven organization and enhancement of spin-orbit fields in collective spin excitations

Spin-orbit (SO) fields in a spin-polarized electron gas are studied by angle-resolved inelastic light scattering on a CdMnTe quantum well. We demonstrate a striking organization and enhancement of SO fields acting on the collective spin excitation (spin-flip wave). While individual electronic SO fields have a broadly distributed momentum dependence, giving rise to D'yakonov-Perel' dephasing, the collective spin dynamics is governed by a single collective SO field which is drastically enhanced due to many-body effects. The enhancement factor is experimentally determined. These results provide a powerful indication that these constructive phenomena are universal to collective spin excitations of conducting systems.

cond-mat.mes-hall↗

arXiv2013

Giant Collective Spin-Orbit Field in a Quantum Well: Fine Structure of Spin Plasmons

We employ inelastic light scattering with magnetic fields to study intersubband spin plasmons in a quantum well. We demonstrate the existence of a giant collective spin-orbit (SO) field that splits the spin-plasmon spectrum into a triplet. The effect is remarkable as each individual electron would be expected to precess in its own momentum-dependent SO field, leading to D'yakonov-Perel' dephasing. Instead, many-body effects lead to a striking organization of the SO fields at the collective level. The macroscopic spin moment is quantized by a uniform collective SO field, five times higher than the individual SO field. We provide a momentum-space cartography of this field.

cond-mat.mes-hall↗

arXiv2013

Direct calculation of exciton binding energies with time-dependent density-functional theory

Excitons are electron-hole pairs appearing below the band gap in insulators and semiconductors. They are vital to photovoltaics, but are hard to obtain with time-dependent density-functional theory (TDDFT), since most standard exchange-correlation (xc) functionals lack the proper long-range behavior. Furthermore, optical spectra of bulk solids calculated with TDDFT often lack the required resolution to distinguish discrete, weakly bound excitons from the continuum. We adapt the Casida equation formalism for molecular excitations to periodic solids, which allows us to obtain exciton binding energies directly. We calculate exciton binding energies for both small- and large-gap semiconductors and insulators, study the recently proposed bootstrap xc kernel [S. Sharma et al., Phys. Rev. Lett. 107, 186401 (2011)], and extend the formalism to triplet excitons.

cond-mat.mtrl-sci↗

arXiv2013

Application of object-oriented programming in a time-dependent density-functional theory calculation of exciton binding energies

This paper discusses the benefits of object-oriented programming to scientific computing, using our recent calculations of exciton binding energies with time-dependent density-functional theory (arXiv: 1302.6972) as a case study. We find that an object-oriented approach greatly facilitates the development, the debugging, and the future extension of the code by promoting code reusing. We show that parallelism is added easily in our code in a object-oriented fashion with ScaLAPACK, Boost::MPI and OpenMP.

physics.comp-ph↗

arXiv2012

A minimal model for excitons within time-dependent density-functional theory

The accurate description of the optical spectra of insulators and semiconductors remains an important challenge for time-dependent density-functional theory (TDDFT). Evidence has been given in the literature that TDDFT can produce bound as well as continuum excitons for specific systems, but there are still many unresolved basic questions concerning the role of dynamical exchange and correlation (xc). In particular, the role of the long spatial range and the frequency dependence of the xc kernel $f_{\rm xc}$ for excitonic binding are still not very well explored. We present a minimal model for excitons in TDDFT, consisting of two bands from a one-dimensional Kronig-Penney model and simple approximate xc kernels, which allows us to address these questions in a transparent manner. Depending on the system, it is found that adiabatic xc kernels can produce a single bound exciton, and sometimes two bound excitons, where the long spatial range of $f_{\rm xc}$ is not a necessary condition. It is shown how the Wannier model, featuring an effective electron-hole interaction, emerges from TDDFT. The collective, many-body nature of excitons is explicitly demonstrated.

cond-mat.mtrl-sci↗