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Stefan Blügel

Publications and source records attributed to Stefan Blügel.

At least 55 records · Page 3Linked to original sources
arXiv2023

Investigation of magnetic properties of $4f$-adatoms on graphene

Rare-earth (RE) atoms on top of 2D materials represent an interesting platform with the prospect of tailoring the magnetic anisotropy for practical applications. Here, we investigate the ground state and magnetic properties of selected $4f$-atoms deposited on a graphene substrate in the framework of the DFT+$U$ approach. The inherent strong spin-orbit interaction in conjunction with crystal field effects acting on the localized $4f$-shells results in a substantial magnetic anisotropy energy (tens of meVs), whose angular dependence is dictated by the $C_{6v}$ symmetry of the graphene substrate. We obtain the crystal field parameters and investigate spin-flip events via quantum tunneling of magnetization in the view of achieving a protected quantum-spin behavior. Remarkably, the large spin and orbital moments of the open $4f$-shells (Dy, Ho and Tm) generate a strong magneto-elastic coupling which provides more flexibility to control the magnetic state via the application of external strain.

cond-mat.mes-hall↗
arXiv2023

Promoting $p$-based Hall effects by $p$-$d$-$f$ hybridization in Gd-based dichalcogenides

We conduct a first-principles study of Hall effects in rare-earth dichalcogenides, focusing on monolayers of the H-phase EuX$_2$ and GdX$_2$, where X = S, Se, and Te. Our predictions reveal that all EuX$_2$ and GdX$_2$ systems exhibit high magnetic moments and wide bandgaps. We observe that while in case of EuX$_2$ the $p$ and $f$ states hybridize directly below the Fermi energy, the absence of $f$ and $d$ states of Gd at the Fermi energy results in $p$-like spin-polarized electronic structure of GdX$_2$, which mediates $p$-based magnetotransport. Notably, these systems display significant anomalous, spin, and orbital Hall conductivities. We find that in GdX$_2$ the strength of correlations controls the relative position of $p$, $d$ and $f$-states and their hybridization which has a crucial impact on $p$-state polarization and the anomalous Hall effect, but not the spin and orbital Hall effect. Moreover, we find that the application of strain can significantly modify the electronic structure of the monolayers, resulting in quantized charge, spin and orbital transport in GdTe$_2$ via a strain-mediated orbital inversion mechanism taking place at the Fermi energy. Our findings suggest that rare-earth dichalcogenides hold promise as a platform for topological spintronics and orbitronics.

cond-mat.mes-hall↗
arXiv2023

Density-functional description of materials for topological qubits and superconducting spintronics

Interfacing superconductors with magnetic or topological materials offers a playground where novel phenomena like topological superconductivity, Majorana zero modes, or superconducting spintronics are emerging. In this work, we discuss recent developments in the Kohn-Sham Bogoliubov-de Gennes method, which allows to perform material-specific simulations of complex superconducting heterostructures on the basis of density functional theory. As a model system we study magnetically-doped Pb. In our analysis we focus on the interplay of magnetism and superconductivity. This combination leads to Yu-Shiba-Rusinov (YSR) in-gap bound states at magnetic defects and the breakdown of superconductivity at larger impurity concentrations. Moreover, the influence of spin-orbit coupling and on orbital splitting of YSR states as well as the appearance of a triplet component in the order parameter is discussed. These effects can be exploited in S/F/S-type devices (S=superconductor, F=ferromagnet) in the field of superconducting spintronics.

cond-mat.supr-con↗
arXiv2023

Inter-orbital Cooper pairing at finite energies in Rashba surface states

Multi-band effects in hybrid structures provide a rich playground for unconventional superconductivity. We combine two complementary approaches based on density-functional theory (DFT) and effective low-energy model theory in order to investigate the proximity effect in a Rashba surface state in contact to an $s$-wave superconductor. We discuss these synergistic approaches and combine the effective model and DFT analysis at the example of a Au/Al heterostructure. This allows us to predict finite-energy superconducting pairing due to the interplay of the Rashba surface state of Au, and hybridization with the electronic structure of superconducting Al. We investigate the nature of the induced superconducting pairing and quantify its mixed singlet-triplet character. Our findings demonstrate general recipes to explore real material systems that exhibit inter-orbital pairing away from the Fermi energy.

cond-mat.supr-con↗
arXiv2023

Flat band-engineered spin-density wave and the emergent multi-$k$ magnetic state in the topological kagome metal Mn$_{3}$Sn

Magnetic kagome metals, in which topologically non-trivial band structures and electronic correlation are intertwined, have recently emerged as an exciting platform to explore exotic correlated topological phases, that are usually not found in weakly interacting materials described within the semi-classical picture of electrons. Here, via a comprehensive single-crystal neutron diffraction and first-principles density functional theory study of the archetypical topological kagome metal Mn$_3$Sn, which is also a magnetic Weyl fermion material and a promising chiral magnet for antiferromagnetic spintronics, we report the realisation of an emergent spin-density wave (SDW) order, a hallmark correlated many-body phenomenon, that is engineered by the Fermi surface nesting of topological flat bands. We further reveal that the phase transition, from the well-known high-temperature coplanar and non-collinear k = 0 inverse triangular antiferromagnetic order to a double-$k$ non-coplanar modulated incommensurate magnetic structure below $T_1$ = 280 K, is primarily driven by the SDW instability. The double-$k$ nature of this complex low-temperature magnetic order, which can be regarded as an intriguing superposition of a longitudinal SDW with a modulation wavevector k$_L$ and a transverse incommensurate helical magnetic order with a modulation wavevector k$_T$, is unambiguously confirmed by our observation of the inter-modulation high-order harmonics of the type of 2k$_L$+k$_T$. This discovery not only solves a long-standing puzzle concerning the nature of the phase transition at $T_1$, but also provides an extraordinary example on the intrinsic engineering of correlated many-body phenomena in topological matter. The identified multi-$k$ magnetic state can be further exploited for the engineering of the new modes of magnetization and chirality switching in antiferromagnetic spintronics.

cond-mat.str-el↗
arXiv2023

How to verify the precision of density-functional-theory implementations via reproducible and universal workflows

In the past decades many density-functional theory methods and codes adopting periodic boundary conditions have been developed and are now extensively used in condensed matter physics and materials science research. Only in 2016, however, their precision (i.e., to which extent properties computed with different codes agree among each other) was systematically assessed on elemental crystals: a first crucial step to evaluate the reliability of such computations. We discuss here general recommendations for verification studies aiming at further testing precision and transferability of density-functional-theory computational approaches and codes. We illustrate such recommendations using a greatly expanded protocol covering the whole periodic table from Z=1 to 96 and characterizing 10 prototypical cubic compounds for each element: 4 unaries and 6 oxides, spanning a wide range of coordination numbers and oxidation states. The primary outcome is a reference dataset of 960 equations of state cross-checked between two all-electron codes, then used to verify and improve nine pseudopotential-based approaches. Such effort is facilitated by deploying AiiDA common workflows that perform automatic input parameter selection, provide identical input/output interfaces across codes, and ensure full reproducibility. Finally, we discuss the extent to which the current results for total energies can be reused for different goals (e.g., obtaining formation energies).

cond-mat.mtrl-sci↗
arXiv2023

Rashba-like spin textures in Graphene promoted by ferromagnet-mediated Electronic-Hybridization with heavy metal

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals (HM) have been proposed for the realization of novel spintronic devices because of their perpendicular magnetic anisotropy and sizeable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes towards this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission along with density functional theory, we show that the interaction of the HM with the C atomic layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of $\sim$\,100 meV (negligible) for in-plane (out-of-plane) spin polarized Gr $π$ bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr $π$ states are electronically decoupled from the HM. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

cond-mat.mtrl-sci↗
arXiv2023

Optical properties of MoSe$_2$ monolayer implanted with ultra-low energy Cr ions

The paper explores the optical properties of an exfoliated MoSe$_2$ monolayer implanted with Cr$^+$ ions, accelerated to 25 eV. Photoluminescence of the implanted MoSe$_2$ reveals an emission line from Cr-related defects that is present only under weak electron doping. Unlike band-to-band transition, the Cr-introduced emission is characterised by non-zero activation energy, long lifetimes, and weak response to the magnetic field. To rationalise the experimental results and get insights into the atomic structure of the defects, we modelled the Cr-ion irradiation process using ab-initio molecular dynamics simulations followed by the electronic structure calculations of the system with defects. The experimental and theoretical results suggest that the recombination of electrons on the acceptors, which could be introduced by the Cr implantation-induced defects, with the valence band holes is the most likely origin of the low energy emission. Our results demonstrate the potential of low-energy ion implantation as a tool to tailor the properties of 2D materials by doping.

cond-mat.mtrl-sci↗
arXiv2023

Heliknoton in a film of cubic chiral magnet

Cubic chiral magnets exhibit a remarkable diversity of two-dimensional topological magnetic textures, including skyrmions. However, the experimental confirmation of topological states localized in all three spatial dimensions remains challenging. In this paper, we investigate a three-dimensional topological state called a heliknoton, which is a hopfion embedded into a helix or conic background. We explore the range of parameters at which the heliknoton can be stabilized under realistic conditions using micromagnetic modeling, harmonic transition state theory, and stochastic spin dynamics simulations. We present theoretical Lorentz TEM images of the heliknoton, which can be used for experimental comparison. Additionally, we discuss the stability of the heliknoton at finite temperatures and the mechanism of its collapse. Our study offers a pathway for future experimental investigations of three-dimensional topological solitons in magnetic crystals.

cond-mat.mes-hall↗
arXiv2023

Ultrafast optical generation of antiferromagnetic meron-antimeron pairs with conservation of topological charge

We propose a new mechanism to produce a meron-antimeron pair in a two dimensional antiferromagnet with an ultrafast laser pulse via thermal Schwinger mechanism. Unlike ultrafast skyrmion nucleation, this process conserves total topological charge. We systematically show different stages of the dynamics and define proper topological invariants to characterise the configurations. The emergent structure can retain its topological structure for up to 100 ps. By introducing a topological structure factor we show that pair formation is robust against any random choice of initial magnetic configuration and can survive against disorder. Our findings demonstrate that the rich world of spin textures, which goes beyond conventional skyrmions, can be reached optically.

cond-mat.mes-hall↗
arXiv2023

Construction of Wannier functions from the spectral moments of correlated electron systems

When the first four spectral moments are considered, spectral features missing in standard Kohn-Sham (KS) density-functional theory (DFT), such as upper and lower Hubbard bands, as well as spectral satellite peaks, can be described, and the bandwidths can be corrected. Therefore, we have devised a \textit{moment-functional based spectral density functional theory} (MFbSDFT) recently. However, many computational tools in theoretical solid state physics, such as the construction of maximally localized Wannier functions (MLWFs), have been developed for KS-DFT and require modifications if they are supposed to be used in MFbSDFT. Here, we show how generalized Wannier functions may be constructed from the first four spectral moment matrices. We call these functions \textit{maximally localized spectral moment Wannier functions} (MLSMWFs). We demonstrate how MLSMWFs may be used to compute the anomalous Hall effect (AHE) in fcc Ni by Wannier interpolation. More generally, MLSMWFs may be computed from the first $2P$ moments ($P=1,2,3,\dots$). Using more than 4 moments opens the perspective of reproducing all spectral features accurately in MFbSDFT.

cond-mat.str-el↗
arXiv2022

Moment potentials for spectral density functional theory: Exploiting the momentum distribution of the uniform electron gas

In standard Kohn-Sham (KS) density-functional theory (DFT) the valence band satellites in Ni and Pd are missing, the band widths in Ni and Na are too large, and the formation of lower and upper Hubbard bands in SrVO$_3$ is not described. These spectral features may be corrected by constructing the spectral function from the first four spectral moments, which may be obtained numerically efficiently within a \textit{moment-functional based spectral density functional theory} (MFbSDFT). In order to obtain a suitable potential for the second moment, one may use existing models of the uniform electron gas (UEG). However, models for the third moment of the UEG are not yet available. Therefore, we show that reproducing the momentum distribution of the UEG within the two-pole approximation of the spectral function determines the third moment, when the second moment is given. This allows us to find a model for the second and third moment potentials, which reproduces the experimental spectra of Ni, Pd, Na, and SrVO$_3$, and which is consistent with the second moment of the UEG at low density. Additionally, we describe an efficient algorithm to compute the spectral function from the first $2P$ spectral moment matrices, which paves the way to increasing the accuracy of MFbSDFT by using more than 4 spectral moments.

cond-mat.mtrl-sci↗
arXiv2022

Emergence of zero-field non-synthetic single and interchanged antiferromagnetic skyrmions in thin films

Antiferromagnetic (AFM) skyrmions are envisioned as ideal localized topological magnetic bits in future information technologies. In contrast to ferromagnetic (FM) skyrmions, they are immune to the skyrmion Hall effect, might offer potential terahertz dynamics while being insensitive to external magnetic fields and dipolar interactions. Although observed in synthetic AFM structures and as complex meronic textures in intrinsic AFM bulk materials, their realization in non-synthetic AFM films, of crucial importance in racetrack concepts, has been elusive. Here, we unveil their presence in a row-wise AFM Cr film deposited on PdFe bilayer grown on fcc Ir(111) surface. Using first principles, we demonstrate the emergence of single and strikingly interpenetrating chains of AFM skyrmions, which can co-exist with the rich inhomogeneous exchange field, including that of FM skyrmions, hosted by PdFe. Besides the identification of an ideal platform of materials for intrinsic AFM skyrmions, we anticipate the uncovered knotted solitons to be promising building blocks in AFM spintronics.

cond-mat.mtrl-sci↗
arXiv2022

Stability of Hopfions in Bulk Magnets with Competing Exchange Interactions

Magnetic hopfions are string-like three-dimensional topological solitons, characterised by the Hopf invariant. They serve as a fundamental prototype for three-dimensional magnetic quasi-particles and are an inspiration for novel device concepts in the field of spintronics. Based on a micromagnetic model and without considering temperature, the existence of such hopfions has been predicted in certain magnets with competing exchange interactions. However, physical realisation of freely moving hopfions in bulk magnets have so far been elusive. Here, we consider an effective Heisenberg model with competing exchange interactions and study the stability of small toroidal hopfions with Hopf number $Q_\text{H}=1$ by finding first-order saddle points on the energy surface representing the transition state for the decay of hopfions via the formation of two coupled Bloch points. We combine the geodesic nudged elastic band method and an adapted implementation of the dimer method to resolve the sharp energy profile of the reaction path near the saddle point. Our analysis reveals that the energy barrier can reach substantial height and is largely determined by the size of the hopfion relative to the lattice constant.

cond-mat.mes-hall↗
arXiv2022

Geometry-induced spin-filtering in photoemission maps from WTe$_2$ surface states

We demonstrate that an important quantum material WTe$_2$ exhibits a new type of geometry-induced spin-filtering effect in photoemission, stemming from low symmetry that is responsible for its exotic transport properties. Through the laser-driven spin-polarized angle-resolved photoemission Fermi surface mapping, we showcase highly asymmetric spin textures of electrons photoemitted from the surface states of WTe$_2$. Such asymmetries are not present in the initial state spin textures, which are bound by the time-reversal and crystal lattice mirror plane symmetries. The findings are reproduced qualitatively by theoretical modeling within the one-step model photoemission formalism. The effect could be understood within the free-electron final state model as an interference due to emission from different atomic sites. The observed effect is a manifestation of time-reversal symmetry breaking of the initial state in the photoemission process, and as such it cannot be eliminated, but only its magnitude influenced, by special experimental geometries.

cond-mat.mtrl-sci↗
arXiv2022

Moment-functional based spectral density-functional theory

We describe a density-functional method which aims at computing the ground state electron density and the spectral function at the same time. One basic ingredient of our method is the construction of the spectral function from the first four spectral moment matrices. The second basic ingredient is the construction of the spectral moment matrices from density functionals. We call our method moment-functional based spectral density-functional theory (MFbSDFT), because it is based on density-functionals for the spectral moments and because it allows us to compute the spectral function. If it is implemented in second variation our method consumes only a fraction more computer time than a standard DFT calculation with the PBE functional. We show that MFbSDFT captures correlation effects such as the valence-band satellite in Ni and the formation of lower and upper Hubbard bands in SrVO$_3$. For the purpose of constructing the spectral function from the first four $N\times N$ spectral moment matrices we describe an efficient algorithm based on the diagonalization of one hermitean $2N\times 2N$ matrix.

cond-mat.mtrl-sci↗
arXiv2022

Hidden interplay of current-induced spin and orbital torques in bulk Fe$_3$GeTe$_2$

Low crystal symmetry of magnetic van der Waals materials naturally promotes spin-orbital complexity unachievable in common magnetic materials used for spin-orbit torque switching. Here, using first-principles methods, we demonstrate that an interplay of spin and orbital degrees of freedom has a profound impact on spin-orbit torques in a prototype van der Waals ferromagnet: Fe$_3$GeTe$_2$ (FGT). While we show that bulk FGT hosts strong "hidden" current-induced torques harvested by each of its layers, we uncover that their origin alternates between the conventional spin flux torque and the so-called orbital torque as the magnetization direction is varied. A drastic difference in the behavior of the two types of torques results in a non-trivial evolution of switching properties with doping. Our findings promote the design of non-equilibrium orbital properties as the guiding mechanism for crafting the properties of spin-orbit torques in layered van der Waals materials.

cond-mat.mtrl-sci↗
arXiv2022

Proximity induced superconductivity in a topological insulator

Interfacing a topological insulator (TI) with an $s$-wave superconductor (SC) is a promising material platform that offers the possibility to realize a topological superconductor through which Majorana-based topologically protected qubits can be engineered. In our computational study of the prototypical SC/TI interface between Nb and Bi$_2$Te$_3$, we identify the benefits and possible bottlenecks of this potential Majorana material platform. Bringing Nb in contact with the TI film induces charge doping from the SC to the TI, which shifts the Fermi level into the TI conduction band. For thick TI films, this results in band bending leading to the population of trivial TI quantum-well states at the interface. In the superconducting state, we uncover that the topological surface state experiences a sizable superconducting gap-opening at the SC/TI interface, which is furthermore robust against fluctuations of the Fermi energy. We also show that the trivial interface state is only marginally proximitized, potentially obstructing the realization of Majorana-based qubits in this material platform.

cond-mat.mes-hall↗