arXiv subjects

Daniel Guterding

Publications and source records attributed to Daniel Guterding.

30 records · Page 2Linked to original sources

arXiv2016

Non-trivial role of interlayer cation states in iron-based superconductors

Unconventional superconductivity in iron pnictides and chalcogenides has been suggested to be controlled by the interplay of low-energy antiferromagnetic spin fluctuations and the particular topology of the Fermi surface in these materials. Based on this premise, one would also expect the large class of isostructural and isoelectronic iron germanide compounds to be good superconductors. As a matter of fact, they, however, superconduct at very low temperatures or not at all. In this work we establish that superconductivity in iron germanides is suppressed by strong ferromagnetic tendencies, which surprisingly do not originate from changes in bond-angles or -distances with respect to iron pnictides and chalcogenides, but are due to changes in the electronic structure in a wide range of energies happening upon substitution of atom species (As by Ge and the corresponding spacer cations). Our results indicate that superconductivity in iron-based materials may not always be fully understood based on $d$ or $dp$ model Hamiltonians only.

cond-mat.supr-con↗

arXiv2016

Reduction of magnetic interlayer coupling in barlowite through isoelectronic substitution

Materials with a perfect kagome lattice structure of magnetic ions are intensively sought for, because they may exhibit exotic ground states like the a quantum spin liquid phase. Barlowite is a natural mineral that features perfect kagome layers of copper ions. However, in barlowite there are also copper ions between the kagome layers, which mediate strong interkagome couplings and lead to an ordered ground state. Using {\it ab initio} density functional theory calculations we investigate whether selective isoelectronic substitution of the interlayer copper ions is feasible. After identifying several promising candidates for substitution we calculate the magnetic exchange couplings based on crystal structures predicted from first-principles calculations. We find that isoelectronic substitution with nonmagnetic ions significantly reduces the interkagome exchange coupling. As a consequence, interlayer-substituted barlowite can be described by a simple two-parameter Heisenberg Hamiltonian, for which a quantum spin liquid ground state has been predicted.

cond-mat.str-el↗

arXiv2016

Near-degeneracy of extended $s + d_{x^2-y^2}$ and $d_{xy}$ order parameters in quasi-two-dimensional organic superconductors

The symmetry of the superconducting order parameter in quasi-two-dimensional BEDT-TTF organic superconductors is a subject of ongoing debate. We report ab initio density functional theory calculations for a number of organic superconductors containing $κ$-type layers. Using projective Wannier functions we derive parameters of a common low-energy Hamiltonian based on individual BEDT-TTF molecular orbitals. In a random phase approximation spin-fluctuation approach we investigate the evolution of the superconducting pairing symmetry within this model and point out a phase-transition between extended $s + d_{x^2-y^2}$ and $d_{xy}$ symmetry. We discuss the origin of the mixed order parameter and the relation between the realistic molecule description and the widely used dimer approximation. Based on our ab initio calculations we position the investigated materials in the obtained molecule model phase diagram and simulate scanning tunneling spectroscopy experiments for selected cases. Our calculations show that many $κ$-type materials lie close to the phase transition line between the two pairing symmetry types found in our calculation, possibly explaining the multitude of contradictory experiments in this field.

cond-mat.supr-con↗

arXiv2016

Ab-initio perspective on structural and electronic properties of iron-based superconductors

The discovery of iron pnictides and iron chalcogenides as a new class of unconventional superconductors in 2008 has generated an enourmous amount of experimental and theoretical work that identifies these materials as correlated metals with multiorbital physics, where magnetism, nematicity and superconductivity are competing phases that appear as a function of pressure and doping. A microscopic understanding of the appearance of these phases is crucial in order to determine the nature of superconductivity in these systems. Here we review our recent theoretical efforts to describe and understand from first principles the properties of iron pnictides and chalcogenides with special focus on (i) pressure dependence, (ii) effects of electronic correlation and (iii) origin of magnetism and superconductivity.

cond-mat.str-el↗

arXiv2016

Evidence for eight node mixed-symmetry superconductivity in a correlated organic metal

We report a combined theoretical and experimental investigation of the superconducting state in the quasi-two-dimensional organic superconductor $κ$-(ET)$_2$Cu[N(CN)$_2$]Br. Applying spin-fluctuation theory to a low-energy material-specific Hamiltonian derived from ab initio density functional theory we calculate the quasiparticle density of states in the superconducting state. We find a distinct three-peak structure that results from a strongly anisotropic mixed-symmetry superconducting gap with eight nodes and twofold rotational symmetry. This theoretical prediction is supported by low-temperature scanning tunneling spectroscopy on in situ cleaved single crystals of $κ$-(ET)$_2$Cu[N(CN)$_2$]Br with the tunneling direction parallel to the layered structure.

cond-mat.supr-con↗

arXiv2016

Prospect of quantum anomalous Hall and quantum spin Hall effect in doped kagome lattice Mott insulators

Electronic states with non-trivial topology host a number of novel phenomena with potential for revolutionizing information technology. The quantum anomalous Hall effect provides spin-polarized dissipation-free transport of electrons, while the quantum spin Hall effect in combination with superconductivity has been proposed as the basis for realizing decoherence-free quantum computing. We introduce a new strategy for realizing these effects, namely by hole and electron doping kagome lattice Mott insulators through, for instance, chemical substitution. As an example, we apply this new approach to the natural mineral herbertsmithite. We prove the feasibility of the proposed modifications by performing ab-initio density functional theory calculations and demonstrate the occurrence of the predicted effects using realistic models. Our results herald a new family of quantum anomalous Hall and quantum spin Hall insulators at affordable energy/temperature scales based on kagome lattices of transition metal ions.

cond-mat.mes-hall↗

arXiv2016

Ab initio determination of spin Hamiltonians with anisotropic exchange interactions: the case of the pyrochlore ferromagnet Lu$_2$V$_2$O$_7$

We present a general framework for deriving effective spin Hamiltonians of correlated magnetic systems based on a combination of relativistic ab initio density functional theory calculations (DFT), exact diagonalization of a generalized Hubbard Hamiltonian on finite clusters and spin projections onto the low-energy subspace. A key motivation is to determine anisotropic bilinear exchange couplings in materials of interest. As an example, we apply this method to the pyrochlore Lu$_2$V$_2$O$_7$ where the vanadium ions form a lattice of corner-sharing spin-1/2 tetrahedra. In this compound, anisotropic Dzyaloshinskii-Moriya interactions (DMI) play an essential role in inducing a magnon Hall effect. We obtain quantitative estimates of the nearest-neighbor Heisenberg exchange, the DMI, and the symmetric part of the anisotropic exchange tensor. Finally, we compare our results with experimental ones on the Lu$_2$V$_2$O$_7$ compound.

cond-mat.str-el↗

arXiv2015

Influence of molecular conformations on the electronic structure of organic charge transfer salts

We report ab-initio calculations for the electronic structure of organic charge transfer salts $κ$-(ET)$_2$Cu[N(CN)$_2$]Br, $κ$-(ET)$_2$Cu[N(CN)$_2$]I, $κ^{\prime \prime}$-(ET)$_2$Cu[N(CN)$_2$]Cl and $κ$-(ET)$_2$Cu$_2$(CN)$_3$. These materials show an ordering of the relative orientation of terminal ethylene groups in the BEDT-TTF molecules at finite temperature and our calculations correctly predict the experimentally observed ground state molecular conformations (eclipsed or staggered). Further, it was recently demonstrated that the ethylene endgroup relative orientations can be used to reversibly tune $κ$-(ET)$_2$Cu[N(CN)$_2$]Br through a metal-insulator transition. Using a tight-binding analysis, we show that the molecular conformations of ethylene endgroups are intimately connected to the electronic structure and significantly influence hopping and Hubbard repulsion parameters. Our results place $κ$-(ET)$_2$Cu[N(CN)$_2$]Br in eclipsed and staggered configurations on opposite sides of the metal-insulator transition.

cond-mat.str-el↗

arXiv2015

Origin of the superconducting state in the collapsed tetragonal phase of KFe2As2

Recently, KFe$_2$As$_2$ was shown to exhibit a structural phase transition from a tetragonal to a collapsed tetragonal phase under applied pressure of about $15~\mathrm{GPa}$. Surprisingly, the collapsed tetragonal phase hosts a superconducting state with $T_c \sim 12~\mathrm{K}$, while the tetragonal phase is a $T_c \leq 3.4~\mathrm{K}$ superconductor. We show that the key difference between the previously known non-superconducting collapsed tetragonal phase in AFe$_2$As$_2$ (A= Ba, Ca, Eu, Sr) and the superconducting collapsed tetragonal phase in KFe$_2$As$_2$ is the qualitatively distinct electronic structure. While the collapsed phase in the former compounds features only electron pockets at the Brillouin zone boundary and no hole pockets are present in the Brillouin zone center, the collapsed phase in KFe$_2$As$_2$ has almost nested electron and hole pockets. Within a random phase approximation spin fluctuation approach we calculate the superconducting order parameter in the collapsed tetragonal phase. We propose that a Lifshitz transition associated with the structural collapse changes the pairing symmetry from $d$-wave (tetragonal) to $s_\pm$ (collapsed tetragonal). Our DFT+DMFT calculations show that effects of correlations on the electronic structure of the collapsed tetragonal phase are minimal. Finally, we argue that our results are compatible with a change of sign of the Hall coefficient with pressure as observed experimentally.

cond-mat.supr-con↗

arXiv2015

Unified picture of the doping dependence of superconducting transition temperatures in alkali metal/ammonia intercalated FeSe

In the recently synthesized Li$_x$(NH$_2$)$_y$(NH$_3$)$_z$Fe$_2$Se$_2$ family of iron chalcogenides a molecular spacer consisting of lithium ions, lithium amide and ammonia separates layers of FeSe. It has been shown that upon variation of the chemical composition of the spacer layer, superconducting transition temperatures can reach $T_c\sim 44 \mathrm{K}$, but the relative importance of the layer separation and effective doping to the $T_c$ enhancement is currently unclear. Using state of the art band structure unfolding techniques, we construct eight-orbital models from ab-initio density functional theory calculations for these materials. Within an RPA spin-fluctuation approach, we show that the electron doping enhances the superconducting pairing, which is of $s_\pm$-symmetry and explain the experimentally observed limit to $T_c$ in the molecular spacer intercalated FeSe class of materials.

cond-mat.supr-con↗

arXiv2014

Correlation effects in the tetragonal and collapsed tetragonal phase of CaFe2As2

We investigate the role of correlations in the tetragonal and collapsed tetragonal phases of CaFe2As2 by performing charge self-consistent DFT+DMFT (density functional theory combined with dynamical mean-field theory) calculations. While the topology of the Fermi surface is basically unaffected by the inclusion of correlation effects, we find important orbital-dependent mass renormalizations which show good agreement with recent angle-resolved photoemission (ARPES) experiments. Moreover, we observe a markedly different behavior of these quantities between the low-pressure tetragonal and the high-pressure collapsed tetragonal phase. We attribute these effects to the increased hybridization between the iron- and arsenic orbitals as one enters the collapsed tetragonal phase.

cond-mat.str-el↗

arXiv2014

Electronic structure and de Haas-van Alphen frequencies in KFe2As2 within LDA+DMFT

Recent density functional theory (DFT) calculations for KFe2As2 have shown to be insufficient to satisfactorily describe angle-resolved photoemission (ARPES) measurements as well as observed de Haas van Alphen (dHvA) frequencies. In the present work, we extend DFT calculations based on the full-potential linear augmented plane-wave method by dynamical mean field theory (DFT+DMFT) to include correlation effects beyond the local density approximation. Our results indicate that KFe2As2 is a moderately correlated metal with a mass renormalization factor of the Fe 3d orbitals between 1.6 and 2.7. Also, the obtained shape and size of the Fermi surface are in good agreement with ARPES measurements and we observe some topological changes with respect to DFT calculations like the opening of an inner hole cylinder at the Z point. As a result, our calculated dHvA frequencies differ greatly from existing DFT results and qualitatively agree with experimental data. On this basis, we argue that correlation effects are important to understand the -presently under debate- nature of superconducting state in KFe2As2.

cond-mat.str-el↗