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M. Daghofer

Publications and source records attributed to M. Daghofer.

At least 19 recordsLinked to original sources

Proximate ferromagnetic state in the Kitaev model material $\alpha$-RuCl$_{3}$

$\alpha$-RuCl$_{3}$ is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of $\alpha$-RuCl$_{3}$ by a resonant inelastic x-ray scattering study at the Ru $L_{3}$ absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilized by competing ferromagnetic correlations. The classical ground state of the experimentally determined Hamiltonian is actually ferromagnetic. The zigzag state is stabilized via a quantum "order by disorder" mechanism, leaving ferromagnetism -- along with the Kitaev spin liquid -- as energetically proximate metastable states. The three closely competing states and their collective excitations hold the key to the theoretical understanding of the unusual properties of $\alpha$-RuCl$_{3}$ in magnetic fields.

cond-mat.str-el

Block-spiral magnetism: An exotic type of frustrated order

Competing interactions in Quantum Materials induce novel states of matter such as frustrated magnets, an extensive field of research both from the theoretical and experimental perspectives. Here, we show that competing energy scales present in the low-dimensional orbital-selective Mott phase (OSMP) induce an exotic magnetic order, never reported before. Earlier neutron scattering experiments on iron-based 123 ladder materials, where OSMP is relevant, already confirmed our previous theoretical prediction of block-magnetism (magnetic order of the form $\uparrow\uparrow\downarrow\downarrow$). Now we argue that another novel phase can be stabilized in multi-orbital Hubbard models, the {\it block-spiral state}. In this state, the magnetic islands form a spiral propagating through the chain but with the blocks maintaining their identity, namely rigidly rotating. This new spiral state is stabilized without any apparent frustration, the common avenue to generate spiral arrangements in multiferroics. By examining the behaviour of the electronic degrees of freedom, parity breaking quasiparticles are revealed. Finally, a simple phenomenological model that accurately captures the macroscopic spin spiral arrangement is also introduced, and fingerprints for the neutron scattering experimental detection of our new state are provided.

cond-mat.str-el

Novel Magnetic Block States in Low-Dimensional Iron-Based Superconductors

Inelastic neutron scattering recently confirmed the theoretical prediction of a $\uparrow\uparrow\downarrow\downarrow$-magnetic state along the legs of quasi-one-dimensional (quasi-1D) iron-based ladders in the orbital-selective Mott phase (OSMP). We show here that electron-doping of the OSMP induces a whole class of novel block-states with a variety of periodicities beyond the previously reported $\pi/2$ pattern. We discuss the magnetic phase diagram of the OSMP regime that could be tested by neutrons once appropriate quasi-1D quantum materials with the appropriate dopings are identified.

cond-mat.str-el

A Unique Crystal Structure of Ca$_2$RuO$_4$ in the Current Stabilized Semi-Metallic State

The electric-current stabilized semi-metallic state in the quasi-two-dimensional Mott insulator Ca$_2$RuO$_4$ exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and X-ray diffraction, we show that this non-equilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semi-metallic state with partially gapped Fermi surface. Our neutron diffraction data show that the non-equilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual non-equilibrium diamagnetism in Ca$_2$RuO$_4$.

cond-mat.str-el

Excitonic quasiparticles in a spin-orbit Mott insulator

In condensed matter systems, out of a large number of interacting degrees of freedom emerge weakly coupled particles, in terms of which most physical properties are described. For example, Landau quasiparticles (QP) determine all electronic properties of a normal metal. The lack of identification of such QPs is major barrier for understanding myriad exotic properties of correlated electrons, such as unconventional superconductivity and non-Fermi liquid behaviours. Here, we report the observation of a composite particle in a Mott insulator Sr2IrO4---and exciton dressed with magnons---that propagates with the canonical characteristics of a QP: a finite QP residue and a lifetime longer than the hopping time scale. The dynamics of this charge-neutral bosonic excitation mirrors the fundamental process of the analogous one-hole propagation in the background of ordered spins, for which a well-defined QP has never been observed. The much narrower linewidth of the exciton reveals the same intrinsic dynamics that is obscured for the hole and is intimately related to the mechanism of high temperature superconductivity.

cond-mat.str-el

Giant Magnon Gap in Bilayer Iridate Sr3Ir2O7: Enhanced Pseudo-dipolar Interactions Near the Mott Transition

Using resonant inelastic x-ray scattering, we observe in the bilayer iridate Sr3Ir2O7, a spin-orbit coupling driven magnetic insulator with a small charge gap, a magnon gap of ~92 meV for both acoustic and optical branches. This exceptionally large magnon gap exceeds the total magnon bandwidth of ~70 meV and implies a marked departure from the Heisenberg model, in stark contrast to the case of the single-layer iridate Sr2IrO4. Analyzing the origin of these observations, we find that the giant magnon gap results from bond-directional pseudo-dipolar interactions that are strongly enhanced near the metal-insulator transition boundary. This suggests that novel magnetism, such as that inspired by the Kitaev model built on the pseudo-dipolar interactions, may emerge in small charge-gap iridates.

cond-mat.str-el

Dimensionality Driven Spin-Flop Transition in Layered Iridates

Using resonant x-ray diffraction, we observe an easy c-axis collinear antiferromagnetic structure for the bilayer Sr$_3$Ir$_2$O$_7$, a significant contrast to the single layer Sr$_2$IrO$_4$ with in-plane canted moments. Based on a microscopic model Hamiltonian, we show that the observed spin-flop transition as a function of number of IrO$_2$ layers is due to strong competition among intra- and inter-layer bond-directional pseudo-dipolar interactions of the spin-orbit entangled $J_{eff}$=1/2 moments. With this we unravel the origin of anisotropic exchange interactions in a Mott insulator in the strong spin-orbit coupling regime, which holds the key to the various types of unconventional magnetism proposed in 5$d$ transition metal oxides.

cond-mat.str-el

Probing the Unconventional Superconducting State of LiFeAs by Quasiparticle Interference

A crucial step in revealing the nature of unconventional superconductivity is to investigate the symmetry of the superconducting order parameter. Scanning tunneling spectroscopy has proven a powerful technique to probe this symmetry by measuring the quasiparticle interference (QPI) which sensitively depends on the superconducting pairing mechanism. A particularly well suited material to apply this technique is the stoichiometric superconductor LiFeAs as it features clean, charge neutral cleaved surfaces without surface states and a relatively high Tc~18K. Our data reveal that in LiFeAs the quasiparticle scattering is governed by a van-Hove singularity at the center of the Brillouin zone which is in stark contrast with other pnictide superconductors where nesting is crucial for both scattering and s+- superconductivity. Indeed, within a minimal model and using the most elementary order parameters, calculations of the QPI suggest a dominating role of the hole-like bands for the quasiparticle scattering. Our theoretical findings do not support the elementary singlet pairing symmetries s++, s+-, and d-wave. This brings to mind that the superconducting pairing mechanism in LiFeAs is based on an unusual pairing symmetry such as an elementary p-wave (which provides optimal agreement between the experimental data and QPI simulations) or a more complex order parameter (e.g. s+id-wave symmetry).

cond-mat.supr-con

Isospin Dynamics in Sr2IrO4 : Forging Links to Cuprate Superconductivity

We used resonant inelastic x-ray scattering to reveal the nature of magnetic interactions in Sr2IrO4, a 5d transition-metal oxide with a spin-orbit entangled ground state and Jeff=1/2 magnetic momemts, referred to as 'isospins'. The magnon dispersion in Sr2IrO4 is well described by an antiferromagnetic Heisenberg model with isospin one-half moments on a square lattice, which renders the low-energy effective physics of Sr2IrO4 much akin to that in superconducting cuprates. This is further supported by the observation of exciton modes in Sr2IrO4 whose dispersion is strongly renormalized by magnons, which can be understood by analogy to the hole propagation in the background of antiferromagnetically ordered spins in the cuprates.

cond-mat.str-el

Breakdown of the mirror image symmetry in the optical absorption/emission spectra of oligo(para-phenylene)s

The absorption and emission spectra of most luminescent, pi-conjugated, organic molecules are the mirror image of each other. In some cases, however, this symmetry is severely broken. In the present work, the asymmetry between the absorption and fluorescence spectra in molecular systems consisting of para-linked phenyl rings is studied. The vibronic structure of the emission and absorption bands is calculated from ab-initio quantum chemical methods and a subsequent, rigorous Franck-Condon treatment. Good agreement with experiment is achieved. A clear relation can be established between the strongly anharmonic double-well potential for the phenylene ring librations around the long molecular axis and the observed deviation from the mirror image symmetry. Consequences for related compounds and temperature dependent optical measurements are also discussed.

cond-mat.soft

Theory for Magnetism and Triplet Superconductivity in LiFeAs

Superconducting pnictides are widely found to feature spin-singlet pairing in the vicinity of an antiferromagnetic phase, for which nesting between electron and hole Fermi surfaces is crucial. LiFeAs differs from the other pnictides by (i) poor nesting properties and (ii) unusually shallow hole pockets. Investigating magnetic and pairing instabilities in an electronic model that incorporates these differences, we find antiferromagnetic order to be absent. Instead we observe almost ferromagnetic fluctuations which drive an instability toward spin-triplet p-wave superconductivity.

cond-mat.supr-con

Model for the Magnetic Order and Pairing Channels in Fe Pnictide Superconductors

A two-orbital model for Fe-pnictide superconductors is investigated using computational techniques on two-dimensional square clusters. The hopping amplitudes are derived from orbital overlap integrals, or by band structure fits, and the spin frustrating effect of the plaquette-diagonal Fe-Fe hopping is remarked. A spin 'striped' state is stable in a broad range of couplings in the undoped regime, in agreement with neutron scattering. Adding two electrons to the undoped ground state of a small cluster, the dominant pairing operators are found. Depending on parameters, two pairing operators were identified: they involve inter-xz-yz orbital combinations forming spin singlets or triplets, transforming according to the B_2g and A_2g representations of the D_4h group, respectively.

cond-mat.str-el

Phase diagram and single-particle spectrum of CuO$_2$ layers within a variational cluster approach to the 3-band Hubbard model

We carry out a detailed numerical study of the three-band Hubbard model in the underdoped region both in the hole- as well as in the electron-doped case by means of the variational cluster approach. Both the phase diagram and the low-energy single-particle spectrum are very similar to recent results for the single-band Hubbard model with next-nearest-neighbor hoppings. In particular, we obtain a mixed antiferromagnetic+superconducting phase at low doping with a first-order transition to a pure superconducting phase accompanied by phase separation. In the single-particle spectrum a clear Zhang-Rice singlet band with an incoherent and a coherent part can be seen, in which holes enter upon doping around $(π/2,π/2)$. The latter is very similar to the coherent quasi-particle band crossing the Fermi surface in the single-band model. Doped electrons go instead into the upper Hubbard band, first filling the regions of the Brillouin zone around $(π,0)$. This fact can be related to the enhanced robustness of the antiferromagnetic phase as a function of electron doping compared to hole doping.

cond-mat.str-el

Properties of a two orbital model for oxypnictide superconductors: Magnetic order, B_2g spin-singlet pairing channel, and its nodal structure

A two orbital model for the new Fe-based superconductors is studied using the Lanczos method as well as pairing mean-field approximations. Our main goals are (i) to provide a comprehensive analysis of this model using numerical techniques with focus on half-filling and on the state with two more electrons than half-filling and (ii) to investigate the nodal structure of the mean-field superconducting state and compare the results with angle-resolved photoemission data. In particular, we provide evidence that at half-filling spin 'stripes', as observed experimentally, dominate over competing states. Depending on parameters, the state with two more electrons added to half filling is either triplet or singlet. Since experiments suggest spin singlet pairs, our focus is on this state. Under rotation, it transforms as the B_2g representation of the D_4h group. We also show that the s+/- pairing operator transforms as A_1g and becomes dominant only in an unphysical regime of the model where the undoped state is an insulator. For robust values of the effective electronic attraction producing the Cooper pairs, assumption compatible with recent angle-resolved photoemission (ARPES) results that suggesting small Cooper-pair size, the nodes of the two-orbital model are found to be located only at the electron pockets. Since recent ARPES efforts have searched for nodes at the hole pockets or only in a few directions at the electron pockets, our results for the nodal distribution may help to guide future experiments. More in general, the investigations reported here aim to establish several of the properties of the two orbital model. Only a detailed comparison with experiments will clarify how far this simple model present a valid description of the Fe pnictides.

cond-mat.supr-con

Magnetism of one-dimensional Wigner lattices and its impact on charge order

The magnetic phase diagram of the quarter-filled generalized Wigner lattice with nearest- and next-nearest-neighbor hopping t_1 and t_2 is explored. We find a region at negative t_2 with fully saturated ferromagnetic ground states that we attribute to kinetic exchange. Such interaction disfavors antiferromagnetism at t_2 <0 and stems from virtual excitations across the charge gap of the Wigner lattice, which is much smaller than the Mott-Hubbard gap proportional to U. Remarkably, we find a strong dependence of the charge structure factor on magnetism even in the limit U to infinity, in contrast to the expectation that charge ordering in the Wigner lattice regime should be well described by spinless fermions. Our results, obtained using the density-matrix renormalization group and exact diagonalization, can be transparently explained by means of an effective low-energy Hamiltonian.

cond-mat.str-el

Absence of Hole Confinement in Transition Metal Oxides with Orbital Degeneracy

We investigate the spectral properties of a hole moving in a two-dimensional Hubbard model for strongly correlated t_2g electrons. Although superexchange interactions are Ising-like, a quasi-one-dimensional coherent hole motion arises due to effective three-site terms. This mechanism is fundamentally different from the hole motion via quantum fluctuations in the conventional spin model with SU(2) symmetry. The orbital model describes also propagation of a hole in some e_g compounds, and we argue that orbital degeneracy alone does not lead to hole self-localization.

cond-mat.str-el

Fractional charges and spin-charge separation in one-dimensional Wigner lattices

We study density response N(k,omega) and one-particle spectra A(k,omega) for a Wigner lattice model at quarter filling using exact diagonalization. We investigate these observables for models with short and long-range electron-electron interaction and show that truncation of the electron repulsion can lead to very different results. The spectra show clear signatures of charge fractionalization into pairs of domain walls, whose interaction can be attractive or repulsive and is controlled by the formal fractional charges. In striking contrast to a bound exciton in N(k,omega), we find an antibound quasi-particle in A(k,omega), which undergoes spin-charge separation. We present a case of extreme particle-hole asymmetry, where photoemission shows spin-charge separation, while inverse photoemission exhibits an uncorrelated one-particle band.

cond-mat.str-el

Orbital correlations in monolayer manganites - From spin t-J model to orbital t-J model

On the example of monolayer manganites we show that the theoretical ideas developed long ago along the derivation of the spin t-J model from the Hubbard model are nowadays very helpful in strongly correlated oxides with partly filled degenerate orbitals. We analyze a realistic orbital t-J model for e_g electrons in La_{1-x}Sr_{1+x}MnO_4 monolayer manganites, and discuss the evolution of spin and orbital correlations under increasing doping by performing exact diagonalization of finite clusters, with electronic kinetic energy determined self-consistently at finite temperature by classical Monte Carlo for t_2g spins. Several experimental results are reproduced.

cond-mat.str-el