arXiv subjects

Krzysztof Wohlfeld

Publications and source records attributed to Krzysztof Wohlfeld.

At least 37 records · Page 2Linked to original sources

arXiv2022

Limited ferromagnetic interactions in monolayers of MPS$_3$ (M=Mn, Ni)

We present a systematic study of the electronic and magnetic properties of two-dimensional ordered alloys, consisting of two representative hosts (MnPS$_3$ and NiPS$_3$) of transition metal phosphorus trichalcogenides doped with $3d$ elements. For both hosts our DFT+U calculations are able to qualitatively reproduce the ratios and signs of all experimentally observed magnetic couplings. The relative strength of all antiferromagnetic exchange couplings, both in MnPS$_3$ as well as in NiPS$_3$, can successfully be explained using an effective direct exchange model: they reveal that the third-neighbor exchange dominates in NiPS$_3$ due to the filling of the $t_{2g}$ subshell, whereas for MnPS$_3$ the first neighbor exchange is prevailed owing to the presence of the $t_{2g}$ magnetism. On the other hand, the nearest neighbor ferromagnetic coupling in NiPS$_3$ can only be explained using a more complex superexchange model and is (also) largely triggered by the absence of the $t_{2g}$ magnetism. For the doped systems, the DFT+U calculations revealed that magnetic impurities do not affect the magnetic ordering observed in the pure phases and thus in general in these systems ferromagnetism may not be easily induced by such a kind of elemental doping. However, unlike for the hosts, the first and second (dopant-host) exchange couplings are of similar order of magnitude. This leads to frustration in case of antiferromagnetic coupling and may be one of the reasons of the observed lower magnetic ordering temperature of the doped systems.

cond-mat.mtrl-sci↗

arXiv2021

Chalcogenic orbital density waves in weak and strong coupling limit

Stimulated by recent works highlighting the indispensable role of Coulomb interactions in the formation of helical chains and chiral electronic order in the elemental chalcogens, we explore the p-orbital Hubbard model on a one-dimensional helical chain. By solving it in the Hartree approximation we find a stable ground state with a period-three orbital density wave. We establish that the precise form of the emerging order strongly depends on the Hubbard interaction strength. In the strong coupling limit, the Coulomb interactions support an orbital density wave that is qualitatively different from that in the weak-coupling regime. We identify the phase transition separating these two orbital ordered phases, and show that realistic values for the inter-orbital Coulomb repulsion in elemental chalcogens place them in the weak coupling phase, in agreement with observations of the order in the elemental chalcogens.

cond-mat.str-el↗

arXiv2021

Unraveling the orbital physics in a canonical orbital system KCuF$_3$

We explore the existence of the collective orbital excitations, orbitons, in the canonical orbital system KCuF$_3$. Using the Cu $L_3$-edge resonant inelastic X-ray scattering we show that the non-dispersive high-energy peaks result from the Cu$^{2+}$ $dd$ orbital excitations. These high-energy modes show good agreement with the {\it ab-initio} quantum chemistry calculation based on a single cluster, indicating that the $dd$ excitations are highly localized. At the same time, the low-energy excitations present clear dispersion. They match extremely well with the two-spinon continuum following the comparison with Mueller Ansatz calculations. The localized $dd$ excitations and the observation of the strongly dispersive magnetic excitations suggest that orbiton dispersion is below the resolution detection limit. Our results can reconcile with the strong {\it local} Jahn-Teller effect in KCuF$_3$, which predominantly drives orbital ordering.

cond-mat.str-el↗

arXiv2021

Hole in the 2D Ising Antiferromagnet: Origin of the Incoherent Spectrum

We develop a "self-avoiding walks" approximation and use it to calculate the spectral function of a single hole introduced into the 2D square lattice Ising antiferromagnet. The obtained local spectral function qualitatively agrees with the exact diagonalisation result and is largely incoherent. Such a result stays in contrast with the spectrum obtained on a Bethe lattice, which consists of the well-separated quasiparticle-like peaks and stems from the motion of a hole in an effective linear potential. We determine that this onset of the incoherent spectrum on a square lattice (i) is not triggered by the so-called Trugman loops but (ii) originates in the warping of the linear potential by the interactions between magnons created along the tangential paths of the moving hole.

cond-mat.str-el↗

arXiv2020

Emergence of Quasiparticles in a Doped Mott Insulator

How a Mott insulator develops into a weakly coupled metal upon doping is a central question to understanding various emergent correlated phenomena. To analyze this evolution and its connection to the high-$T_c$ cuprates, we study the single-particle spectrum for the doped Hubbard model using cluster perturbation theory on superclusters. Starting from extremely low doping, we identify a heavily renormalized quasiparticle dispersion that immediately develops across the Fermi level, and a weakening polaronic side band at higher binding energy. The quasiparticle spectral weight roughly grows at twice the rate of doping in the low doping regime, but this rate is halved at optimal doping. In the heavily doped regime, we find both strong electron-hole asymmetry and a persistent presence of Mott spectral features. Finally, we discuss the applicability of the single-band Hubbard model to describe the evolution of nodal spectra measured by angle-resolved photoemission spectroscopy (ARPES) on the single-layer cuprate La$_{2-x}$Sr$_x$CuO$_4$ ($0 \le x \le 0.15$). This work benchmarks the predictive power of the Hubbard model for electronic properties of high-$T_c$ cuprates.

cond-mat.str-el↗

arXiv2020

Strain-engineering of the charge and spin-orbital interactions in Sr2IrO4

In the high spin-orbit coupled Sr2IrO4, the high sensitivity of the ground state to the details of the local lattice structure shows a large potential for the manipulation of the functional properties by inducing local lattice distortions. We use epitaxial strain to modify the Ir-O bond geometry in Sr2IrO4 and perform momentum-dependent Resonant Inelastic X-ray Scattering (RIXS) at the metal and at the ligand sites to unveil the response of the low energy elementary excitations. We observe that the pseudospin-wave dispersion for tensile-strained Sr2IrO4 films displays large softening along the [h,0] direction, while along the [h,h] direction it shows hardening. This evolution reveals a renormalization of the magnetic interactions caused by a strain-driven crossover from anisotropic to isotropic interactions between the magnetic moments. Moreover, we detect dispersive electron-hole pair excitations which shift to lower (higher) energies upon compressive (tensile) strain, manifesting a reduction (increase) in the size of the charge gap. This behavior shows an intimate coupling between charge excitations and lattice distortions in Sr2IrO4, originating from the modified hopping elements between the t2g orbitals. Our work highlights the central role played by the lattice degrees of freedom in determining both the pseudospin and charge excitations of Sr2IrO4 and provides valuable information towards the control of the ground state of complex oxides in the presence of high spin-orbit coupling.

cond-mat.str-el↗

arXiv2020

Evolution of Spin-Orbital Entanglement with Increasing Ising Spin-Orbit Coupling

Several realistic spin-orbital models for transition metal oxides go beyond the classical expectations and could be understood only by employing the quantum entanglement. Experiments on these materials confirm that spin-orbital entanglement has measurable consequences. Here, we capture the essential features of spin-orbital entanglement in complex quantum matter utilizing 1D spin-orbital model which accommodates SU(2)xSU(2) symmetric Kugel-Khomskii superexchange as well as the Ising on-site spin-orbit coupling. Building on the results obtained for full and effective models in the regime of strong spin-orbit coupling, we address the question whether the entanglement found on superexchange bonds always increases when the Ising spin-orbit coupling is added. We show that (i) quantum entanglement is amplified by strong spin-orbit coupling and, surprisingly, (ii) almost classical disentangled states are possible. We complete the latter case by analyzing how the entanglement existing for intermediate values of spin-orbit coupling can disappear for higher values of this coupling.

cond-mat.str-el↗

arXiv2020

A $j_\mathrm{eff} = 1/2$ pseudospinon continuum in CaIrO$_3$

In so-called $j_\mathrm{eff} = 1/2$ systems, including some iridates and ruthenates, the coherent superposition of $t_\mathrm{2g}$ orbitals in the ground state gives rise to hopping processes that strongly depend on the bond geometry. Resonant inelastic x-ray scattering (RIXS) measurements on CaIrO$_3$ reveal a prototypical $j_\mathrm{eff} = 1/2$ pseudospinon continuum, a hallmark of one-dimensional (1D) magnetic systems despite its three-dimensional crystal structure. The experimental spectra compare very well to the calculated magnetic dynamical structure factor of weakly coupled spin-1/2 chains. We attribute the onset of such quasi-1D magnetism to the fundamental difference in the magnetic interactions between the $j_\mathrm{eff} = 1/2$ pseudospins along the corner- and edge-sharing bonds in CaIrO$_3$.

cond-mat.str-el↗

arXiv2020

Origin of monoclinic distortion and its impact on the electronic properties in KO$_2$

We use the density functional theory and lattice dynamics calculations to investigate the properties of potassium superoxide KO$_2$ in which spin, orbital, and lattice degrees of freedom are interrelated and determine the low-temperature phase. After calculating phonon dispersion relations in the high-temperature tetragonal $I4/mmm$ structure, we identify a soft phonon mode leading to the monoclinic $C2/c$ symmetry and optimize the crystal geometry resulting from this mode. Thus we reveal a displacive character of the structural transition with the group-subgroup relation between the tetragonal and monoclinic phases. We compare the electronic structure of KO$_2$ with antiferromagnetic spin order in the tetragonal and monoclinic phases. We emphasize that realistic treatment of the electronic structure requires including the local Coulomb interaction $U$ in the valence orbitals of the O$^-_2$ ions. The presence of the `Hubbard' $U$ leads to the gap opening at the Fermi energy in the tetragonal structure without orbital order but with weak spin-orbit interaction. We remark that the gap opening in the tetragonal phase could also be obtained when the orbital order is initiated in the calculations with a realistic value of $U$. Finally, we show that the local Coulomb interactions and the finite lattice distortion, which together lead to the orbital order via the Jahn-Teller effect, are responsible for the enhanced insulating gap in the monoclinic structure.

cond-mat.str-el↗

arXiv2020

Quantum walk versus classical wave: Distinguishing ground states of quantum magnets by spacetime dynamics

We investigate the wavepacket spreading after a single spin flip in prototypical two-dimensional ferromagnetic and antiferromagnetic quantum spin systems. We find characteristic spatial magnon density profiles: While the ferromagnet shows a square-shaped pattern reflecting the underlying lattice structure, as exhibited by quantum walkers, the antiferromagnet shows a circular-shaped pattern which hides the lattice structure and instead resembles a classical wave pattern. We trace these fundamentally different behaviors back to the distinctly different magnon energy-momentum dispersion relations and also provide a real-space interpretation. Our findings point to new opportunities for real-time, real-space imaging of quantum magnets both in materials science and in quantum simulators.

cond-mat.str-el↗

arXiv2020

Mobile orbitons in Ca$_2$CuO$_3$: crucial role of the Hund's exchange

We investigate the Cu $L_3$ edge resonant inelastic x-ray scattering (RIXS) spectra of a quasi-1D antiferromagnet Ca$_2$CuO$_3$. In addition to the magnetic excitations, which are well-described by the two-spinon continuum, we observe two dispersive orbital excitations, the $3d_{xy}$ and the $3d_{yz}$ orbitons. We carry out a quantitative comparison of the RIXS spectra, obtained with two distinct incident polarizations, with a theoretical model. We show that any realistic spin-orbital model needs to include a finite, but realistic, Hund's exchange $J_H \approx 0.5$ eV. Its main effect is an increase in orbiton velocities, so that their theoretically calculated values match those observed experimentally. Even though Hund's exchange also mediates some interaction between spinon and orbiton, the picture of spin-orbit separation remains intact and describes orbiton motion in this compound.

cond-mat.str-el↗

arXiv2020

How spin-orbital entanglement depends on the spin-orbit coupling in a Mott insulator

The concept of the entanglement between spin and orbital degrees of freedom plays a crucial role in understanding various phases and exotic ground states in a broad class of materials, including orbitally ordered materials and spin liquids. We investigate how the spin-orbital entanglement in a Mott insulator depends on the value of the spin-orbit coupling of the relativistic origin. To this end, we numerically diagonalize a 1D spin-orbital model with the 'Kugel-Khomskii' exchange interactions between spins and orbitals on different sites supplemented by the on-site spin-orbit coupling. In the regime of small spin-orbit coupling w.r.t. the spin-orbital exchange, the ground state to a large extent resembles the one obtained in the limit of vanishing spin-orbit coupling. On the other hand, for large spin-orbit coupling the ground state can, depending on the model parameters, either still show negligible spin-orbital entanglement, or can evolve to a highly spin-orbitally entangled phase with completely distinct properties that are described by an effective XXZ model. The presented results suggest that: (i) the spin-orbital entanglement may be induced by large on-site spin-orbit coupling, as found in the 5d transition metal oxides, such as the iridates; (ii) for Mott insulators with weak spin-orbit coupling of Ising-type, such as e.g. the alkali hyperoxides, the effects of the spin-orbit coupling on the ground state can, in the first order of perturbation theory, be neglected.

cond-mat.str-el↗

arXiv2019

Propagation of an orbiton in the antiferromagnets: theory and experimental verification

In this short review, which is based on the works published between 2011 and 2016, we discuss the problem of the propagation of a collective orbital excitation (orbiton) created in the Mott insulating and antiferromagnetic ground state. On the theoretical side, the problem is solved by mapping a Kugel-Khomskii spin-orbital model describing an orbiton moving in an antiferromagnet onto an effective t-J model with a 'single hole' moving in an antiferromagnet. The most important consequence of the existence of the above mapping is the fractionalisation of the electron's spin and orbital degree of freedom in the 1D antiferromagnets---a spin-orbital separation phenomenon that is similar to the spin-charge separation in 1D but corresponds to an exotic regime where spinons are faster than holons. Besides a detailed explanation and benchmarking of the mapping, in this review we also discuss its application to several relatively realistic spin-orbital models, that are able to describe the experimentally observed orbital excitation spectra of copper and iridium oxides.

cond-mat.str-el↗

arXiv2019

From "Weak" to "Strong" Hole Confinement in a Mott Insulator

We study the problem of a single hole in an Ising antiferromagnet and, using the magnon expansion and analytical methods, determine the expansion coefficients of its wave function in the magnon basis. In the 1D case, the hole is "weakly" confined in a potential well and the magnon coefficients decay exponentially in the absence of a string potential. This behavior is in sharp contrast to the 2D square plane where the hole is "strongly" confined by a string potential and the magnon coefficients decay superexponentially. The latter is identified here to be a fingerprint of the strings in doped antiferromagnets that can be recognized in the numerical or cold atom simulations of the 2D doped Hubbard model. Finally, we attribute the differences between the 1D and 2D cases to the magnon-magnon interactions being crucially important in a 1D spin system.

cond-mat.str-el↗

arXiv2019

Photoemission Spectrum of Ca2RuO4: Spin Polaron Physics in an S=1 Antiferromagnet with Anisotropies

We derive an S=1 spin polaron model which describes the motion of a single hole introduced into the S=1 spin antiferromagnetic ground state of Ca2RuO4. We solve the model using the self-consistent Born approximation and show that its hole spectral function qualitatively agrees with the experimentally observed high-binding energy part of the Ca2RuO4 photoemission spectrum. We explain the observed peculiarities of the photoemission spectrum by linking them to two anisotropies present in the employed model---the spin anisotropy and the hopping anisotropy. We verify that these anisotropies, and not the possible differences between the ruthenate (S=1) and the cuprate (S=1/2) spin polaron models, are responsible for the strong qualitative differences between the photoemission spectrum of Ca2RuO4 and of the undoped cuprates.

cond-mat.str-el↗

arXiv2019

Numerical Investigation of Spin Excitations in a Doped Spin Chain

We study the doping evolution of spin excitations in a 1D Hubbard model and its downfolded spin Hamiltonians, by using exact diagonalization combined with cluster perturbation theory. In all models, we observe hardening (softening) of spin excitations upon electron (hole) doping, which are reminiscent of recent experiments on 2D cuprate materials. We also find that the 3-site and even higher-order terms are crucial for the low-energy effective spin models to reproduce the magnetic spectra of doped Hubbard systems at a quantitative level. To interpret the numerical results, we further employ a strong coupling slave-boson mean-field theory. The mean-field theory provides an intuitive understanding of the overall compact support of dynamic spin structure factors, including the shift of zero-energy modes and change of spin excitation bandwidth with doping. Our results can serve as predictive benchmarks for future inelastic x-ray or neutron scattering experiments on doped 1D antiferromagnetic Mott insulators.

cond-mat.str-el↗

arXiv2019

Orbital Symmetry and Orbital Excitations in High-$T_c$ Superconductors

We discuss a few possibilities of high-$T_c$ superconductivity with more than one orbital symmetry contributing to the pairing. First, we show that the high energies of orbital excitations in various cuprates suggest a simplified model with a single orbital of $x^2-y^2$ symmetry doped by holes. Next, several routes towards involving both $e_g$ orbital symmetries for doped holes are discussed: (i) some give superconductivity in a CuO$_2$ monolayer on Bi2212 superconductors, Sr$_2$CuO$_{4-δ}$, Ba$_2$CuO$_{4-δ}$, while (ii) others as nickelate heterostructures or Eu$_{2-x}$Sr$_x$NiO$_4$, could in principle realize it as well. At low electron filling of Ru ions, spin-orbital entangled states of $t_{2g}$ symmetry contribute in Sr$_2$RuO$_4$. Finally, electrons with both $t_{2g}$ and $e_g$ orbital symmetries contribute to the superconducting properties and nematicity of Fe-based superconductors, pnictides or FeSe. Some of them provide examples of orbital-selective Cooper pairing.

cond-mat.supr-con↗

arXiv2018

The silver route to cuprate analogs

The parent compound of high-Tc superconducting cuprates is a unique Mott state consisting of layers of spin-1/2 ions arranged on a square lattice and with a record high antiferromagnetic coupling within the layers. Compounds with similar characteristics have long been searched for. Nickelates and iridates had been proposed as cuprate analogs but so far have not reached a satisfactory similarity. Here we use a combination of experimental and theoretical tools to show that the commercial compound AgF2 is an excellent cuprate analog with remarkably similar electronic parameters to La2CuO4 but larger buckling of planes. Two-magnon Raman scattering reveals a superexchange constant which reaches 70% of that of a typical cuprate. We argue that structures that reduce or eliminate the buckling of the AgF2 planes could have an antiferromagnetic coupling that matches or surpasses the cuprates.

cond-mat.str-el↗