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J. Chaloupka

Publications and source records attributed to J. Chaloupka.

14 recordsLinked to original sources

Three-dimensional zigzag correlations in the van der Waals Kitaev magnet RuBr$_3$

Ruthenium trihalides Ru$X_3$ ($X$ = Cl, Br, I) provide a tunable platform for Kitaev magnetism in two-dimensional van der Waals materials. Despite their similar crystal structures and zigzag antiferromagnetic order, RuBr$_3$ exhibits a higher N\'eel temperature ($T_N$) than RuCl$_3$, suggesting their distinct proximity to the Kitaev quantum spin liquid phase. Using Ru $L_3$-edge resonant x-ray scattering, we show that, while the long-range zigzag order in RuBr$_3$ disappears at $T_N$, the zigzag correlations that persist well above $T_N$ show a pronounced spectral weight redistribution along the interlayer direction. These results suggest that the enhanced interlayer magnetic interactions driven by the extended Br 4$p$ orbitals stabilize three-dimensional zigzag correlations in RuBr$_3$.

cond-mat.str-el

Circular Dichroism in Resonant Inelastic X-ray Scattering: Probing Altermagnetic Domains in MnTe

X-ray magnetic circular dichroism provides a means to identify ferromagnetic, chiral, and altermagnetic orders via their time-reversal-symmetry ($\mathcal{T}$) breaking. However, differentiating magnetic domains related by crystallographic symmetries remains a technical challenge. Here we reveal a circular dichroism (CD) in the resonant inelastic x-ray scattering (RIXS) spectra from the altermagnetic MnTe. The azimuthal dependence of the RIXS-CD intensity of the magnon excitations indicates a dominant occupation of a single altermagnetic domain. The RIXS-CD in our scattering geometry is ascribed to the mirror-symmetry breaking associated with the $\mathcal{T}$-broken altermagnetic order. Our results establish RIXS-CD as a domain-sensitive probe of elementary excitations in quantum materials.

cond-mat.str-el

Hidden covalent insulator and spin excitations in SrRu$_2$O$_6$

The density functional plus dynamical mean-field theory is used to study the spin excitation spectra of SrRu$_2$O$_6$. A good quantitative agreement with experimental spin excitation spectra is found. Depending on the size of the Hund's coupling $J_H$ the systems chooses either Mott insulator or covalent insulator state when magnetic ordering is not allowed. We find that the nature of the paramagnetic state has negligible influence on the charge and spin excitation spectra. We find that antiferromagnetic correlations hide the covalent insulator state for realistic choices of the interaction parameters.

cond-mat.str-el

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

$α$-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 $α$-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 $α$-RuCl$_{3}$ in magnetic fields.

cond-mat.str-el

Higgs mode and its decay in a two dimensional antiferromagnet

Condensed-matter analogs of the Higgs boson in particle physics allow insights into its behavior in different symmetries and dimensionalities. Evidence for the Higgs mode has been reported in a number of different settings, including ultracold atomic gases, disordered superconductors, and dimerized quantum magnets. However, decay processes of the Higgs mode (which are eminently important in particle physics) have not yet been studied in condensed matter due to the lack of a suitable material system coupled to a direct experimental probe. A quantitative understanding of these processes is particularly important for low-dimensional systems where the Higgs mode decays rapidly and has remained elusive to most experimental probes. Here, we discover and study the Higgs mode in a two-dimensional antiferromagnet using spin-polarized inelastic neutron scattering. Our spin-wave spectra of Ca$_2$RuO$_4$ directly reveal a well-defined, dispersive Higgs mode, which quickly decays into transverse Goldstone modes at the antiferromagnetic ordering wavevector. Through a complete mapping of the transverse modes in the reciprocal space, we uniquely specify the minimal model Hamiltonian and describe the decay process. We thus establish a novel condensed matter platform for research on the dynamics of the Higgs mode.

cond-mat.str-el

Soft spin-amplitude fluctuations in a Mott-insulating ruthenate

Magnetism in transition-metal compounds (TMCs) has traditionally been associated with spin degrees of freedom, because the orbital magnetic moments are typically largely quenched. On the other hand, magnetic order in 4f- and 5d-electron systems arises from spin and orbital moments that are rigidly tied together by the large intra-atomic spin-orbit coupling (SOC). Using inelastic neutron scattering on the archetypal 4d-electron Mott insulator Ca$_2$RuO$_4$, we report a novel form of excitonic magnetism in the intermediate-strength regime of the SOC. The magnetic order is characterized by ``soft'' magnetic moments with large amplitude fluctuations manifested by an intense, low-energy excitonic mode analogous to the Higgs mode in particle physics. This mode heralds a proximate quantum critical point separating the soft magnetic order driven by the superexchange interaction from a quantum-paramagnetic state driven by the SOC. We further show that this quantum critical point can be tuned by lattice distortions, and hence may be accessible in epitaxial thin-film structures. The unconventional spin-orbital-lattice dynamics in Ca$_2$RuO$_4$ identifies the SOC as a novel source of quantum criticality in TMCs.

cond-mat.str-el

Direct Evidence for Dominant Bond-directional Interactions in a Honeycomb Lattice Iridate Na2IrO3

Heisenberg interactions are ubiquitous in magnetic materials and have been prevailing in modeling and designing quantum magnets. Bond-directional interactions offer a novel alternative to Heisenberg exchange and provide the building blocks of the Kitaev model, which has a quantum spin liquid (QSL) as its exact ground state. Honeycomb iridates, A2IrO3 (A=Na,Li), offer potential realizations of the Kitaev model, and their reported magnetic behaviors may be interpreted within the Kitaev framework. However, the extent of their relevance to the Kitaev model remains unclear, as evidence for bond-directional interactions remains indirect or conjectural. Here, we present direct evidence for dominant bond-directional interactions in antiferromagnetic Na2IrO3 and show that they lead to strong magnetic frustration. Diffuse magnetic x-ray scattering reveals broken spin-rotational symmetry even above Neel temperature, with the three spin components exhibiting nano-scale correlations along distinct crystallographic directions. This spin-space and real-space entanglement directly manifests the bond-directional interactions, provides the missing link to Kitaev physics in honeycomb iridates, and establishes a new design strategy toward frustrated magnetism.

cond-mat.mtrl-sci

Intense paramagnon excitations in a large family of high-temperature superconductors

In the search for the mechanism of high-temperature superconductivity, intense research has been focused on the evolution of the spin excitation spectrum upon doping from the antiferromagnetic insulating to the superconducting states of the cuprates. Because of technical limitations, the experimental investigation of doped cuprates has been largely focused on low-energy excitations in a small range of momentum space. Here we use resonant inelastic x-ray scattering to show that a large family of superconductors, encompassing underdoped YBa$_2$Cu$_4$O$_8$ and overdoped YBa$_2$Cu$_3$O$_{7}$, exhibits damped spin excitations (paramagnons) with dispersions and spectral weights closely similar to those of magnons in undoped cuprates. %The results are in excellent agreement with the spin excitations obtained by exact diagonalization of the $\bf t-J$ Hamiltonian on finite-sized clusters. The comprehensive experimental description of this surprisingly simple spectrum permits quantitative tests of magnetic Cooper pairing models. A numerical solution of the Eliashberg equations for the magnetic spectrum of YBa$_2$Cu$_3$O$_{7}$ reproduces its superconducting transition temperature within a factor of two, a level of agreement comparable to Eliashberg theories of conventional superconductors.

cond-mat.supr-con

Microscopic gauge-invariant theory of the c-axis infrared response of bilayer cuprate superconductors and the origin of the superconductivity induced absorption bands

We report on results of our theoretical study of the c-axis infrared conductivity of bilayer high-Tc cuprate superconductors using a microscopic model involving the bilayer-split (bonding and antibonding) bands. An emphasis is on the gauge-invariance of the theory, which turns out to be essential for the physical understanding of the electrodynamics of these compounds. The description of the optical response involves local (intra-bilayer and inter-bilayer) current densities and local conductivities. The local conductivities are obtained using a microscopic theory, where the quasiparticles of the two bands are coupled to spin fluctuations. The coupling leads to superconductivity and is described at the level of generalized Eliashberg theory. Also addressed is the simpler case of quasiparticles coupled by a separable and nonretarded interaction. The gauge invariance of the theory is achieved by including a suitable class of vertex corrections. The resulting response of the model is studied in detail and an interpretation of two superconductivity-induced peaks in the experimental data of the real part of the c-axis conductivity is proposed. The peak around 400/cm is attributed to a collective mode of the intra-bilayer regions, that is an analogue of the Bogolyubov-Anderson mode playing a crucial role in the theory of the longitudinal response of superconductors. For small values of the bilayer splitting, its nature is similar to that of the transverse plasmon of the phenomenological Josephson superlattice model. The peak around 1000/cm is interpreted as a pair breaking-feature that is related to the electronic coupling through the spacing layers separating the bilayers.

cond-mat.supr-con

Unusual electron correlations in NaxCoO2 due to the spin-state quasidegeneracy of cobalt ions

Recent studies exposed many remarkable properties of layered cobaltates NaxCoO2. Surprisingly, many-body effects have been found to increase at sodium-rich compositions of NaxCoO2 where one expects a simple, nearly free motion of the dilute S=1/2 holes doped into a band insulator NaCoO2. Here we discuss the origin of enigmatic correlations that turn a doped NaCoO2 into a strongly correlated electronic system. A minimal model including orbital degeneracy is proposed and its predictions are discussed. The model is based on a key property of cobalt oxides - the spin-state quasidegeneracy of CoO6 octahedral complex - which has been known, e.g., in the context of an unusual physics of LaCoO3 compound. Another important ingredient of the model is the 90-degree Co-O-Co bonding in NaxCoO2 which allows nearest-neighbor $t_{2g}-e_g$ hopping. This hopping introduces a dynamical mixture of electronic configurations $t_{2g}^6, S=0$ and $t_{2g}^5e_g^1, S=1$ of neighboring cobalt ions. We show that scattering of charge carriers on spin-state fluctuations suppresses their coherent motion and leads to the spin-polaron physics at $x\sim 1$. At larger doping when coherent fermionic bands are formed, the model predicts singlet superconductivity of extended s-wave symmetry. The presence of low-lying spin states of Co$^{3+}$ is essential for the pairing mechanism. Implications of the model for magnetic orderings are also discussed.

cond-mat.str-el

The origin of strong correlations and superconductivity in Na$_x$CoO$_2$

We propose a minimal model resolving a puzzle of enigmatic correlations observed in sodium-rich Na$_x$CoO$_2$ where one expects a simple, free motion of the dilute $S=1/2$ holes doped into a band insulator NaCoO$_2$. The model also predicts singlet superconductivity at experimentally observed compositions. The model is based on a key property of cobalt oxides -- the spin-state quasidegeneracy of CoO$_6$ octahedral complex -- leading to an unusual physics of, {\it e.g.}, LaCoO$_3$. We show that correlated hopping between $t_{2g}$ and $e_g$ states leads to the spin-polaron physics at $x\sim 1$, and to an extended s-wave pairing at larger doping when coherent fermionic bands are formed.

cond-mat.str-el

Selfconsistent gauge-invariant theory of in-plane infrared response of high-Tc cuprate superconductors involving spin fluctuations

We report on results of our theoretical study of the in-plane infrared conductivity of the high-Tc cuprate superconductors using the model where charged planar quasiparticles are coupled to spin fluctuations. The computations include both the renormalization of the quasiparticles and the corresponding modification of the current-current vertex function (vertex correction), which ensures gauge invariance of the theory and local charge conservation in the system. The incorporation of the vertex corrections leads to an increase of the total intraband optical spectral weight (SW) at finite frequencies, a SW transfer from far infrared to mid infrared, a significant reduction of the SW of the superconducting condensate, and an amplification of characteristic features in the superconducting state spectra of the inverse scattering rate 1/tau. We also discuss the role of selfconsistency and propose a new interpretation of a kink occurring in the experimental low temperature spectra of 1/tau around 1000cm^{-1}.

cond-mat.supr-con

Spin polaron theory for the photoemission spectra of layered cobaltates

Recently, strong reduction of the quasiparticle peaks and pronounced incoherent structures have been observed in the photoemission spectra of layered cobaltates. Surprisingly, these many-body effects are found to increase near the band insulator regime. We explain these unexpected observations in terms of a novel spin-polaron model for CoO_2 planes which is based on a fact of the spin-state quasidegeneracy of Co^{3+} ions in oxides. Scattering of the photoholes on spin-state fluctuations suppresses their coherent motion. The observed ``peak-dip-hump'' type lineshapes are well reproduced by the theory.

cond-mat.str-el

Spectroscopic distinction between the normal state pseudogap and the superconducting gap of cuprate high T_{c} superconductors

We report on broad-band infrared ellipsometry measurements of the c-axis conductivity of underdoped RBa_{2}Cu_{3}O_{7-d} (R=Y, Nd, and La) single crystals. Our data provide a detailed account of the spectral weight (SW) redistributions due to the normal state pseudogap (PG) and the superconducting (SC) gap. They show that these phenomena involve different energy scales, exhibit distinct doping dependencies and thus are likely of different origin. In particular, the SW redistribution in the PG state closely resembles the one of a conventional charge- or spin density wave (CDW or SDW) system.

cond-mat.supr-con