arXiv subjects

A. Zorko

Publications and source records attributed to A. Zorko.

At least 37 records · Page 2Linked to original sources

arXiv2020

Development of short and long-range magnetic order in the double perovskite based frustrated triangular lattice antiferromagnet Ba2MnTeO6

Oxide double perovskites wherein octahedra formed by both 3d elements and sp-based heavy elements give rise to unconventional magnetic ordering and correlated quantum phenomena crucial for futuristic applications. Here, by carrying out experimental and first principles investigations, we present the electronic structure and magnetic phases of Ba2MnTeO6, where Mn^2+ ions with S = 5/2 spins constitute a perfect triangular lattice. The magnetic susceptibility reveals a large Curie- Weiss temperature -152 K suggesting the presence of strong antiferromagnetic interactions between Mn^2+ moments in the spin lattice. A phase transition at 20 K is revealed by magnetic susceptibility and specific heat which is attributed to the presence of a sizeable inter-plane interactions. Below the transition temperature, the specific heat data show antiferromagnetic magnon excitations with a gap of 1.4 K. Furthermore, muon spin-relaxation reveals the presence of static internal fields in the ordered state and provides strong evidence of short-range spin correlations for T > TN. The DFT+U calculations and spin-dimer analysis infer that Heisenberg interactions govern the inter and intra-layer spin-frustrations in this perovskite. The inter and intra-layer exchange interactions are of comparable strengths (J1 = 4.6 K, J2 = 0.92 J1). However, a weak third nearest-neighbor ferromagnetic inter-layer interaction exists (J3=-0.04 J1) due to double-exchange interaction via the linear path Mn-O-Te-O-Mn. The combined effect of J2 and J3 interactions stabilizes a three dimensional long-range magnetic ordering in this frustrated magnet.

cond-mat.str-el↗

arXiv2020

Thermal effects versus spin nematicity in a frustrated spin-1/2 chain

The spin-nematic phase is an intriguing state of matter that lacks usual long-range dipolar order, yet it exhibits higher multipolar order. This makes its detection extremely difficult and controversial. Recently, nuclear magnetic resonance (NMR) has been proposed as one of the most suitable techniques to confirm its existence. We report a $^{17}$O NMR observation of the reduction of the local magnetization in the polarized state of the frustrated spin-1/2 chain $β$-TeVO$_4$, which was previously proposed to be a fingerprint of the spin-nematic behavior. However, our detailed study shows that the detected missing fraction of the magnetization, probed by NMR frequency shift, is thermally activated, thus undermining the presence of the spin-nematic phase in the investigated compound. This highlights the importance of careful considerations of temperature-dependent NMR shift that has been overlooked in previous studies of spin nematicity.

cond-mat.str-el↗

arXiv2020

Origin of Magnetic Ordering in a Structurally-Perfect Quantum Kagome Antiferromagnet

The ground state of the simple Heisenberg nearest-neighbor quantum kagome antiferromagnetic model is a magnetically disordered spin liquid, yet various perturbations may lead to fundamentally different states. Here we disclose the origin of magnetic ordering in the structurally-perfect kagome material YCu$_3$(OH)$_6$Cl$_3$, which is free of the widespread impurity problem. {\it Ab-initio} calculations and modeling of its magnetic susceptibility reveal that, similar to the archetypal case of herbertsmithite, the nearest-neighbor exchange is by far the dominant isotropic interaction. Dzyaloshinskii-Moriya (DM) magnetic anisotropy deduced from electron spin resonance and specific-heat measurements is, however, significantly larger than in herbertsmithite. By enhancing spin correlations within kagome planes, this anisotropy is essential for magnetic ordering. Our study isolates the effect of DM anisotropy from other perturbations and unambiguously confirms the theoretical phase diagram.

cond-mat.str-el↗

arXiv2019

Spin-dimer ground state driven by consecutive charge and orbital ordering transitions in the anionic mixed-valence compound Rb$_4$O$_6$

Recently, a Verwey-type transition in the mixed-valence alkali sesquioxide Cs$_4$O$_6$ was deduced from the charge ordering of molecular peroxide O$_2^{2-}$ and superoxide O$_2^-$ anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al, Sci. Adv 4, eaap7581 (2018)]. Here, we report that in the sister compound Rb$_4$O$_6$ a similar Verwey-type charge ordering transition is strongly linked to O$_2^-$ orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering and a cubic-to-tetragonal transition at $T_{\rm CO}=290$ K, which is followed by a further structural instability at $T_{\rm s}=92$ K that involves an additional reorientation of magnetic O$_2^-$ anions. Magnetic resonance techniques supported by density functional theory computations suggest the emergence of a peculiar type of $π^*$-orbital ordering of the magnetically active O$_2^-$ units, which promotes the formation of a quantum spin state composed of weakly coupled spin dimers. These results reveal that similarly as in 3$d$ transition metal compounds, also in in the $π^*$ open-shell alkali sesquioxides the interplay between Jahn-Teller-like electron-lattice coupling and Kugel-Khomskii-type superexchange determines the nature of orbital ordering and the magnetic ground state.

cond-mat.str-el↗

arXiv2019

Gapless ground state in the archetypal quantum kagome antiferromagnet ZnCu$_3$(OH)$_6$Cl$_2$

Spin liquids are exotic phases of quantum matter challenging Landau's paradigm of symmetry-breaking phase transitions. Despite strong exchange interactions, spins do not order or freeze down to zero temperature. While well-established for 1D quantum antiferromagnets, in higher dimension where quantum fluctuations are less acute, realizing and understanding such states represent major issues, both theoretical and experimental. In this respect the simplest nearest-neighbor Heisenberg antiferromagnet Hamiltonian on the highly frustrated kagome lattice has proven to be a fascinating and inspiring model. The exact nature of its ground state remains elusive and the existence of a spin-gap is the first key-issue to be addressed to discriminate between the various classes of proposed spin liquids. Here, through low-temperature Nuclear Magnetic Resonance (NMR) contrast experiments on high quality single crystals, we single out the kagome susceptibility and the corresponding dynamics in the kagome archetype, the mineral herbertsmithite, ZnCu$_3$(OH)$_6$Cl$_2$. We firmly conclude that this material does not harbor any spin-gap, which restores a convergence with recent numerical results promoting a gapless Dirac spin liquid as the ground state of the Heisenberg kagome antiferromagnet.

cond-mat.str-el↗

arXiv2019

Negative-vector-chirality 120$^\circ$ spin structure in the defect- and distortion-free quantum kagome antiferromagnet YCu$_3$(OH)$_6$Cl$_3$

The magnetic ground state of the ideal quantum kagome antiferromagnet (QKA) has been a long-standing puzzle, mainly because perturbations to the nearest-neighbor isotropic Heisenberg Hamiltonian can lead to various fundamentally different ground states. Here we investigate a recently synthesized QKA representative YCu$_3$(OH)$_6$Cl$_3$, where perturbations commonly present in real materials, like lattice distortion and intersite ion mixing, are absent. Nevertheless, this compound enters a long-range magnetically ordered state below $T_N=15$ K. Our powder neutron diffraction experiment reveals that its magnetic structure corresponds to a coplanar $120^\circ$ state with negative vector spin chirality. The ordered magnetic moments are suppressed to $0.42(2)μ_B$, which is consistent with the previously detected spin dynamics persisting to the lowest experimentally accessible temperatures. This indicates either a coexistence of magnetic order and disorder or the presence of strong quantum fluctuations in the ground state of YCu$_3$(OH)$_6$Cl$_3$. The origin of the magnetic order is sought in terms of Dzyaloshinskii-Moriya magnetic anisotropy and further-neighbor isotropic exchange interactions.

cond-mat.str-el↗

arXiv2019

Magnetic ground state of the frustrated spin-1/2 chain compound $β$-TeVO$_4$ at high magnetic fields

Frustrated spin-1/2 chains, despite the apparent simplicity, exhibit remarkably rich phase diagram comprising vector-chiral (VC), spin-density-wave (SDW) and multipolar/spin-nematic phases as a function of the magnetic field. Here we report a study of $β$-TeVO$_4$, an archetype of such compounds, based on magnetization and neutron diffraction measurements up to 25 T. We find the transition from the helical VC ground state to the SDW state at $\sim$3 T for the magnetic field along the $a$ and $c$ crystal axes, and at $\sim$9 T for the field along the $b$ axis. The high-field (HF) state, existing above $\sim$18 T, i.e., above $\sim$1/2 of the saturated magnetization, is an incommensurate magnetically ordered state and not the spin-nematic state, as theoretically predicted for the isotropic frustrated spin-1/2 chain. The HF state is likely driven by sizable interchain interactions and symmetric intrachain anisotropies uncovered in previous studies. Consequently, the potential existence of the spin nematic phase in $β$-TeVO$_4$ is limited to a narrow field range, i.e., a few tenths of a tesla bellow the saturation of the magnetization, as also found in other frustrated spin-1/2 chain compounds.

cond-mat.str-el↗

arXiv2019

Coexistence of magnetic order and persistent spin dynamics in a quantum kagome antiferromagnet with no intersite mixing

One of the key questions concerning frustrated lattices that has lately emerged is the role of disorder in inducing spin-liquid-like properties. In this context, the quantum kagome antiferromagnets YCu$_3$(OH)$_6$Cl$_3$, which has been recently reported as the first geometrically perfect realization of the kagome lattice with negligible magnetic/non-magnetic intersite mixing and a possible quantum-spin-liquid ground state, is of particular interest. However, contrary to previous conjectures, here we show clear evidence of bulk magnetic ordering in this compound below $T_N=15$\,K by combining bulk magnetization and heat capacity measurements, and local-probe muon spin relaxation measurements. The magnetic ordering in this material is rather unconventional in several respects. Firstly, a crossover regime where the ordered state coexists with the paramagnetic state extends down to $T_N/3$ and, secondly, the fluctuation crossover is shifted far below $T_N$. Moreover, a reduced magnetic-entropy release at $T_N$ and persistent spin dynamics that is observed at temperatures as low as $T/T_N=1/300$ could be a sign of emergent excitations of correlated spin-loops or, alternatively, a sign of fragmentation of each magnetic moment into an ordered and a fluctuating part.

cond-mat.str-el↗

arXiv2019

Elementary excitation in the spin-stripe phase in quantum chains

Elementary excitations in condensed matter capture the complex many-body dynamics of interacting basic entities in a simple quasiparticle picture. In magnetic systems the most established quasiparticles are magnons, collective excitations that reside in ordered spin structures, and spinons, their fractional counterparts that emerge in disordered, yet correlated spin states. Here we report on the discovery of elementary excitation inherent to spin-stripe order that represents a bound state of two phason quasiparticles, resulting in a wiggling-like motion of the magnetic moments. We observe these excitations, which we dub "wigglons", in the frustrated zigzag spin-1/2 chain compound $β$-TeVO$_4$, where they give rise to unusual low-frequency spin dynamics in the spin-stripe phase. This result provides insights into the stripe physics of strongly-correlated electron systems.

cond-mat.str-el↗

arXiv2019

Kondo screening in a charge-insulating spinon metal

The Kondo effect, an eminent manifestation of many-body physics in condensed matter, is traditionally explained as exchange scattering of conduction electrons on a spinful impurity in a metal. The resulting screening of the impurity's local moment by the electron Fermi sea is characterized by a Kondo temperature $T_K$, below which the system enters a non-perturbative strongly-coupled regime. In recent years, this effect has found its realizations beyond the bulk-metal paradigm in many other itinerant-electron systems, such as quantum dots in semiconductor heterostructures and in nanomaterials, quantum point contacts, and graphene. Here we report on the first experimental observation of the Kondo screening by chargeless quasiparticles. This occurs in a charge-insulating quantum spin liquid, where spinon excitations forming a Fermi surface take the role of conduction electrons. The observed impurity behaviour therefore bears a strong resemblance to the conventional case in a metal. The discovered spinon-based Kondo effect provides a prominent platform for characterising and possibly manipulating enigmatic host spin liquids.

cond-mat.str-el↗

arXiv2018

Coexisting spinons and magnons in frustrated zigzag spin-1/2 chain compound $β$-TeVO$_4$

We investigate magnetic excitations in the frustrated zigzag spin-1/2 chain compound $β$-TeVO$_4$ by inelastic neutron scattering. In the magnetically ordered ground state, the excitation spectrum exhibits coexisting magnon dispersion, characteristic of long-range magnetic order, and a spinon-like continuum that prevails above 2 meV, indicating the dominance of intrachain interactions. Combining linear-spin-wave-theory and pre-calculated spinon-continuum results, we reproduce the experimental spectrum. Our analysis offers a minimal exchange-network model which determines dominant intrachain interactions, their anisotropies and weak interchain interactions. The obtained parameters explain the magnetic ordering vector and spin excitations in the magnetic ground state.

cond-mat.str-el↗

arXiv2018

Magnetic inhomogeneity in the copper pseudochalcogenide CuNCN

Copper carbodiimide, CuNCN, is a geometrically frustrated nitrogen-based analogue of cupric oxide, whose magnetism remains ambiguous. Here, we employ a combination of local-probe techniques, including $^{63,\, 65}$Cu nuclear quadrupole resonance, $^{13}$C nuclear magnetic resonance and muon spin rotation to show that the magnetic ground state of the Cu$^{2+}$ ($S=1/2$) spins is frozen and disordered. Moreover, these complementary experiments unequivocally establish an onset of intrinsically inhomogeneous magnetic state at $T_h=80$ K. Below $T_h$, the low-temperature frozen component coexist with the remnant high-temperature dynamical component down to $T_l = 20$ K, where the latter finally ceases to exist. Based on a scaling of internal magnetic fields of both components we conclude that the two components coexist on a microscopic level.

cond-mat.str-el↗

arXiv2017

Field-Induced Instability of a Gapless Spin Liquid with a Spinon Fermi Surface

The ground state of the quantum kagome antiferromagnet Zn-brochantite, ZnCu$_3$(OH)$_6$SO$_4$, which is one of only a few known spin-liquid (SL) realizations in two or three dimensions, has been described as a gapless SL with a spinon Fermi surface. Employing nuclear magnetic resonance in a broad magnetic-field range down to millikelvin temperatures, we show that in applied magnetic fields this enigmatic state is intrinsically unstable against a SL with a full or a partial gap. A similar instability of the gapless Fermi-surface SL was previously encountered in an organic triangular-lattice antiferromagnet, suggesting a common destabilization mechanism that most likely arises from spinon pairing. A salient property of this instability is that an infinitesimal field suffices to induce it, as predicted theoretically for some other types of gapless SL's.

cond-mat.str-el↗

arXiv2017

Observation of two types of anyons in the Kitaev honeycomb magnet

Quantum spin liquid is a disordered magnetic state with fractional spin excitations. Its clearest example is found in an exactly solved Kitaev honeycomb model where a spin flip fractionalizes into two types of anyons, quasiparticles that are neither fermions nor bosons: a pair of gauge fluxes and a Majorana fermion. Here we demonstrate this kind of fractionalization in the Kitaev paramagnetic state of the honeycomb magnet $α$-RuCl$_3$. The spin-excitation gap measured by nuclear magnetic resonance consists of the predicted Majorana fermion contribution following the cube of the applied magnetic field, and a finite zero-field contribution matching the predicted size of the gauge-flux gap. The observed fractionalization into gapped anyons survives in a broad range of temperatures and magnetic fields despite inevitable non-Kitaev interactions between the spins, which are predicted to drive the system towards a gapless ground state. The gapped character of both anyons is crucial for their potential application in topological quantum computing.

cond-mat.str-el↗

arXiv2017

Symmetry Reduction in the Quantum Kagome Antiferromagnet Herbertsmithite

Employing complementary torque magnetometry and electron spin resonance on single crystals of herbertsmithite, the closest realization to date of a quantum kagome antiferromagnet featuring a spin-liquid ground state, we provide novel insight into different contributions to its magnetism. At low temperatures, two distinct types of defects with different magnetic couplings to the kagome spins are found. Surprisingly, their magnetic response contradicts the three-fold symmetry of the ideal kagome lattice, suggesting the presence of a global structural distortion that may be related to the establishment of the spin-liquid ground state.

cond-mat.str-el↗

arXiv2016

Exchange anisotropy as mechanism for spin-stripe formation in frustrated spin chains

We investigate the spin-stripe mechanism responsible for the peculiar nanometer modulation of the incommensurate magnetic order that emerges between the vector-chiral and the spin-density-wave phase in the frustrated zigzag spin-1/2 chain compound $β$-TeVO$_4$. A combination of magnetic-torque, neutron-diffraction and spherical-neutron-polarimetry measurements is employed to determine the complex magnetic structures of all three ordered phases. Based on these results, we develop a simple phenomenological model, which exposes the exchange anisotropy as the key ingredient for the spin-stripe formation in frustrated spin systems.

cond-mat.str-el↗

arXiv2016

$μ$SR Insight into the Impurity Problem in Quantum Kagome Antiferromagnets

Impurities, which are inherently present in any real material, may play an important role in the magnetism of frustrated spin systems with spin-liquid ground states. We address the impurity issue in quantum kagome antiferromagnets by investigating ZnCu$_3$(OH)$_6$SO$_4$ (Zn-brochantite) by means of muon spin spectroscopy. We show that muons couple to the impurity magnetism, originating from Cu-Zn intersite disorder, and that the impurities are highly correlated with the kagome spins, allowing us to probe the intrinsic kagome physics via a Kondo-like effect. The low-temperature plateau in local susceptibility identifies the spin-liquid ground state as being gapless. The corresponding spin fluctuations exhibit an unconventional spectral density and an intriguing field dependence.

cond-mat.str-el↗

arXiv2016

Helical bunching and symmetry lowering inducing multiferroicity in Fe langasites

The chiral Fe-based langasites represent model systems of triangle-based frustrated magnets with a strong potential for multiferroicity. We report neutron scattering measurements for the multichiral Ba3MFe3Si2O14 (M = Nb, Ta) langasites revealing new important features of the magnetic order of these systems: the bunching of the helical modulation along the c-axis and the in-plane distortion of the 120{\textdegree} Fe-spin arrangement. We discuss these subtle features in terms of the microscopic spin Hamiltonian, and provide the link to the magnetically-induced electric polarization observed in these systems. Thus, our findings put the multiferroicity of this attractive family of materials on solid ground.

cond-mat.str-el↗