arXiv subjects

Oksana Zaharko

Publications and source records attributed to Oksana Zaharko.

33 records · Page 2Linked to original sources

arXiv2022

Investigation of metamagnetism and crystal-field splitting in pseudo-hexagonal CeRh$_3$Si$_2$

CeRh$_3$Si$_2$ has been reported to exhibit metamagnetic transitions below 5~K, a giant crystal field splitting, and anisotropic magnetic properties from single crystal magnetization and heat capacity measurements. Here we report results of neutron and x-ray scattering studies of the magnetic structure and crystal-field excitations to further understand the magnetism of this compound. Inelastic neutron scattering (INS) and resonant inelastic x-ray scattering (RIXS) reveal a $J_z$\,=\,1/2 groundstate for Ce when considering the crystallographic $a$ direction as quantization axis, thus explaining the anisotropy of the static susceptibility. Furthermore, we find a total splitting of 78\,meV for the $J$\,=\,5/2 multiplet. The neutron diffraction study in zero field reveals that on cooling from the paramagnetic state, the system first orders at $T_{\text{N}_1}=4.7$\,K in a longitudinal spin density wave with ordered Ce moments along the $b$-axis (i.e. the [0 1 0] crystal direction) and an incommensurate propagation vector $\textbf{k}=(0,0.43,0$). Below the lower-temperature transition $T_{\text{N}_2}=4.48$\,K, the propagation vector locks to the commensurate value $\textbf{k}=(0,0.5,0)$, with a so-called lock-in transition. Our neutron diffraction study in applied magnetic field $H\parallel b$-axis shows a change in the commensurate propagation vector and development of a ferromagnetic component at $H=3$\,kOe, followed by a series of transitions before the fully field-induced ferromagnetic phase is reached at $H = 7$\,kOe. This explains the nature of the steps previously reported in field-dependent magnetization measurements. A very similar behaviour is also observed for the $H\parallel$ [0 1 1] crystal direction.

cond-mat.str-el↗

arXiv2021

Magnetic field induced quantum spin liquid in the two coupled trillium lattices of K$_2$Ni$_2$(SO$_4$)$_3$

Quantum spin liquids are exotic states of matter which form when strongly frustrated magnetic interactions induce a highly entangled quantum paramagnet far below the energy scale of the magnetic interactions. Three-dimensional cases are especially challenging due to the significant reduction of the influence of quantum fluctuations. Here, we report the magnetic characterization of {\kni} forming a three dimensional network of Ni$^{2+}$ spins. Using density functional theory calculations we show that this network consists of two interconnected spin-1 trillium lattices. In the absence of a magnetic field, magnetization, specific heat, neutron scattering and muon spin relaxation experiments demonstrate a highly correlated and dynamic state, coexisting with a peculiar, very small static component exhibiting a strongly renormalized moment. A magnetic field $B \gtrsim 4$ T diminishes the ordered component and drives the system in a pure quantum spin liquid state. This shows that a system of interconnected $S=1$ trillium lattices exhibit a significantly elevated level of geometrical frustration.

cond-mat.str-el↗

arXiv2020

Fractional antiferromagnetic skyrmion lattice induced by anisotropic couplings

Magnetic skyrmions are topological solitons with a nanoscale winding spin texture that hold promise for spintronics applications. Until now, skyrmions have been observed in a variety of magnets that exhibit nearly parallel alignment for the neighbouring spins, but theoretically, skyrmions with anti-parallel neighbouring spins are also possible. The latter, antiferromagnetic skyrmions, may allow more flexible control compared to the conventional ferromagnetic skyrmions. Here, by combining neutron scattering and Monte Carlo simulations, we show that a fractional antiferromagnetic skyrmion lattice with an incipient meron character is stabilized in MnSc$_2$S$_4$ through anisotropic couplings. Our work demonstrates that the theoretically proposed antiferromagnetic skyrmions can be stabilized in real materials and represents an important step towards implementing the antiferromagnetic-skyrmion based spintronic devices.

cond-mat.str-el↗

arXiv2020

Giant anomalous Hall effect in quasi-two-dimensional layered antiferromagnet Co$_{1/3}$NbS$_2$

The discovery of the anomalous Hall effect (AHE) in bulk metallic antiferromagnets (AFMs) motivates the search of the same phenomenon in two-dimensional (2D) systems, where a quantized anomalous Hall conductance can in principle be observed. Here, we present experiments on micro-fabricated devices based on Co$_{1/3}$NbS$_2$, a layered AFM that was recently found to exhibit AHE in bulk crystals below the Néel temperature T$_N$ = 29 K. Transport measurements reveal a pronounced resistivity anisotropy, indicating that upon lowering temperature the electronic coupling between individual atomic layers is increasingly suppressed. The experiments also show an extremely large anomalous Hall conductivity of approximately 400 S/cm, more than one order of magnitude larger than in the bulk, which demonstrates the importance of studying the AHE in small exfoliated crystals, less affected by crystalline defects. Interestingly, the corresponding anomalous Hall conductance, when normalized to the number of contributing atomic planes, is $\sim \, 0.6 \; e^2/h$ per layer, approaching the value expected for the quantized anomalous Hall effect. The observed strong anisotropy of transport and the very large anomalous Hall conductance per layer make the properties of Co$_{1/3}$NbS$_2$ compatible with the presence of partially filled topologically non-trivial 2D bands originating from the magnetic superstructure of the antiferromagnetic state. Isolating atomically thin layers of this material and controlling their charge density may therefore provide a viable route to reveal the occurrence of the quantized AHE in a 2D AFM.

cond-mat.mes-hall↗

arXiv2019

Magnetic phase diagram of the triangular antiferromagnetic $Cs_2CuCl_{4-x}Br_x$ mixed system

The novel magnetic phase diagram of the $Cs_2CuCl_{4-x}Br_x$ mixed system is established by means of single crystal neutron diffraction in the lowest temperature region and zero magnetic field. Two long-range ordered magnetic phases exist in this mixed system depending on the Cl/Br concentration. In the rich Cl concentration range, the ordered magnetic state occurs below the ordering temperature $T_N = 0.51(1)K$ for $Cs_2CuCl_3Br_1$ and at $Cs_2CuCl_{2.6}Br_{1.4}$ below $T_N = 0.24(2)K$. Magnetic order with a temperature-independent position $(0, 0.573(1), 0)$ below the ordering temperature $T_N = 0.63(1)K$ appears in the rich Br concentration for $Cs_2CuCl_{0.6}Br_{3.4}$. Between the rich Cl and rich Br concentration ranges (two magnetic phases), there is a range of x without magnetic order down to $50mK$. A suggestion about the magnetic exchange paths in the $bc$-layer for different regimes is presented, which can be controlled depending on the preferred Br-occupation in the [CuX4] tetrahedra. The density functional theory (DFT) calculations of the exchange coupling constants J, J^' for some ordered compositions of the mixed system $Cs_2CuCl_{4-x}Br_x$ indicate that these are not frustrated.

cond-mat.mtrl-sci↗

arXiv2019

Ordering phenomena of spin trimers accompanied by large geometrical Hall effect

The wavefuntion of conduction electrons moving in the background of a non-coplanar spin structure can gain a quantal phase - Berry phase - as if the electrons were moving in a strong fictitious magnetic field. Such an emergent magnetic field effect is approximately proportional to the solid angle subtended by the spin moments on three neighbouring spin sites, termed the scalar spin chirality. The entire spin chirality of the crystal, unless macroscopically canceled, causes the geometrical Hall effect of real-space Berry-phase origin, whereas the intrinsic anomalous Hall effect (AHE) in a conventional metallic ferromagnet is of the momentum-space Berry-phase origin induced by relativistic spin-orbit coupling (SOC). Here, we report the ordering phenomena of the spin-trimer scalar spin chirality and the consequent large geometrical Hall effect in the breathing kagomé lattice compound Dy$_3$Ru$_4$Al$_{12}$, where the Dy$^{3+}$ moments form non-coplanar spin trimers with local spin chirality. Using neutron diffraction, we show that the local spin chirality of the spin trimers as well as its ferroic/antiferroic orders can be switched by an external magnetic field, accompanying large changes in the geometrical Hall effect. Our finding reveals that systems composed of tunable spin trimers can be a fertile field to explore large emergent electromagnetic responses arising from real-space topological magnetic orders.

cond-mat.str-el↗

arXiv2019

Dzyaloshinskii-Moriya interaction and the magnetic ground state in magnetoelectric LiCoPO$_4$

Magnetic structures are investigated by means of neutron diffraction to shine a light on the intricate details that are believed to be key to understanding the magnetoelectric effect in LiCoPO$_4$ . At zero field, a spontaneous spin canting of $φ= 7(1)^{\circ}$ is found. The spins tilt away from the easy $b$-axis toward $c$. Symmetry considerations lead to the magnetic point group $m'_z$, which is consistent with the previously observed magnetoelectric tensor form and weak ferromagnetic moment along $b$. For magnetic fields applied along $a$, the induced ferromagnetic moment couples via the Dzyaloshinskii-Moriya interaction to yield an additional field-induced spin canting. An upper limit to the size of the interaction is estimated from the canting angle.

cond-mat.str-el↗

arXiv2018

Dipolar spin ice states with fast monopole hopping rate in CdEr$_2$X$_4$ (X = Se, S)

Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr$_2$Se$_4$ is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three-orders of magnitude faster than the canonical spin ice Dy$_2$Ti$_2$O$_7$. In this letter we use diffuse neutron scattering to show that both CdEr$_2$Se$_4$ and CdEr$_2$S$_4$ support a dipolar spin ice state -- the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to that in Dy$_2$Ti$_2$O$_7$, i.e. dilute and uncorrelated, so cannot provide three-orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er$^{3+}$ ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr$_2$X$_4$ (X = Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr$_2$X$_4$ offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples.

cond-mat.str-el↗

arXiv2018

Giant pressure dependence and dimensionality switching in a metal-organic quantum antiferromagnet

We report an extraordinary pressure dependence of the magnetic interactions in the metal-organic system [(CuF$_2$(H$_2$O)$_2$)$_2$pyrazine]. At zero pressure, this material realizes a quasi-two-dimensional (Q2D) spin-1/2 square-lattice Heisenberg antiferromagnet. By high-pressure, high-field susceptibility measurements we show that the dominant exchange parameter is reduced continuously by a factor of 2 upon compression. Above 18 kbar, a phase transition occurs, inducing an orbital re-ordering that switches the dimensionality, transforming the Q2D lattice into weakly coupled chains (Q1D). We explain the microscopic mechanisms for both phenomena by combining detailed x-ray and neutron diffraction results with quantitative modeling using spin-polarized density functional theory.

cond-mat.mtrl-sci↗

arXiv2018

Neutron diffraction study and theoretical analysis of the antiferromagnetic order and diffuse scattering in the layered Kagome system CaBaCo$_2$Fe$_2$O$_7$

The hexagonal swedenborgite, CaBaCo$_2$Fe$_2$O$_7$, is a chiral frustrated antiferromagnet, in which magnetic ions form alternating Kagome and triangular layers. We observe a long range $\sqrt{3} \times \sqrt{3}$ antiferromagnetic order setting in below $T_N = 160$ K by neutron diffraction on single crystals of CaBaCo$_2$Fe$_2$O$_7$. Both magnetization and polarized neutron single crystal diffraction measurements show that close to $T_N$ spins lie predominantly in the $ab$-plane, while upon cooling the spin structure becomes increasingly canted due to Dzyaloshinskii-Moriya interactions. The ordered structure can be described and refined within the magnetic space group $P31m^\prime$. Diffuse scattering between the magnetic peaks reveals that the spin order is partial. Monte Carlo simulations based on a Heisenberg model with two nearest-neighbor exchange interactions show a similar diffuse scattering and coexistence of the $\sqrt{3} \times \sqrt{3}$ order with disorder. The coexistence can be explained by the freedom to vary spins without affecting the long range order, which gives rise to ground-state degeneracy. Polarization analysis of the magnetic peaks indicates the presence of long-period cycloidal spin correlations resulting from the broken inversion symmetry of the lattice, in agreement with our symmetry analysis.

cond-mat.str-el↗

arXiv2018

Singlet state formation and its impact on magnetic structure in tetramer system SeCuO$_3$

We present an experimental investigation of the magnetic structure in a tetramer system SeCuO$_3$ using neutron diffraction and nuclear resonance techniques. We establish a non-collinear, commensurate antiferromagnetic ordering with a propagation vector $\textbf{k} = \left(0,0,1 \right)$. The order parameter follows a critical behavior near $T_N = 8$ K, with a critical exponent $β= 0.32$ in agreement with a 3D universality class. Evidence is presented that a singlet state starts to form on tetramers at temperatures as high as 200 K, and its signature is preserved within the ordered state through a strong renormalization of the ordered magnetic moment on two non-equivalent copper sites, $m_{Cu1} \approx 0.4 μ_B$ and $m_{Cu2} \approx 0.7 μ_B$ at 1.5 K.

cond-mat.str-el↗

arXiv2017

Coulomb spin liquid in anion-disordered pyrochlore Tb$_2$Hf$_2$O$_7$

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. In the pyrochlore Tb$_2$Hf$_2$O$_7$, we demonstrate that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly-fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.

cond-mat.str-el↗

arXiv2017

Magnetic Structure and Dielectric State in the Multiferroic Ca$_{2}$CoSi$_{2}$O$_{7}$

Magnetic structure of the multiferroic Ca$_{2}$CoSi$_{2}$O$_{7}$ was determined by neutron diffraction techniques. Combination of the polycrystalline and single-crystal samples experiments revealed a collinear antiferromagnetic structure with the easy axis along $<$100$>$ directions. The dielectric state was discussed in the framework of the spin-dependent $d$-$p$ hybridization mechanism, leading to the realization of the antiferroelectric structure. The origin of the magnetic anisotropy was discussed in comparison with the isostructural Ba$_{2}$CoGe$_{2}$O$_{7}$.

cond-mat.str-el↗

arXiv2016

Spiral spin-liquid and the emergence of a vortex-like state in MnSc$_2$S$_4$

Spirals and helices are common motifs of long-range order in magnetic solids, and they may also be organized into more complex emergent structures such as magnetic skyrmions and vortices. A new type of spiral state, the spiral spin-liquid, in which spins fluctuate collectively as spirals, has recently been predicted to exist. Here, using neutron scattering techniques, we experimentally prove the existence of a spiral spin-liquid in MnSc$_2$S$_4$ by directly observing the 'spiral surface' - a continuous surface of spiral propagation vectors in reciprocal space. We elucidate the multi-step ordering behavior of the spiral spin-liquid, and discover a vortex-like triple-q phase on application of a magnetic field. Our results prove the effectiveness of the $J_1$-$J_2$ Hamiltonian on the diamond lattice as a model for the spiral spin-liquid state in MnSc$_2$S$_4$, and also demonstrate a new way to realize a magnetic vortex lattice.

cond-mat.str-el↗

arXiv2014

Magnetic nano-fluctuations in a frustrated magnet

Frustrated systems exhibit remarkable properties due to the high degeneracy of their ground states. Stabilised by competing interactions, a rich diversity of typically nanometre-sized phase structures appear in polymer and colloidal systems, while the surface of ice pre-melts due to geometrically frustrated interactions. Atomic spin systems where magnetic interactions are frustrated by lattice geometry provide a fruitful source of emergent phenomena, such as fractionalised excitations analogous to magnetic monopoles. The degeneracy inherent in frustrated systems may prevail all the way down to absolute zero temperature, or it may be lifted by small perturbations or entropic effects. In the geometrically frustrated Ising--like magnet Ca3Co2O6, we follow the temporal and spatial evolution of nanoscale magnetic fluctuations firmly embedded inside the spin--density--wave magnetic structure. These fluctuations are a signature of a competing ferrimagnetic phase with an incommensurability that is different from, but determined by the host. As the temperature is lowered, the fluctuations slow down into a super-paramagnetic regime of stable spatiotemporal nano-structures.

cond-mat.str-el↗