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Ivica Živković

Publications and source records attributed to Ivica Živković.

12 recordsLinked to original sources

Reentrant behavior and possible $2/3$ magnetization plateau on the double-trillium langbeinite K$_2$Ni$_2$(SO$_4$)$_3$

K$_2$Ni$_2$(SO$_4$)$_3$ is a member of the langbeinite family, consisting of two intertwined $S=1$ trillium lattices, out of which one is strongly coupled (strong-TL) and the other is weakly coupled (weak-TL). Further inter-trillium interactions give rise to a highly-frustrated Heisenberg Hamiltonian. Despite ordering at low temperatures, K$_2$Ni$_2$(SO$_4$)$_3$ lies close in parameter space to a spin-liquid region that surrounds the tetratrillium limit, where each triangle belonging to strong-TL turns into a tetrahedron by connecting to a single spin from weak-TL. Here, we compare the experimentally determined magnetization process using pulsed magnetic fields up to $40$ T with classical Monte Carlo calculations, uncovering a series of phase transitions at both low and intermediate fields. Furthermore, we reveal a signature of a $2/3$ magnetization plateau consisting of a $1/3$ phase on strong-TL and a fully polarized phase on weak-TL. Although in the classical limit no plateau is expected, we find a very prominent dome structure reflecting the tendency of the system to stabilize this particular spin configuration. The presence of a dome leads to a reentrant phenomenon in which the system recovers the Hamiltonian symmetries when increasing the magnetic field. Finally, we show that this plateau-like phase is also present in the classical Heisenberg model on the single trillium and tetratrillium lattices, indicating its possible presence in the large family of double-trillium langbeinite compounds. Our findings motivate future studies on the presence of the plateau phase in the quantum limit of both trillium and double-trillium materials within the langbeinite family.

cond-mat.str-el↗

Single-ion anisotropy-stabilized short-period helimagnetism in frustrated chiral Co$_5$TeO$_8$

Chiral spin textures in magnetic insulators promise magneto-electric (ME) spintronics with orders-of-magnitude lower power consumption than metallic systems. However, realizing the short magnetic periods required for high-density device integration remains difficult, as conventional Dzyaloshinskii-Moriya interaction (DMI)-based mechanisms typically constrain spiral periods to tens of nanometers. While theory predicts that strong single-ion anisotropy (SIA) on frustrated lattices can stabilize complex non-coplanar textures, the potential for using this mechanism to engineer such compact textures remains largely unexplored. Here we report that a cubic chiral insulator Co$_5$TeO$_8$ provides an experimental example of this paradigm. Comprehensive neutron scattering and magnetometry reveal helimagnetic spirals with continuously tunable pitch of 5.7-10 nm embedded in a complex phase diagram spanning eight distinct phases. Capacitance anomalies throughout the phase diagram indicate magneto-electric coupling, pointing to the possibility of future $E$-field control of these textures. The temperature- and field-dependence of the helical wavevector strongly support a scenario in which site-dependent SIA provides the leading contribution to the selection of the helical period from a frustration-induced degenerate manifold. Consistent with this interpretation, $ab\,initio$ calculations place SIA approximately an order of magnitude above DMI, distinct from conventional helimagnets. Co$_5$TeO$_8$ thus offers an experimental realization of sub-10 nm helimagnetism and motivates a design principle for anisotropy-engineered correlated insulators.

cond-mat.str-el↗

Persistent quantum vibronic dynamics in a $5d^1$ double perovskite oxide

Quantum entanglement between the spin, orbital, and lattice degrees of freedom in condensed matter systems can emerge due to an interplay between spin-orbit and vibronic interactions. Heavy transition metal ions decorated on a face-centered cubic lattice, for example, in $5d^1$ double perovskites, are particularly suited to support these quantum entangled states, but direct evidence has not yet been presented. In this work, we report additional peaks in the low-energy spectra of a $5d^1$ double perovskite, Ba$_2$CaReO$_6$, which cannot be explained by adopting a purely classical description of lattice vibrations. Instead, our theoretical analysis demonstrates that these spectroscopic signatures are characteristic of orbital-lattice entangled states in Ba$_2$CaReO$_6$. Crucially, both theory and experiment demonstrate that these quantum-entangled states persist to low temperatures, despite the onset of multipolar order.

cond-mat.str-el↗

Fluctuation-driven topological Hall effect in room-temperature itinerant helimagnet Fe3Ga4

The topological Hall effect (THE) is a hallmark of a non-trivial geometric spin arrangement in a magnetic metal, originating from a finite scalar spin chirality (SSC). The associated Berry phase is often a consequence of non-coplanar magnetic structures identified by multiple k-vectors. For single-k magnetic structures however with zero SSC, the emergence of a finite topological Hall signal presents a conceptual challenge. Here, we report that a fluctuation-driven mechanism involving chiral magnons is responsible for the observed THE in a low-symmetry compound, monoclinic Fe3Ga4. Through neutron scattering experiments, we discovered several nontrivial magnetic phases in this system. In our focus is the helical spiral phase at room temperature, which transforms into a transverse conical state in applied magnetic field, supporting a significant THE signal up to and above room temperature. Our work offers a fresh perspective in the search for novel materials with intertwined topological magnetic and transport properties.

cond-mat.str-el↗

Spectroscopic signatures and origin of a hidden order in Ba$_2$MgReO$_6$

Clarifying the underlying mechanisms that govern ordering transitions in condensed matter systems is crucial for comprehending emergent properties and phenomena. While transitions are often classified as electronically driven or lattice-driven, we present a departure from this conventional paradigm in the case of the double perovskite Ba$_2$MgReO$_6$. Leveraging resonant and non-resonant elastic x-ray scattering techniques, we unveil the simultaneous ordering of structural distortions and charge quadrupoles at a critical temperature of $T_\mathrm{q}$$\sim$33 K. Using a variety of complementary first-principles-based computational techniques, we demonstrate that while electronic interactions drive the ordering at $T_\mathrm{q}$, it is ultimately the lattice that dictates the specific ground state that emerges. Our findings highlight the crucial interplay between electronic and lattice degrees of freedom, providing a unified framework to understand and predict unconventional emergent phenomena in quantum materials.

cond-mat.str-el↗

Electronic transport and magnetism in the alternating stack of metallic and highly frustrated magnetic layers in Co$_{1/3}$NbS$_2$

Transition-metal dichalcogenides (TMDs) are layered compounds that support many electronic phases, including various charge density waves, superconducting, and Mott insulating states. Their intercalation with magnetic ions introduces magnetic sublayers, which strongly influence the coupling between host layers, and feature various magnetic states adjustable by external means. Co$_{1/3}$NbS$_2$ hosts a particularly sensitive magnetic subsystem with the lowest magnetic ordering temperature in the family of magnetically intercalated TMDs, and the only one where the complete suppression of magnetic order under pressure has been recently suggested. By combining the results of several experimental methods, electronic ab initio calculations, and modeling, we develop insights into the mechanisms of electric transport, magnetic ordering, and their interaction in this compound. The elastic neutron scattering is used to directly follow the evolution of the antiferromagnetic order parameter with pressure and temperature. Our results unambiguously disclose the complete suppression of the observed magnetic order around 1.7 GPa. We delve into possible mechanisms of magnetic order suppression under pressure, highlighting the role of magnetic frustrations indicated by magnetic susceptibility measurements and ab-initio calculations. Electronic conduction anisotropy is measured in the wide temperature and pressure range. Here we show that the transport in directions along and perpendicular to layers respond differently to the appearance of magnetic ordering or the application of the hydrostatic pressure. We propose the 'spin-valve' mechanism where the intercalated Co ions act as spin-selective electrical transport bridges between host layers. The mechanism applies to various magnetic states and can be extended to other magnetically intercalated TMDs.

cond-mat.str-el↗

Structure, heat capacity and Raman spectra of mm-sized Ba$_{2}$MgWO$_{6}$ single crystals synthesized by BaCl$_{2}$-MgCl$_{2}$ flux method

We present a new method of Ba$_{2}$MgWO$_{6}$ single crystal synthesis that allows to grow larger crystals using BaCl$_{2}$ and MgCl$_{2}$ flux. Difficulties to grow single crystal of a size suitable for macroscopic material property measurements caused the majority of characterisation being published on polycrystalline samples. Single crystal diffraction and energy dispersive X-ray analysis confirmed high quality of synthesised samples. Heat capacity measurements from 300~K to 2~K do not show any transitions. However, Raman spectra measured down to 77~K contain additional peaks at all temperatures probed, which is in a contrast with only 4 Raman active modes expected from the reducible representation. This calls for a more detailed study of potential symmetry breaking that could also influence the electronic properties of the material.

cond-mat.mtrl-sci↗

Experimental and theoretical thermodynamic studies in Ba$_2$MgReO$_6$ -- the ground state in the context of Jahn-Teller effect

We address the degeneracy of the ground state multiplet on the 5$d^1$ Re$^{6+}$ ion in double perovskite Ba$_{2}$MgReO$_{6}$ using a combination of specific heat measurements and density functional calculations. For Ba$_{2}$MgReO$_{6}$, two different ground state multiplets have previously been proposed - a quartet (with degeneracy $N$=4) [1] and a doublet ($N$=2) [2]. Here we employ two independent methods for the estimation of phonon contribution in heat capacity data to obtain the magnetic entropy $S_{mag}$, which reflects the degeneracy of the ground state multiplet $N$ through $S_{mag}=R$ln$N$. In both cases, we obtain a better fit to $S_{mag}=R$ln2 indicating evidence of $N$=2 degeneracy in the range from 2 to 120~K. The detailed nature of the ground state multiplet in Ba$_{2}$MgReO$_{6}$ remains an open question.

cond-mat.mtrl-sci↗

Charge multipoles correlations and order in Cs$_2$TaCl$_6$

We examine the role of charge, structural, and spin degrees of freedom in the previously poorly understood phase transition in the 5$d^1$ transition-metal double perovskite Cs$_2$TaCl$_6$, using a combination of computational and experimental techniques. Our heat capacity measurements of single-crystalline Cs$_2$TaCl$_6$, reveal a clear anomaly at the transition temperature, $T_\mathrm{Q}$, which was not previously observed in polycrystalline samples. Density functional calculations indicate the emergence of local charge quadrupoles in the cubic phase, mediated by the paramagnetic spins or local structural distortions which then develop into long-range ordered charge quadrupoles in the tetragonal phase. Our resonant elastic x-ray scattering on Cs$_2$TaCl$_6$, single crystals lend support to our calculations. Our work provides new insight into the phase transition in Cs$_2$TaCl$_6$, at $T_\mathrm{Q}$, and demonstrates the utility of this combination of techniques in understanding the complex physics of hidden orders in paramagnetic spin-orbit-entangled compounds.

cond-mat.mtrl-sci↗

Synthesis of Murunskite Single Crystals: A Bridge Between Cuprates and Pnictides

Numerous contemporary investigations in condensed matter physics are devoted to high temperature (high-$T_c$ ) cuprate superconductors. Despite its unique effulgence among research subjects, the enigma of the high-$T_c$ mechanism still persists. One way to advance its understanding is to discover and study new analogous systems. Here we begin a novel exploration of the natural mineral murunskite, K$_2$FeCu$_3$S$_4$, as an interpolation compound between cuprates and ferropnictides, the only known high-$T_c$ superconductors at ambient pressure. Because in-depth studies can be carried out only on single crystals, we have mastered the synthesis and growth of high quality specimens. Similar to the cuprate parent compounds, these show semiconducting behavior in resistivity and optical transmittance, and an antiferromagnetic ordering at 100 K. Spectroscopy (XPS) and calculations (DFT) concur that the sulfur 3$p$ orbitals are partially open, making them accessible for charge manipulation, which is a prerequisite for superconductivity in analogous layered structures. DFT indicates that the valence band is more cuprate-like, while the conduction band is more pnictide-like. With appropriate doping strategies, this parent compound promises exciting future developments.

cond-mat.mtrl-sci↗

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↗

Doping-induced quantum cross-over in Er$_2$Ti$_{2-x}$Sn$_x$O$_7$

We present the results of the investigation of magnetic properties of the Er$_2$Ti$_{2-x}$Sn$_x$O$_7$ series. For small doping values the ordering temperature decreases linearly with $x$ while the moment configuration remains the same as in the $x = 0$ parent compound. Around $x = 1.7$ doping level we observe a change in the behavior, where the ordering temperature starts to increase and new magnetic Bragg peaks appear. For the first time we present evidence of a long-range order (LRO) in Er$_2$Sn$_2$O$_7$ ($x = 2.0$) below $T_N = 130$ mK. It is revealed that the moment configuration corresponds to a Palmer-Chalker type with a value of the magnetic moment significantly renormalized compared to $x = 0$. We discuss our results in the framework of a possible quantum phase transition occurring close to $x = 1.7$.

cond-mat.str-el↗