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M. Pregelj

Publications and source records attributed to M. Pregelj.

At least 19 recordsLinked to original sources

Coexistence of static order and spin dynamics in an S = 5/2 frustrated triangular antiferromagnet

Frustrated triangular-lattice antiferromagnets in the classical high-spin limit provide a paradigmatic setting in which the interplay of competing exchange interactions, anisotropy, and collective degrees of freedom can lead to unconventional low-energy excitations, anomalous criticality, and persistent dynamical responses. Here, we present comprehensive thermodynamic, $\mu$SR, and neutron diffraction experiments, along with first-principles calculations, on a triangular-lattice antiferromagnet, MnSnB$_2$O$_6$, where Mn$^{2+}$ ($S=5/2$) moments form a nearly perfect 2D triangular network without any anti-site disorder. The Curie-Weiss fit to the magnetic susceptibility yields a moderate Curie-Weiss temperature of $-12$ K, indicating dominant antiferromagnetic interactions between Mn$^{2+}$ moments, which is supported by first-principles calculations. Specific-heat measurements reveal the onset of long-range magnetic order at $T_{\rm N}\approx 1$ K, which is ascribed to intraplane exchange interactions. The specific heat exhibits pronounced short-range correlations above $T_{\rm N}$ and an unconventional power-law behavior, $C\propto T^{1.37}$, deep in the ordered state, suggesting the presence of non-trivial low-energy excitations. Zero-field $\mu$SR experiments down to 50~mK confirm the presence of magnetic ordering below $T_{\rm N}$, in agreement with thermodynamic and neutron diffraction experiments. The $\mu$SR measurements detect persistent spin dynamics coexisting with static magnetic order. The temperature evolution of the order parameter down to 50~mK from neutron diffraction suggests that the ordered state is consistent with a 3D Ising-like antiferromagnet. This family of archetypal frustrated magnets offers a promising venue for the experimental realization of emergent phenomena governed by competing exchange interactions and exotic low-energy excitations.

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Exotic magnetism and persistent spin dynamics in a frustrated Jeff = 1/2 triangular lattice antiferromagnet

The delicate interplay between competing degrees of freedom, anisotropy, and frustration-induced strong quantum fluctuations in pseudospin-$J_{\rm eff}=1/2$ rare-earth triangular-lattice antiferromagnets offers a promising platform for the experimental realization of exotic states with nontrivial low-energy excitations. Here, we present thermodynamic, inelastic neutron scattering (INS), and muon spin relaxation ($\mu$SR) investigations of the frustrated magnet K$_3$NdTe$_2$O$9$, in which Nd$^{3+}$ ions constitute a structurally perfect triangular lattice with no detectable site disorder. The experiments reveal the realization of a Kramers doublet ground state with $J{\rm eff}=1/2$ moments, well separated from the first excited state, which interact antiferromagnetically with an exchange interaction of $\sim$0.6 K between the Nd$^{3+}$ moments in the triangular plane. The absence of oscillations and the so-called 1/3 plateau in the zero-field $\mu$SR asymmetry down to 50 mK rules out long-range magnetic ordering and spin freezing on the $\mu$SR time scale, respectively. The temperature dependence of the zero-field $\mu$SR relaxation rate is well described by the Orbach relaxation mechanism, indicating the existence of fluctuating moments in the ground state of this frustrated magnet. Our results demonstrate exotic magnetism and persistent spin dynamics down to 50 mK. These observations establish this new family of frustrated rare-earth triangular-lattice antiferromagnets as a promising venue for the experimental realization of nontrivial quantum states with exotic low-energy excitations.

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Quantum spin liquid on a 3D bipartite lattice of spin trimers stabilized by enhanced effective anisotropy

Quantum spin liquids (QSLs) represent highly entangled states of matter in which frustration-induced quantum fluctuations suppress any symmetry-breaking phase transition down to absolute zero, giving rise to fractionalized excitations and emergent gauge fields. Theoretically, bond anisotropy can stabilize QSLs even on bipartite lattices, as exemplified by the Kitaev honeycomb model; however, no material has so far been established to realize such a state as its true ground state. Here we identify the three-dimensional spin-trimer magnet KBa$_3$Ca$_4$Cu$_3$V$_7$O$_{28}$ as a promising candidate for a bipartite quantum spin liquid persisting to the lowest temperatures. Strongly coupled Cu$^{2+}$ trimers form effective pseudospin-1/2 degrees of freedom upon cooling, which in turn constitute a three-dimensional bipartite network. Bulk thermodynamic measurements, neutron scattering, $\mu$SR, and NMR detect no spin freezing or symmetry-breaking phase transition down to 20 mK, but instead reveal a gapless dynamical ground state with algebraic spin autocorrelations. Complementary Monte Carlo and exact-diagonalization calculations show that this state is stabilized by a strong enhancement of effective anisotropy: a weak microscopic Cu-Cu exchange anisotropy of approximately 15 percent is generically amplified at the trimer level, producing effective pseudospin-pseudospin interaction anisotropies of 60 to 100 percent. Our results establish trimer-based networks as a promising platform for realizing anisotropy-stabilized quantum entangled states, even in three-dimensional bipartite systems with only weak microscopic anisotropy.

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Melting upon cooling in a quantum magnet

Heating enhances thermal fluctuations and typically leads to melting of solids, but in exceptional cases, heating can also cause liquids to solidify. The paradigm of this counterintuitive phenomenon is solidification of liquid $^3$He upon increasing temperature, known as the Pomeranchuk effect. Here we show that such inverse melting also appears in quantum magnetism. We find that, on cooling, the Ising-like triangular-lattice antiferromagnet erbium heptatantalate first develops a three-sublattice long-range magnetic order -- analogous to a solid -- which then, unexpectedly, melts at even lower temperatures into a short-range correlated spin-stripe state -- analogous to a liquid. We propose that such an unprecedented ``spin Pomeranchuk effect" can generically arise from strong competition between spin-spin interactions in frustrated magnets, and provides a novel avenue to transformations between exotic magnetic phases.

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Incommensurate magnetic order arising from frustrated interchain interactions in the spin-1/2 chain compound AgCuVO$_4$

Quantum spin chains with competing interactions offer a platform where low dimensionality and frustration--both acting to suppress magnetic order--intersect. We studied magnetic ordering in the spin-1/2 chain compound AgCuVO$_4$ using muon spin spectroscopy and neutron diffraction. Long-range magnetic order emerges at $T_N = 2.0(1)$ K, which is $\sim$1/200 of the dominant intrachain coupling $J$ and $\sim$1/15 of the interchain interactions. The collinear incommensurate amplitude-modulated magnetic structure features a reduced ordered moment of 0.13(3) $\mu_\mathrm{B}$, confined to the $ab$ plane and modulated along the $c$ axis--perpendicular to the spin chains--indicating frustrated interchain couplings. The low $T_N$, small moment, and incommensurate order highlight strong frustration, positioning AgCuVO$_4$ as a model system for exploring frustration in quantum spin chains.

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Coexistence of static and dynamic local magnetic fields in an S = 3/2 honeycomb lattice antiferromagnet Co2Te3O8

Two-dimensional honeycomb lattices, characterized by their low coordination numbers, provide a fertile platform for exploring various quantum phenomena due to the intricate interplay between competing magnetic interactions, spin-orbit coupling, and crystal electric fields. Beyond the widely studied Jeff= 1/2 honeycomb systems, S = 3/2 honeycomb lattices present a promising alternative route to realizing the classical spin liquid-like state within the spin-S Kitaev models. Herein, we present crystal structure, thermodynamic, neutron diffraction and muon spin relaxation (muSR) measurements, complemented by density functional theory (DFT) calculations on an unexplored 3d transition metal based compound Co2Te3O8, where Co2+ (S = 3/2) ions form a distorted honeycomb lattice in the crystallographic bc-plane without any anti-side disorder between constituent atoms. A clear lambda type anomaly around 55 K in both magnetic susceptibility and specific heat data indicates the onset of a long-range ordered state below TN= 55 K. The dominant antiferromagnetic interaction between S = 3/2 moments is evidenced by a relatively large negative Curie-Weiss temperature of -103 K derived from magnetic susceptibility data and supported by DFT calculations. The signature of long-range antiferomagnetic order state in the thermodynamic data is corroborated by neutron diffraction and muSR results. Furthermore, muSR experiments reveal the coexistence of static and dynamic local magnetic fields below TN, along with a complex magnetic structure that can be associated with XY-like antiferromagnet, as confirmed by neutron diffraction experiments.

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On the pseudo-doublet ground state of the non-Kramers compound SrTm2O4 and its frustrated antiferromagnetic interactions

Here we present experimental evidence of the pseudo-doublet ground state of the non-Kramers compound SrTm2O4, based on specific heat, magnetic entropy and electron paramagnetic resonance. We demonstrate that the two crystallographic Tm3+ sites give rise to distinct single-ion anisotropies, and by extension, SrTm2O4 hosts two magnetic sublattices. Inelastic neutron scattering reveals low-lying dispersing crystal-field excitations, which we modelled using an effective charge model and mean field random phase approximation. The extracted magnetic exchange interactions are both antiferromagnetic and frustrated for both chains. Interchain magnetic exchange interactions are negligible. The strength of the magnetic exchange interactions in relation to the size of crystal field gaps, together with the frustration and low dimensionality, force the system to remain paramagnetic down to the lowest experimentally reachable temperature despite the pseudo-doublet nature of its ground state.

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Spin-liquid-like spin dynamics in the frustrated antiferromagnet TbBO3

The synergistic interplay between spin correlations, spin-orbit coupling, and competing exchange interactions provides a promising route to realize exotic quantum states with nontrivial excitations in rare-earth based frustrated magnets. Here, by using thermodynamic and local-probe measurements down to 16 mK, we demonstrate the exotic magnetism and spin dynamics in the distorted triangular lattice TbBO3. Thermodynamic experiments reveal the presence of dominant antiferromagnetic exchange and subdominant dipolar interactions. Despite sizable antiferromagnetic exchange interactions between the Tb3+ moments, muon-spin relaxation experiment does not detect any signatures of long-range magnetic order or spin-freezing down to 16 mK, corroborating the specific heat and ac magnetic susceptibility down to 45 mK that suggests a persistent spin dynamics in this frustrated triangular lattice. The scaling of muon relaxation rate as a function of the characteristic energy scale for several spin-liquid candidates, including TbBO3, demonstrates that a common underlying mechanism is at play. The persistent dynamics in this frustrated triangular lattice antiferromagnet is reminiscent of a universal spin-liquid-like spin fluctuations, here attributed to dominant two dimensional (2D) antiferromagnetic short-range spin correlations, confirmed by the presence of a broad magnetic diffuse scattering in the elastic and low-energy inelastic neutron scattering channels at Q ~ 1.03 Ang**$^{-1}$** at low temperatures. Our results demonstrate that non-Kramers ion based triangular lattice hosts spin-liquid-like dynamics of local moments arising from the admixture of excited crystal electric field states into the ground state and intertwining of frustration and spin-orbit interaction.

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Magnetic properties of a spin-orbit entangled Jeff=1/2 three-dimensional frustrated rare-earth hyperkagome

The interplay between competing degrees of freedom can stabilize non-trivial magnetic states in correlated electron materials. Frustration-induced strong quantum fluctuations can evade long-range magnetic ordering leading to exotic quantum states such as spin liquids in two-dimensional spin-lattices such as triangular and kagome structures. However, the experimental realization of dynamic and correlated quantum states is rare in three-dimensional (3D) frustrated magnets wherein quantum fluctuations are less prominent. Herein, we report the crystal structure, magnetic susceptibility, electron spin resonance (ESR) and specific heat studies accompanied by crystal electric field (CEF) calculations on a 3D frustrated magnet Yb3Sc2Ga3O12. In this material, Yb3+ ions form a three-dimensional network of corner-sharing triangles known as hyperkagome lattice without any detectable anti-site disorder. Our results reveal a low energy state with Jeff = 1/2 degrees of freedom in the Kramers doublet state. The zero field-cooled and field cooled magnetic susceptibility taken in 0.001 T rules out the presence of spin-freezing down to 1.8K. The Curie-Weiss (CW) fit to low-T susceptibility data yields a small and negative CW temperature indicating the presence of a weak antiferromagnetic interaction between Jeff = 1/2 (Yb3+) moments. The Yb-ESR displays a broad line of non-Lorentzian shape that suggests considerable magnetic anisotropy in Yb3Sc2Ga3O12. The CEF calculations suggest that the ground state is well separated from the excited states, which are in good agreement with experimental results. The absence of long-range magnetic ordering indicates a dynamic liquid-like ground state at least down to 130 mK. Furthermore, zero field specific heat shows a broad maximum around 200 mK suggesting the presence of short-range spin correlations in this 3D frustrated antiferromagnet.

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Competing magnetic phases in the frustrated spin-1/2 chain compound $β$-TeVO$_4$ probed by NMR

In frustrated spin-1/2 chains the competition between the nearest- and next-nearest-neighbor exchange interactions leads to a rich phase diagram that becomes even richer in the presence of perturbations in their material realizations. These effects are still largely unexplored, so that new insight into static and dynamic magnetism, in particular by sensitive local probes, is highly desired. Here we present a comprehensive $^{17}$O nuclear magnetic resonance study of $β$-TeVO$_4$, where the anisotropy of the main exchange interactions and additional weak interchain exchange interactions complement the theoretical phase diagram. Our results confirm the dynamical nature of the intriguing spin-stripe phase that has been reported in previous studies. In addition, we find that the magnetic order in the high-field phase, which develops just below the magnetization saturation, is consistent with an unusual type of spin-density-wave (SDW) order with different alignments of the magnetic moments on the neighboring chains. This is reminiscent of the ordering in the SDW phase, realized in the absence of the magnetic field, and is thus most likely stabilized by magnetic anisotropy.

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Magnetic properties of triangular lattice antiferromagnets Ba3RB9O18 (R = Yb, Er)

Frustration, spin correlations and interplay between competing degrees of freedom are some of the key ingredients that underlie exotic states with fractional excitations in quantum materials. Rare-earth based two dimensional magnetic lattice wherein crystal electric field, spin-orbit coupling, anisotropy and electron correlation between rare-earth moments offer a new paradigm in this context. Herein, we present crystal structure, magnetic susceptibility and specific heat accompanied by crystal electric field calculations on the polycrystalline sample of Ba3RB9O18 (R = Yb, Er) in which R3+ ions form a perfect triangular lattice without anti-site disorder. The localized R3+ spins show neither long-range order nor spin-glass state down to 1.9 K in Ba3RB9O18. Magnetization data reveal a pseudospin Jeff = 1/2 ( Yb3+) in the Kramers doublet state and a weak antiferromagnetic interaction between Jeff = 1/2 moments in the Yb variant. On the other hand, the effective moment μeff = 8.8 μB was obtained from the Curie-Weiss fit of the low-temperature susceptibility data of Er variant suggests the admixture of higher crystal electric field states with the ground state. The Curie-Weiss fit of low-temperature susceptibility data for Er system unveils the presence of a relatively strong antiferromagnetic interaction between Er3+ moments compared to its Yb3+ analog. Ba3ErB9O18 does not show long-range magnetic ordering down to 500 mK. Furthermore, our crystal electric field calculations based on magnetization data of Ba3ErB9O18 suggest the presence of a small gap between the ground and first excited Kramers doublets. The broad maximum around 4 K in magnetic specific heat in zero-field is attributed to the thermal population of the first CEF excited state in Ba3ErB9O18, which is consistent with our CEF calculations.

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Quantum spin liquid in the Ising triangular-lattice antiferromagnet neodymium heptatantalate

Disordered magnetic states known as spin liquids are of paramount importance in both fundamental and applied science. A classical state of this kind was predicted for the Ising antiferromagnetic triangular model more than half a century ago, while additional non-commuting exchange terms were proposed to induce its quantum version -- a quantum spin liquid. These predictions have not been yet confirmed experimentally. Here we report a discovery of such a state in the structurally perfect triangular-lattice antiferromagnet NdTa$_7$O$_{19}$. Its magnetic ground state is characterized by spin-1/2 degrees of freedom with Ising-like interactions and gives rise to low-frequency spin excitations persisting down to the lowest temperatures. Our study demonstrates the key role of strong spin-orbit coupling in stabilizing spin liquids that result from magnetic anisotropy and highlights the large family of rare-earth (RE) heptatantalates RETa$_7$O$_{19}$ as a novel framework for realization of these states, which represent a promising platform for quantum applications.

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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.

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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.

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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.

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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.

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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.

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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.

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