arXiv subjects

Mladen Horvatić

Publications and source records attributed to Mladen Horvatić.

17 recordsLinked to original sources

arXiv2026

Pinwheel-shaped bound triplet pairs in the magnetization plateaus of SrCu$_2$(BO$_3$)$_2$

The sequence of magnetization plateaus at 1/8, 2/15, 1/6, 1/4, 1/3, 2/5, and 1/2 of the saturation observed in SrCu$_2$(BO$_3$)$_2$ remained a puzzle until tensor-networks-based numerical simulations suggested that the low-magnetization plateaus are stabilized as Wigner crystals of spin-2 bound states, and not as one of the standard configurations (semiclassical up-down, or crystals of triplets). We report on $^{63,65}$Cu nuclear magnetic resonance spectra up to 41.9 T: Based on constraints deduced from the 1/3 plateau, we show that the spectra in the 1/8 and 2/15 plateaus indeed agree with the prediction for the spin-2 bound states, while being incompatible with a crystal of triplets. This adds the formation of Wigner crystals of bound states as an alternative fundamental paradigm in the theory of magnetization plateaus.

cond-mat.str-el↗

arXiv2026

Critical Berezinskii-Kosterlitz-Thouless dynamics in the archetypal two-dimensional spin system Ba$_2$CuSi$_2$O$_6$Cl$_2$

We study the spin dynamics in the quasi-2D spin-$1/2$ dimer compound Ba$_2$CuSi$_2$O$_6$Cl$_2$, which exhibits a magnetic field-induced Bose-Einstein condensate (BEC) of triplons. Using nuclear magnetic resonance spin-lattice relaxation rate ($T_1^{-1}$) measurements combined with large-scale quantum Monte Carlo (QMC) simulations, we investigate critical fluctuations across the field-temperature phase diagram. Bridging the behavior observed in 1D and 3D systems, the $T_1^{-1}$ relaxation rate shows a pronounced peak extending well above the Néel temperature $T_N$, indicating strong two-dimensional Berezinskii-Kosterlitz-Thouless (BKT)-type fluctuations. A quantitative match between experimental and theoretical BEC phase boundaries validates an effective XXZ model. The study determines the intrinsic BKT transition temperature $T_{\mathrm{BKT}}$ from QMC, revealing a nearly field-independent $T_{\mathrm{BKT}}/T_N \approx 0.74$. Scaling analysis of the relaxation rate shows critical exponents consistent with 2D universality, and a narrow temperature window is identified where 2D physics dominates. These findings establish Ba$_2$CuSi$_2$O$_6$Cl$_2$ as a model system for exploring BKT dynamics in quantum magnets.

cond-mat.str-el↗

arXiv2026

Gapped 1/9 Magnetization Plateau in the Anisotropic Kagome Antiferromagnet Y-kapellasite

Fractional magnetization plateaus provide a sensitive probe of many-body spin states in frustrated quantum magnets, yet their microscopic origin in kagome antiferromagnets remains unresolved. This is particularly true of the mysterious $1/9$ plateau, which is predicted by theory but infrequently observed in experiment. Here, we investigate this problem in the $S = 1/2$ anisotropic kagome antiferromagnet Y-kapellasite, Y$_3$Cu$_9$(OH)$_{19}$Cl$_8$, using pulsed-field magnetization measurements on single crystals and high-field $^{35}$Cl NMR. We identify a hierarchy of field-induced fractional features, including $1/3$ and $1/9$ plateaus, as well as a weaker low-field feature. Analysis of the NMR spectra and the magnetic susceptibility across the $1/9$ plateau demonstrate that it is accompanied by an ordered local spin configuration, a strong suppression of low-energy spin fluctuations and activated behavior, consistent with a gapped fractional state. These features differ from those in the only other material YCu$_3$(OH)$_6$Br$_2$[Br$_{1-y}$(OH)$_y$] in which this plateau is observed, implying a surprising robustness of the $1/9$ state to the details of the underlying magnetism.

cond-mat.str-el↗

arXiv2024

Properties of an organic model $S=1$ Haldane chain system

We present the properties of a new organic $S=1$ antiferromagnetic chain system $m$-NO$_2$PhBNO (abbreviated BoNO). In this biradical system two unpaired electrons from aminoxyl groups are strongly ferromagnetically coupled ($|J_\text{FM}| /k_B \gtrsim 500$ K) which leads to the formation of an effective $S=1$ state for each molecule. The chains of BoNO biradicals propagate along the crystallographic $a$ axis. Temperature dependence of the $g$ factor and electron paramagnetic resonance (EPR) linewidth are consistent with a low-dimensional system with antiferromagnetic interactions. The EPR data further suggest that BoNO is the first known Haldane system with an almost isotropic $g$ factor ($2.0023 \pm 2 \unicode{x2030}$). The magnetization measurements in magnetic fields up to $40$ T and low-field susceptibility, together with $^1$H nuclear magnetic resonance (NMR) spectra, reveal a dominant intrachain antiferromagnetic exchange coupling of $J_\text{1D}/k_B = (11.3\pm0.1)$ K, and attainable critical magnetic fields of $μ_0 H_\text{c1} \approx 2$ T and $μ_0 H_\text{c2} \approx 33$ T. These measurements therefore suggest that BoNO is a unique Haldane system with extremely small magnetic anisotropy. Present results are crucial for a future in-depth NMR study of the low-temperature Tomonaga-Luttinger liquid (TLL) and magnetic field-induced phases, which can be performed in the entire phase space.

cond-mat.str-el↗

arXiv2023

Longitudinal spin fluctuations driving field-reinforced superconductivity in UTe$_2$

Our measurements of $^{125}$Te NMR relaxations reveal an enhancement of electronic spin fluctuations above $μ_0H^*\sim15$ T, leading to their divergence in the vicinity of the metamagnetic transition at $μ_0H_m\approx35$ T, below which field-reinforced superconductivity appears when a magnetic field ($H$) is applied along the crystallographic $b$ axis. The NMR data evidence that these fluctuations are dominantly longitudinal, providing a key to understanding the peculiar superconducting phase diagram in $H\|b$, where such fluctuations enhance the pairing interactions.

cond-mat.supr-con↗

arXiv2021

Revealing three-dimensional quantum criticality by Sr-substitution in Han Purple

Classical and quantum phase transitions (QPTs), with their accompanying concepts of criticality and universality, are a cornerstone of statistical thermodynamics. An exemplary controlled QPT is the field-induced magnetic ordering of a gapped quantum magnet. Although numerous "quasi-one-dimensional" coupled spin-chain and -ladder materials are known whose ordering transition is three-dimensional (3D), quasi-2D systems are special for several physical reasons. Motivated by the ancient pigment Han Purple (BaCuSi$_{2}$O$_{6}$), a quasi-2D material displaying anomalous critical properties, we present a complete analysis of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$. We measure the zero-field magnetic excitations by neutron spectroscopy and deduce the magnetic Hamiltonian. We probe the field-induced transition by combining magnetization, specific-heat, torque and magnetocalorimetric measurements with low-temperature nuclear magnetic resonance studies near the QPT. By a Bayesian statistical analysis and large-scale Quantum Monte Carlo simulations, we demonstrate unambiguously that observable 3D quantum critical scaling is restored by the structural simplification arising from light Sr-substitution in Han Purple.

cond-mat.str-el↗

arXiv2020

Direct determination of the Tomonaga-Luttinger parameter $K$ in quasi-one-dimensional spin systems

We test the analytical formula for the enhancement of the nuclear magnetic resonance rate $T_1^{-1}$ by the critical spin fluctuations, over the simple power-law dependence predicted for a purely one-dimensional spin system, recently derived in the random phase approximation [M. Dupont et al., Phys. Rev. B 98, 094403 (2018)]. This prediction is experimentally confirmed by excellent fits to the published temperature dependence of $T_1^{-1}$ data in the two representative spin compounds, (C$_7$H$_{10}$N)$_2$CuBr$_4$ (DIMPY) and BaCo$_2$V$_2$O$_8$, providing at the same time a direct and convenient experimental determination of the Tomonaga-Luttinger-liquid parameter $K$, very well in agreement with theoretical predictions.

cond-mat.str-el↗

arXiv2020

$^{105}$Pd NMR and NQR study of the cubic heavy fermion system Ce$_3$Pd$_{20}$Si$_6$

We report $^{105}$Pd NMR and NQR measurements on a single crystal of Ce$_3$Pd$_{20}$Si$_6$, where antiferroquadrupolar and antiferromagnetic orders develop at low temperature. From the analysis of NQR and NMR spectra, we have determined the electric field gradient (EFG) tensors and the anisotropic Knight shift ($K$) components for both inequivalent Pd sites - Pd($32f$) and Pd($48h$). The observed EFG values are in excellent agreement with our state-of-the-art DFT calculations. The principal values of the quadrupolar coupling are $(20.37 \pm 0.02)$ MHz and $(5.45 \pm 0.02)$ MHz, for the Pd($32f$) and Pd($48h$) site, respectively, which is large compared to the Larmor frequency defined by the gyromagnetic constant $γ= 1.94838$ MHz/T for $^{105}$Pd. Therefore, the complete knowledge of $K$ and the EFG tensors is crucial to establish the correspondence between NMR spectra and crystallographic sites, which is needed for a complete analysis of the magnetic structure, static spin susceptibility, and the spin-lattice relaxation rate data and a better understanding of the groundstate of Ce$_3$Pd$_{20}$Si$_6$.

cond-mat.str-el↗

arXiv2019

Dynamics and field-induced order in the layered spin $S=1/2$ dimer system (C$_5$H$_6$N$_2$F)$_2$CuCl$_4$

The quasi-two-dimensional Heisenberg spin $S=1/2$ dimer system bis(2-amino-5-fluoro-pyridinium) tetrachlorocuprate(II) is studied by means of inelastic neutron scattering, calorimetry and nuclear magnetic resonance (NMR) experiments. In the absence of an applied magnetic field we find dispersive triplet excitations with a spin gap of $Δ=1.112(15)$ meV and a bandwidth of $0.715(15)$ meV within the layers and $0.116(15)$ meV between the layers, respectively. In an applied magnetic field of $μ_0H_c\approx 8.5$ T the spin gap is closed and we find a field induced antiferromagnetically ordered phase.

cond-mat.str-el↗

arXiv2017

Nuclear Magnetic Resonance in High Magnetic Field: Application to Condensed Matter Physics

In this review, we describe the potentialities offered by the nuclear magnetic resonance (NMR) technique to explore at a microscopic level new quantum states of condensed matter induced by high magnetic fields. We focus on experiments realised in resistive (up to 34~T) or hybrid (up to 45~T) magnets, which open a large access to these quantum phase transitions. After an introduction on NMR observable, we consider several topics: quantum spin systems (spin-Peierls transition, spin ladders, spin nematic phases, magnetisation plateaus and Bose-Einstein condensation of triplet excitations), the field-induced charge density wave (CDW) in high $T_c$~superconductors, and exotic superconductivity including the Fulde-Ferrel-Larkin-Ovchinnikov superconducting state and the field-induced superconductivity due to the Jaccarino-Peter mechanism.

cond-mat.str-el↗

arXiv2017

Dynamics of Bound Magnon Pairs in the Quasi-One-Dimensional Frustrated Magnet LiCuVO_4

We report on the dynamics of the spin-1/2 quasi-one-dimensional frustrated magnet LiCuVO$\mathrm{_4}$ measured by nuclear spin relaxation in high magnetic fields 10--34 T, in which the ground state has spin-density-wave order. The spin fluctuations in the paramagnetic phase exhibit striking anisotropy with respect to the magnetic field. The transverse excitation spectrum probed by $^{51}$V nuclei has an excitation gap, which increases with field. On the other hand, the gapless longitudinal fluctuations sensed by $^7$Li nuclei grow with lowering temperature, but tend to be suppressed with increasing field. Such anisotropic spin dynamics and its field dependence agree with the theoretical predictions and are ascribed to the formation of bound magnon pairs, a remarkable consequence of the frustration between ferromagnetic nearest neighbor and antiferromagnetic next-nearest-neighbor interactions.

cond-mat.str-el↗

arXiv2017

Competing Bose-Glass physics with disorder-induced Bose-Einstein condensation in the doped $S=1$ antiferromagnet Ni(Cl$_{1-x}$Br$_x$)$_2$-4SC(NH$_2$)$_2$ at high magnetic fields

We study the interplay between disorder and interactions for emergent bosonic degrees of freedom induced by an external magnetic field in the Br-doped spin-gapped antiferromagnetic material Ni(Cl$_{1-x}$Br$_x$)$_2$-4SC(NH$_2$)$_2$ (DTNX). Building on nuclear magnetic resonance experiments at high magnetic field [A. Orlova et al., Phys. Rev. Lett. 118, 067203 (2017)], we describe the localization of isolated impurity states, providing a realistic theoretical modeling for DTNX. Going beyond single impurity localization we use quantum Monte Carlo simulations to explore many-body effects from which pairwise effective interactions lead to a (impurity-induced) BEC revival [M. Dupont, S. Capponi, and N. Laflorencie, Phys. Rev. Lett. 118, 067204 (2017)]. We further address the question of the existence of a many-body localized Bose-glass (BG) phase in DTNX, which is found to compete with a series of a new kind of BEC regimes made out of the multi-impurity states. The global magnetic field-temperature phase diagram of DTNX reveals a very rich structure for low impurity concentration, with consecutive disorder-induced BEC mini-domes separated by intervening many-body localized BG regimes. Upon increasing the impurity level, multiple mini-BEC phases start to overlap, while intermediate BG regions vanish.

cond-mat.str-el↗

arXiv2017

Nuclear magnetic resonance signature of the spin-nematic phase in LiCuVO$_{4}$ at high magnetic fields

We report a 51V nuclear magnetic resonance investigation of the frustrated spin-1/2 chain compound LiCuVO4, performed in pulsed magnetic fields and focused on high-field phases up to 55 T. For the crystal orientations H // c and H // b we find a narrow field region just below the magnetic saturation where the local magnetization remains uniform and homogeneous, while its value is field dependent. This behavior is the first microscopic signature of the spin-nematic state, breaking spin-rotation symmetry without generating any transverse dipolar order, and is consistent with theoretical predictions for the LiCuVO4 compound.

cond-mat.str-el↗

arXiv2017

Nuclear Magnetic Resonance Reveals Disordered Level-Crossing Physics in the Bose-Glass Regime of the Br-doped Ni(Cl$_{1-x}$Br$_x$)$_2$-4SC(NH$_2$)$_2$ Compound at a High Magnetic Field

By measuring the nuclear magnetic resonance (NMR) 1/T_1 relaxation rate in the Br (bond) doped DTN compound, Ni(Cl(1-x)Br_x)2-4SC(NH2)2 (DTNX), we show that the low-energy spin dynamics of its high magnetic field "Bose-glass" regime is dominated by a strong peak of spin fluctuations found at the nearly doping-independent position H* = 13.6 T. From its temperature and field dependence we conclude that this corresponds to a level crossing of the energy levels related to the doping-induced impurity states. Observation of the local NMR signal from the spin adjacent to the doped Br allowed us to fully characterize this impurity state. We have thus quantified a microscopic theoretical model that paves the way to better understanding of the Bose-glass physics in DTNX, as revealed in the related theoretical study [M. Dupont, S. Capponi, and N. Laflorencie, Phys. Rev. Lett. 118, 067204 (2017), arXiv:1610.05136].

cond-mat.str-el↗

arXiv2017

Nuclear magnetic resonance study of the magnetic-field-induced ordered phase in the NiCl2-4SC(NH2)2 compound

Nuclear magnetic resonance (NMR) study of the high magnetic field (H) part of the Bose-Einstein condensed (BEC) phase of the quasi-onedimensional (quasi-1D) antiferromagnetic quantum spin-chain compound NiCl2-4SC(NH2)2 (DTN) was performed. We precisely determined the phase boundary, Tc(H), down to 40 mK; the critical boson density, n_c(Tc); and the absolute value of the BEC order parameter S_perp at very low temperature (T = 0.12 K). All results are accurately reproduced by numerical quantum Monte Carlo simulations of a realistic three-dimensional (3D) model Hamiltonian. Approximate analytical predictions based on the 1D Tomonaga-Luttinger liquid description are found to be precise for Tc(H), but less so for S_perp(H), which is more sensitive to the strength of 3D couplings, in particular close to the critical field. A mean-field treatment, based on the Hartree-Fock-Popov description, is found to be valid only up to n_c = 4% (T < 0.3 K), while for higher n_c boson interactions appear to modify the density of states.

cond-mat.str-el↗

arXiv2015

Emergence of Orbital Nematicity in the Tetragonal Phase of BaFe$_2$(As$_{1-x}$P$_x$)$_2$

We report on $^{75}$As-NMR measurements in single crystalline BaFe$_{2}$(As$_{0.96}$P$_{0.04}$)$_{2}$ for magnetic fields parallel to the orthorhombic $[110]_{\rm o}$ and $[100]_{\rm o}$ directions above the structural transition temperature $T_{\rm S}\simeq121$ K. A large difference in the linewidth between the two field directions reveals in-plane anisotropy of the electric field gradient, even in the tetragonal phase. This provides microscopic evidence of population imbalance between As-$4p_{x}$ and $4p_{y}$ orbitals, which reaches $|n_x-n_y|/|n_x+n_y| \sim 15$\% at $T\rightarrow T_{\rm S}$ and is a natural consequence of the orbital ordering of Fe-3$d_{xz}$ and $d_{yz}$ electrons. Surprisingly, this orbital polarization is found to be already static near room temperature, suggesting that it arises from the pinning of anisotropic orbital fluctuations by disorder. The effect is found to be stronger below $\sim 160$ K, which coincides with the appearance of nematicity in previous torque and photoemission measurements. These results impose strong constraints on microscopic models of the nematic state.

cond-mat.str-el↗

arXiv2013

Incomplete devil's staircase in the magnetization curve of SrCu2(BO3)2

We report on NMR and torque measurements on the frustrated quasi-two-dimensional spin-dimer system SrCu2(BO3)2 in magnetic fields up to 34 T that reveal a sequence of magnetization plateaus at 1/8, 2/15, 1/6, and 1/4 of the saturation and two incommensurate phases below and above the 1/6 plateau. The magnetic structures determined by NMR involve a stripe order of triplets in all plateaus, suggesting that the incommensurate phases originate from proliferation of domain walls. We propose that the magnetization process of SrCu2(BO3)2 is best described as an incomplete devil's staircase.

cond-mat.str-el↗