arXiv subjects

M. Horvatić

Publications and source records attributed to M. Horvatić.

At least 19 recordsLinked to original sources

arXiv2026

Discovery of BKT correlations in the quantum kagome compound Cs$_2$Cu$_3$SnF$_{12}$

We investigate the microscopic properties of the kagome compound Cs$_2$Cu$_3$SnF$_{12}$ using $^{63,65}$Cu nuclear quadrupolar resonance (NQR). Analysis of the local hyperfine fields below the Néel temperature $T_N = 20$ K indicates a spin structure consistent with $P2_1/n$ symmetry of negative vector chirality. Measurements of the spin-lattice relaxation rate $T_1 ^{-1}$ reveal signatures of a gapless ground state and two-dimensional Berezinskii-Kosterlitz-Thouless (BKT)-type correlations above $T_N$, extending over a broad temperature range of approximately 130 K in zero magnetic field. Within the same temperature range, the observed increase in the NQR linewidth is consistent with short-range chiral order recently identified by neutron scattering. Our results establish Cs$_2$Cu$_3$SnF$_{12}$ as a unique quantum kagome system exhibiting BKT behavior.

cond-mat.str-el↗

arXiv2026

Field-induced antiferromagnetic transition in CeIrIn$_5$

We report low-temperature $^{115}$In nuclear magnetic resonance (NMR) study of the prototypical heavy-fermion compound CeIrIn$_5$ in high magnetic fields applied close to the crystallographic $c$ axis. For this orientation, a field-induced transition was previously reported to take place at about 28 T. Although we do not observe any change of the NMR spectrum above the transition, the intensity of the NMR lines drastically decreases as a consequence of a considerable shortening of the $T_2$ relaxation time. In addition, $1/T_1$ shows a pronounced maximum at the transition. Taking into account previous high-field de Haas-van Alphen results in conjunction with band-structure calculations, our NMR results are most naturally explained by the field-induced transition into an antiferromagnetic state with the propagation vector $\mathbf{Q} = (1/2, 1/2, 0)$ and magnetic moments aligned antiferromagnetically along the $c$ axis. This makes CeIrIn$_5$ a unique case where the application of the magnetic field induces an ordered state with moments antiferromagnetically aligned along the field direction.

cond-mat.str-el↗

arXiv2026

Magnetic field-induced phases in a model S=1 Haldane chain system

An $S=1$ Haldane chain is a one-dimensional (1D) quantum magnet where strong fluctuations result in quantum disordered singlet ground state with a gapped excitation spectrum. The gap magnitude is primarily set by the dominant intrachain interaction ($J_\text{1D}$). An applied magnetic field closes the gap at $B_\text{c1}$ and drives the system into a gapless Tomonaga-Luttinger liquid (TLL) regime, followed by, at lower temperatures, a Bose-Einstein condensate (BEC) ground state, persisting up to $B_\text{c2} \propto 4 J_\text{1D}/gμ_B$. Almost all previously studied experimental realizations of such systems were based on transition-metal complexes which typically suffer from intrinsic anisotropies or large $J_\text{1D}$ values, limiting the access to the full theoretical phase diagram. We report a comprehensive study of TLL and BEC phases in the organic Haldane chain system 3,5-bis(N-tert-butylaminoxyl)-3'-nitrobiphenyl (BoNO). The absence of anisotropy and a moderate $J_\text{1D}$ enable exploration of the complete $B-T$ phase diagram. Through $^1$H nuclear magnetic resonance, combined with theoretical analysis, we characterize the TLL properties, map the BEC phase boundary $T_c (B)$, determine the associated critical exponent $ν\approx 0.66$ at $B_\text{c2}$, and demonstrate universal quasiparticle scaling in the quantum-critical regime. These results provide full experimental validation of theoretical predictions for field-induced phases in an $S=1$ Haldane chain, made over two decades ago.

cond-mat.str-el↗

arXiv2024

Narrowly avoided spin-nematic phase in BaCdVO(PO$_4$)$_2$: NMR evidence

We present a $^{31}$P nuclear magnetic resonance (NMR) investigation of BaCdVO(PO$_4$)$_2$ focusing on the nearly saturated regime between $μ_0H_{c1}$ = 4.05 T and $μ_0H_{c2}$ = 6.5 T, which used to be considered a promising candidate for a spin-nematic phase. NMR spectra establish the absence of any dipolar order there, whereas the weak field dependence of the magnetization above $H_{c1}$ is accounted for by Dzyaloshinskii-Moriya interaction terms. The low-energy spin dynamics (fluctuations), measured by the nuclear spin-lattice relaxation rate $T_1^{-1}$, confirms the continuity of this phase and the absence of any low-temperature phase transition. Unexpectedly, the spin dynamics above $H_{c1}$ is largely dominated by two-magnon processes, which is expected above the saturation field of a spin-nematic phase, but not inside. This shows that BaCdVO(PO$_4$)$_2$ is indeed close to a spin-nematic instability; however, this phase is not stabilized. We thus confirm recent theoretical predictions that the spin-nematic phase can be stabilized, at most, in an extremely narrow field range close to saturation or is rather narrowly avoided [Jiang et al., Phys. Rev. Lett. 130, 116701 (2023)].

cond-mat.str-el↗

arXiv2022

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.

cond-mat.str-el↗

arXiv2022

NMR evidence against a spin-nematic nature of the presaturation phase in the frustrated magnet SrZnVO(PO4)2

Using $^{31}$P nuclear magnetic resonance (NMR) we investigate the recently discovered presaturation phase in the highly frustrated two-dimensional spin system SrZnVO(PO$_4$)$_2$ [F. Landolt et al., Phys. Rev. B 104, 224435 (2021)]. Our data provide two pieces of evidence against the presumed spin-nematic character of this phase: i) NMR spectra reveal that it hosts a dipolar spin order and ii) the 1/$T_1$ relaxation rate data recorded above the saturation field can be fitted by the sum of a single-magnon term, exponential in the gap, and a critical second-order term, exponential in the triple gap, leaving no space for a nematic spin dynamics, characterized by a double-gap exponential. We explain the unexpectedly broad validity of the simple fit and the related critical spin dynamics.

cond-mat.str-el↗

arXiv2021

Second order Zeeman interaction and ferroquadrupolar order in TmVO$_4$

TmVO$_{4}$ exhibits ferroquadrupolar order of the Tm 4f electronic orbitals at low temperatures, and is a model system for Ising nematicity that can be tuned continuously to a quantum phase transition via magnetic fields along the $c$-axis. Here we present $^{51}$V nuclear magnetic resonance data in magnetic fields perpendicular to the $c$-axis in a single crystal that has been carefully cut by a plasma focused ion beam to an ellipsoidal shape to minimize the inhomogeneity of the internal demagnetization field. The resulting dramatic increase in spectral resolution enabled us to resolve the anisotropy of the electric field gradient and to measure the magnetic and quadrupolar relaxation channels separately. Perpendicular magnetic fields nominally do not couple to the low energy degrees of freedom, but we find a significant nonlinear contribution for sufficiently large fields that give rise to a rich phase diagram. The in-plane magnetic field can act either as an effective transverse or longitudinal field to the Ising nematic order, depending on the orientation relative to the principle axes of the quadrupole order, and leads to a marked in-plane anisotropy in both relaxation channels. We find that the small in-plane transverse fields initially enhance the ferroquadrupolar ordering temperature but eventually suppress the long-range order. We tentatively ascribe this behavior to the competing effects of field-induced mixing of higher energy crystal field states and the destabilizing effects of field-induced quantum fluctuations.

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

Pre-saturation phase in the frustrated ferro-antiferromagnet Pb$_2$VO(PO$_4$)$_2$

Magnetization, magnetic torque, neutron diffraction and NMR experiments are used to map out the $H$$-$$T$ phase diagram of the prototypical quasi-two-dimensional ferro-antiferromagnet Pb$_2$VO(PO$_4$)$_2$ in magnetic fields up to 27 T. When the field is applied perpendicular to the axis of magnetic anisotropy, a new magnetic state emerges through a discontinuous transition and persists in a narrow field range just below saturation. The measured NMR spectra suggest a complex and possibly incommensurate magnetic order in that regime.

cond-mat.str-el↗

arXiv2018

Detection of a Disorder-Induced Bose-Einstein Condensate in a Quantum Spin Material at High Magnetic Fields

The coupled spin-1 chains material NiCl$_2$-4SC(NH$_2$)$_2$ (DTN) doped with Br impurities is expected to be a perfect candidate for observing many-body localization at high magnetic field: the so-called "Bose glass", a zero-temperature bosonic fluid, compressible, gapless, incoherent, and short-range correlated. Using nuclear magnetic resonance (NMR), we critically address the stability of the Bose glass in doped DTN, and find that it hosts a novel disorder-induced ordered state of matter, where many-body physics leads to an unexpected resurgence of quantum coherence emerging from localized impurity states. An experimental phase diagram of this new "order-from-disorder" phase, established from NMR $T_1^{-1}$ relaxation rate data in the (13 $\pm$ 1)% Br-doped DTN, is found to be in excellent agreement with the theoretical prediction from large-scale quantum Monte Carlo simulations.

cond-mat.str-el↗

arXiv2018

Exotic phases of frustrated antiferromagnet LiCu2O2

7Li NMR spectra were measured in a magnetic field up to 17 T at temperatures 5-30 K on single crystalline LiCu2O2. Earlier reported anomalies on magnetization curves correspond to magnetic field values where we observe changes of the NMR spectral shape. For the interpretation of the field and temperature evolutions of our NMR spectra, the magnetic structures were analyzed in the frame of the phenomenological theoretical approach of the Dzyaloshinskii-Landau theory. A set of possible planar and collinear structures was obtained. Most of these structures have an unusual configuration; they are characterized by a two-component order parameter and their magnetic moments vary harmonically not only in direction, but also in size. From the modeling of the observed spectra, a possible scenario of magnetic structure transformations is obtained.

cond-mat.str-el↗

arXiv2017

Novel Crossover in Coupled Spin Ladders

We report a novel crossover behavior in the long-range-ordered phase of a prototypical spin-$1/2$ Heisenberg antiferromagnetic ladder compound $\mathrm{(C_7H_{10}N)_2CuBr_4}$. The staggered order was previously evidenced from a continuous and symmetric splitting of $^{14}$N NMR spectral lines on lowering temperature below $T_c\simeq 330$ mK, with a saturation towards $\simeq 150$ mK. Unexpectedly, the split lines begin to further separate away below $T^*\sim 100$ mK while the line width and shape remain completely invariable. This crossover behavior is further corroborated by the NMR relaxation rate $T_1^{-1}$ measurements. A very strong suppression reflecting the ordering, $T_1^{-1}\sim T^{5.5}$, observed above $T^*$, is replaced by $T_1^{-1}\sim T$ below $T^*$. These original NMR features are indicative of unconventional nature of the crossover, which may arise from a unique arrangement of the ladders into a spatially anisotropic and frustrated coupling network.

cond-mat.str-el↗

arXiv2016

Observation of electronic bound states in charge-ordered YBa$_2$Cu$_3$O$_y$

Observing how electronic states in solids react to a local symmetry breaking provides insight into their microscopic nature. A striking example is the formation of bound states when quasiparticles are scattered off defects. This is known to occur, under specific circumstances, in some metals and superconductors but not, in general, in the charge-density-wave (CDW) state. Here, we report the unforeseen observation of bound states when a magnetic field quenches superconductivity and induces long-range CDW order in YBa$_2$Cu$_3$O$_y$. Bound states indeed produce an inhomogeneous pattern of the local density of states $N(E_F)$ that leads to a skewed distribution of Knight shifts which is detected here through an asymmetric profile of $^{17}$O NMR lines. We argue that the effect arises most likely from scattering off defects in the CDW state, which provides a novel case of disorder-induced bound states in a condensed-matter system and an insightful window into charge ordering in the cuprates.

cond-mat.supr-con↗

arXiv2016

Dichotomy between Attractive and Repulsive Tomonaga-Luttinger Liquids in Spin Ladders

We present two methods to determine whether the interactions in a Tomonaga-Luttinger liquid (TLL) state of a spin-$1/2$ Heisenberg antiferromagnetic ladder are attractive or repulsive. The first method combines two bulk measurements, of magnetization and specific heat, to deduce the TLL parameter that distinguishes between the attraction and repulsion. The second one is based on a local-probe, NMR measurements of the spin-lattice relaxation. For the strong-leg spin ladder compound $\mathrm{(C_7H_{10}N)_2CuBr_4}$ we find that the isothermal magnetic field dependence of the relaxation rate, $T_1^{-1}(H)$, displays a concave curve between the two critical fields that bound the TLL regime. This is in sharp contrast to the convex curve previously reported for a strong-rung ladder $\mathrm{(C_5H_{12}N)_2CuBr_4}$. Within the TLL description, we show that the concavity directly reflects the attractive interactions, while the convexity reflects the repulsive ones.

cond-mat.str-el↗

arXiv2015

One-Third Magnetization Plateau with a Preceding Novel Phase in Volborthite

We have synthesized high-quality single crystals of volborthite, a seemingly distorted kagome antiferromagnet, and carried out high-field magnetization measurements up to 74 T and 51V NMR measurements up to 30 T. An extremely wide 1/3 magnetization plateau appears above 28 T and continues over 74 T at 1.4 K, which has not been observed in previous study using polycrystalline samples. NMR spectra reveal an incommensurate order (most likely a spin-density wave order) below 22 T and a simple spin structure in the plateau phase. Moreover, a novel intermediate phase is found between 23 and 26 T, where the magnetization varies linearly with magnetic field and the NMR spectra indicate an inhomogeneous distribution of the internal magnetic field. This sequence of phases in volborthite bear a striking similarity to those of frustrated spin chains with a ferromagnetic nearest-neighbor coupling J1 competing with an antiferromagnetic next-nearest-neighbor coupling J2.

cond-mat.str-el↗

arXiv2015

Incipient charge order observed by NMR in the normal state of YBa2Cu3Oy

The pseudogap regime of high-temperature cuprates harbours diverse manifestations of electronic ordering whose exact nature and universality remain debated. Here, we show that the short-ranged charge order recently reported in the normal state of YBa2Cu3Oy corresponds to a truly static modulation of the charge density. We also show that this modulation impacts on most electronic properties, that it appears jointly with intra-unit-cell nematic, but not magnetic, order, and that it exhibits differences with the charge density wave observed at lower temperatures in high magnetic fields. These observations prove mostly universal, they place new constraints on the origin of the charge density wave and they reveal that the charge modulation is pinned by native defects. Similarities with results in layered metals such as NbSe2, in which defects nucleate halos of incipient charge density wave at temperatures above the ordering transition, raise the possibility that order-parameter fluctuations, but no static order, would be observed in the normal state of most cuprates if disorder were absent.

cond-mat.supr-con↗

arXiv2015

Hyperfine coupling and spin polarization in the bulk of the topological insulator Bi$_2$Se$_3$

Nuclear magnetic resonance (NMR) and transport measurements have been performed at high magnetic fields and low temperatures in a series of $n$-type Bi$_{2}$Se$_{3}$ crystals. In low density samples, a complete spin polarization of the electronic system is achieved, as observed from the saturation of the isotropic component of the $^{209}$Bi NMR shift above a certain magnetic field. The corresponding spin splitting, defined in the phenomenological approach of a 3D electron gas with a large (spin-orbit-induced) effective $g$-factor, scales as expected with the Fermi energy independently determined by simultaneous transport measurements. Both the effective electronic $g$-factor and the "contact" hyperfine coupling constant are precisely determined. The magnitude of this latter reveals a non negligible $s$-character of the electronic wave function at the bottom of the conduction band. Our results show that the bulk electronic spin polarization can be directly probed via NMR and pave the way for future NMR investigations of the electronic states in Bi-based topological insulators.

cond-mat.mes-hall↗

arXiv2014

Evidence of Andreev bound states as a hallmark of the FFLO phase in $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$

Superconductivity is a quantum phenomena arising, in its simplest form, from pairing of fermions with opposite spin into a state with zero net momentum. Whether superconductivity can occur in fermionic systems with unequal number of two species distinguished by spin, atomic hyperfine states, flavor, presents an important open question in condensed matter, cold atoms, and quantum chromodynamics, physics. In the former case the imbalance between spin-up and spin-down electrons forming the Cooper pairs is indyced by the magnetic field. Nearly fifty years ago Fulde, Ferrell, Larkin and Ovchinnikov (FFLO) proposed that such imbalanced system can lead to exotic superconductivity in which pairs acquire finite momentum. The finite pair momentum leads to spatially inhomogeneous state consisting of of a periodic alternation of "normal" and "superconducting" regions. Here, we report nuclear magnetic resonance (NMR) measurements providing microscopic evidence for the existence of this new superconducting state through the observation of spin-polarized quasiparticles forming so-called Andreev bound states.

cond-mat.supr-con↗