arXiv subjects

Martin Mourigal

Publications and source records attributed to Martin Mourigal.

At least 19 recordsLinked to original sources

arXiv2026

Revealing Intrinsic Anisotropy of Collective Magnetic Excitations in Twinned Crystals of a Kitaev-Heisenberg Quantum Magnet

Quantum magnets with competing interactions often emerge from delicate balances among microscopic parameters, making it essential to disentangle intrinsic spin dynamics from extrinsic disorder effects. Here, we introduce a multimodal optical approach combining magneto-infrared spectroscopy with domain-resolved micro-Raman spectroscopy at high magnetic fields to reconstruct the intrinsic magnetic excitation spectrum of twinned crystals of the Kitaev-Heisenberg quantum magnet Na$_3$Co$_2$SbO$_6$. Far-infrared spectroscopy reveals multiple field-tunable magnetic excitations, but the intrinsic response is obscured by replica features arising from twin domains. By correlating magneto-infrared and domain-resolved Raman spectra, we isolate the single-domain magnon response and uncover a pronounced twofold in-plane magnon anisotropy. This anisotropy far exceeds that expected from the measured in-plane g-factor anisotropy and is instead dominated by anisotropic bond-dependent exchange interactions. By unifying high-field, high-resolution and spatially selective optical probes, our work establishes a broadly applicable framework for revealing intrinsic spin dynamics and constraining the spin Hamiltonian in multidomain quantum magnets.

cond-mat.mtrl-sci↗

arXiv2026

Spin dynamics of the spin-1 triangular lattice Heisenberg antiferromagnet K$_2$Ni(SeO$_3$)$_2$

Strong quantum fluctuations and unconventional spin dynamics are well established in the spin-1/2 triangular lattice Heisenberg antiferromagnet. However, their survival in the spin-1 case remains an open question. We investigate the spin dynamics of K$_2$Ni(SeO$_3$)$_2$, a nearly ideal spin-1 triangular lattice Heisenberg antiferromagnet, using inelastic neutron scattering. Below the ordering temperature $T_{\rm N}$, we observe coherent one-magnon excitations coexisting with a broad high-energy continuum. Two complementary approaches, a spectrally consistent $1/S$-corrected spin wave theory and a beyond-mean-field Schwinger boson theory, reproduce different facets of the continuum. Neither alone is complete, demonstrating substantial quantum fluctuations survive for $S\!=\!1$ and are reflected primarily in the spectral distribution of the continuum. Above $T_{\rm N}$, the continuum bandwidth is conserved while spectral weight is redistributed as magnons lose spatial coherence. Our results establish K$_2$Ni(SeO$_3$)$_2$ as a model triangular antiferromagnet, identifying bandwidth conservation and the distribution of spectral weight within the continuum as organizing principles to understand the spin dynamics of ordered quantum magnets beyond spin-1/2. Our results highlight the need for controlled calculations of the interacting multi-magnon sector of 2D antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2026

Semiclassical Routes to the $α$-RuCl$_3$ Scattering Continuum via Model Meta$-$Analysis

$α$-RuCl$_3$ is a leading material for proximate Kitaev magnetism. We address the origin of the broad, $Γ$-point centered excitation continuum observed by inelastic neutron scattering at elevated temperatures in this compound. Using stochastic Landau-Lifshitz dynamics augmented with quantum-equivalent corrections, we reproduce the temperature-dependent dynamical spin structure factor across both the correlated and conventional paramagnetic regimes. A meta-analysis of 38 published exchange parameter sets identifies those most consistent with the full temperature evolution. A Bayesian optimization procedure is used to derive parameters that capture the low-energy star-like momentum dependence and the overall bandwidth of the continuum. Rescaling temperatures by the Curie--Weiss scale produces a collapse of spectral measures, demonstrating that the high-$T$ dynamics are governed by correlated paramagnetism below $θ_{\mathrm{CW}}$ rather than by the Kitaev crossover to fractionalized excitations. Complementary 24-site exact diagonalization clarifies finite-size systematics at low temperature and the proximity to zigzag/incommensurate ordering. Beyond $α$-RuCl$_3$, our simulation pipeline provides a reproducible, data-driven framework to infer effective spin models in magnets that exhibit broad continua.

cond-mat.mtrl-sci↗

arXiv2026

Sharp spectroscopic fingerprints of disorder in an incompressible magnetic state

Disorder significantly impacts the electronic properties of conducting quantum materials by inducing electron localization and thus altering the local density of states and electric transport. In insulating quantum magnetic materials, the effects of disorder are less understood and can drastically impact fluctuating spin states like quantum spin liquids. In the absence of transport tools, disorder is typically characterized using chemical methods or by semi-classical modeling of spin dynamics. This requires high magnetic fields that may not always be accessible. Here, we show that magnetization plateaus -- incompressible states found in many quantum magnets -- provide an exquisite platform to uncover small amounts of disorder, regardless of the origin of the plateau. Using optical magneto-spectroscopy on the Ising-Heisenberg triangular-lattice antiferromagnet K$_2$Co(SeO$_3$)$_2$ exhibiting a 1/3 magnetization plateau, we identify sharp spectroscopic lines, the fine structure of which serves as a hallmark signature of disorder. Through analytical and numerical modeling, we show that these fingerprints not only enable us to quantify minute amounts of disorder but also reveal its nature -- as dilute vacancies. Remarkably, this model explains all details of the thermomagnetic response of our system, including the existence of multiple plateaus. Our findings provide a new approach to identifying disorder in quantum magnets.

cond-mat.mtrl-sci↗

arXiv2026

Emulation of quantum correlations by classical dynamics in a spin-1/2 Heisenberg chain

We simulate the dynamical spin structure factor (DSSF) $\mathcal{S}({q},ω)$ of the spin-1/2 Heisenberg antiferromagnetic chain using classical simulations. By employing Landau-Lifshitz Dynamics, we emulate quantum correlations through temperature-dependent corrections, including rescaling of magnetic dipoles and renormalization of exchange interactions. Our results closely match Quantum Monte-Carlo calculations for $k_{\rm B}T/J\!\gtrsim\!1$, extending the applicability of classical dynamics to the challenging case of gapless excitations. At higher temperatures, our simulations comply with general predictions for uncorrelated paramagnetic fluctuations in the infinite temperature limit. Entanglement witnesses derived from the quantum-equivalent DSSF act as sensitive diagnostics for the quantum-to-classical crossover. Their reliability stems from their dependence on spectral features alone, enabling classical dynamics to emulate quantum thresholds without genuine entanglement. This framework also reproduces transverse spin correlations in finite magnetic fields, in agreement with quantum simulations. Together, our results establish quantum-corrected classical dynamics as a scalable and predictive tool for interpreting scattering experiments and exploring quantum correlations in strongly correlated spin systems.

cond-mat.str-el↗

arXiv2025

Magneto-Optical Study of Chiral Magnetic Modes in NiI$_{2}$: Direct Evidence for Kitaev Interactions

Bond-dependent magnetic interactions, particularly those described by the Kitaev model, have emerged as a key pathway toward realizing unconventional magnetic states such as quantum spin liquids and topologically nontrivial excitations, including skyrmions. These interactions frustrate conventional magnetic order and give rise to rich collective behavior that continues to challenge both theory and experiment. While Kitaev physics has been extensively explored in the context of honeycomb magnets, direct evidence for its role in real materials remains scarce. Magnetic van der Waals (vdW) materials have emerged as a versatile platform for exploring low-dimensional electrical, magnetic, and correlated electronic phenomena, and provide a fertile ground for potential applications ranging from spintronics to multiferroic devices and quantum information technologies. Here, we demonstrate, through magneto-transmission, Faraday angle rotation, and magnetic circular dichroism measurements, that the magnetic excitation spectrum of NiI$_2$, a van der Waals multiferroic material, is more accurately captured by a Kitaev-based spin model than by the previously invoked helical spin framework.

cond-mat.str-el↗

arXiv2025

Atomically Modulating Competing Exchange Interactions in Centrosymmetric Skyrmion Hosts GdRu2X2 (X = Si, Ge)

Magnetic skyrmions are topologically protected spin states enabling high-density, low-power spin electronics. Despite growing efforts to find new skyrmion host systems, the microscopic mechanisms leading to skyrmion phase transitions at specific temperatures and magnetic fields remain elusive. Here, we systematically study the isostructural centrosymmetric magnets- GdRu2X2 (X = Si and Ge), and the role of X-p orbitals in modifying magnetic exchange interactions. GdRu2Ge2 single crystals, synthesized by arc melting, exhibit two high-entropy pockets associated with skyrmion phases at 0.9 T < H < 1.2 T and 1.3 T < H < 1.7 T, 2 K < T < 30 K-more accessible condition at lower fields and higher temperatures than that in the Si counterpart. Entropy estimations from heat capacity measurements align with magnetization data, and transport studies confirm a topological Hall effect, highlighting the system's nontrivial spin textures and Berry curvature. Compared to GdRu2Si2, electronic structure and exchange interaction evaluations reveal the more extended Ge-4p orbitals enhance competing exchange interactions in GdRu2Ge2, thereby manifesting the rich skyrmion behavior. This work demonstrates how modifying exchange interactions at the atomic level enables the tunability of topologically nontrivial electronic states while advancing our understanding of skyrmion formation mechanisms for future spintronics.

cond-mat.mtrl-sci↗

arXiv2025

Thermally-induced mimicry of quantum cluster excitations and implications for the magnetic transition in FePSe$_3$

In two dimensional magnets, the interplay of thermal fluctuations and spin anisotropy control the existence of long-range magnetic order. In the van der Waals antiferromagnets FePX$_3$, orbital degeneracy in the $t2g$ levels of the Fe$^{2+}$ ions in octahedral coordination yields strong uniaxial anisotropy, which stabilizes magnetic order up to T$\approx$100 K. Recent inelastic neutron scattering measurements around the magnetic ordering transition have shown the existence of a broad spectrum of magnetic fluctuations with nontrivial momentum dependence, which has been interpreted as evidence for localized entangled cluster excitations. In this paper, we offer an alternative interpretation using classical nonlinear spin dynamics simulations. We present stochastic Landau Lifshitz dynamics simulations that reproduce the neutron scattering measurements of Chen et al. [npj Quantum Mater. 9, 40 (2024)] on FePSe$_3$. These calculations faithfully explain the dynamical structure factor's momentum and energy dependence and point to a classical origin for the excitations observed in neutron spectroscopy and that the order-disorder transition can be understood in terms of thermal fluctuations overcoming the anisotropy energy.

cond-mat.str-el↗

arXiv2025

Kitaev interaction and proximate higher-order skyrmion crystal in the triangular lattice van der Waals antiferromagnet NiI2

Topological spin textures, such as magnetic skyrmions, are a spectacular manifestation of magnetic frustration and anisotropy. Most known skyrmion systems are restricted to a topological charge of one, require an external magnetic field for stabilization, and are only reported in a few materials. Here, we investigate the possibility that the Kitaev anisotropic-exchange interaction stabilizes a higher-order skyrmion crystal in the insulating van der Waals magnet NiI2. We unveil and explain the incommensurate static and dynamic magnetic correlations across three temperature-driven magnetic phases of this compound using neutron scattering measurements, simulations, and modeling. Our parameter optimisation yields a minimal Kitaev-Heisenberg Hamiltonian for NiI2 which reproduces the experimentally observed magnetic excitations. Monte Carlo simulations for this model predict the emergence of the higher-order skyrmion crystal but neutron diffraction and optical experiments in the candidate intermediate temperature regime are inconclusive. We discuss possible deviations from the Kitaev-Heisenberg model that explains our results and conclude that NiI2, in addition to multiferroic properties in the bulk and few-layer limits, is a Kitaev bulk material proximate to the finite temperature higher-order skyrmion crystal phase.

cond-mat.mtrl-sci↗

arXiv2025

Sunny.jl: A Julia Package for Spin Dynamics

Sunny is a Julia package designed to serve the needs of the quantum magnetism community. It supports the specification of a very broad class of spin models and a diverse suite of numerical solvers. These include powerful methods for simulating spin dynamics both in and out of equilibrium. Uniquely, it features a broad generalization of classical and semiclassical approaches to SU(N) coherent states, which is useful for studying systems exhibiting strong spin-orbit coupling or local entanglement effects. Sunny also offers a well-developed framework for calculating the dynamical spin structure factor, enabling direct comparison with scattering experiments. Ease of use is a priority, with tools for symmetry-guided modeling and interactive visualization.

quant-ph↗

arXiv2025

Classical signatures of quenched and thermal disorder in the dynamics of correlated spin systems

Neutron scattering is frequently used to look for evidence of features indicative of quantum-entangled phases of matter such as continua from fractionalisation or quantised excitations. However, the non-specificity of these features and difficulty of both fully quantum treatments and semiclassical models of disorder, make the diagnosis of such states problematic. Here, we demonstrate the feasibility of semiclassical treatments of disordered systems for supercells of $\sim 10,000$ spins. By examining a number of classically disordered models we show the presence of quantised excitations, broad continua and anomalous damping originating from quenched disorder or large classical degeneracies.

cond-mat.str-el↗

arXiv2024

Kernel Polynomial Method for Linear Spin Wave Theory

Calculating dynamical spin correlations is essential for matching model magnetic exchange Hamiltonians to momentum-resolved spectroscopic measurements. A major numerical bottleneck is the diagonalization of the dynamical matrix, especially in systems with large magnetic unit cells, such as those with incommensurate magnetic structures or quenched disorder. In this paper, we demonstrate an efficient scheme based on the kernel polynomial method for calculating dynamical correlations of relevance to inelastic neutron scattering experiments. This method reduces the scaling of numerical cost from cubic to linear in the magnetic unit cell size.

cond-mat.str-el↗

arXiv2024

Monte-Carlo ray-tracing studies of multiplexed prismatic graphite analyzers for the cold-neutron triple-axis spectrometer at the High Flux Isotope Reactor

A modern cold triple-axis spectrometer to study quantum condensed matter systems is planned for the High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory. Here, we describe the conceptual principles and design of a secondary spectrometer using a multiplexed, prismatic analyzer system relying on graphite crystals and inspired by the successful implementation of the Continuous Angle Multiple Energy Analysis (CAMEA) spectrometers at the Paul Scherrer Institute. This project is currently known as MANTA for Multi-analyzer Neutron Triple-Axis. We report Monte-Carlo ray-tracing simulations on a simple but realistic sample scattering kernel to further illustrate the prismatic analyzer concept's workings, calibration, and performance. Then, we introduce a new statistical analysis approach based on the prismatic analyzer concept to improve the number of final energies measured on the spectrometer. We also study possible evolutions in the CAMEA design relevant for MANTA.

physics.ins-det↗

arXiv2024

Noncentrosymmetric Triangular Magnet CaMnTeO$_6$: Strong Quantum Fluctuations and Role of s0 vs. s2 Electronic States in Competing Exchange Interactions

Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, we create a new noncentrosymmetric triangular S = 3/2 magnet CaMnTeO$_6$ based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO$_6$ with an unusually large spin rotation angle of 127 deg.(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) $μ$B, extracted from low-temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 $μ$B. This reduction indicates the presence of strong quantum fluctuations in the half-integer spin S = 3/2 CaMnTeO$_6$ magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO$_6$ (A = Ca, Sr, Pb), we demonstrate how quantum-chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control.

cond-mat.str-el↗

arXiv2024

Cryogenic platform to investigate strong microwave cavity-spin coupling in correlated magnetic materials

We present a comprehensive exploration of loop-gap resonators (LGRs) for electron spin resonance (ESR) studies, enabling investigations into the hybridization of solid-state magnetic materials with microwave polariton modes. The experimental setup, implemented in a Physical Property Measurement System by Quantum Design, allows for ESR spectra at temperatures as low as 2 Kelvin. The versatility of continuous wave ESR spectroscopy is demonstrated through experiments on CuSO4.5H2O and MgCr2O4, showcasing the g-tensor and magnetic susceptibilities of these materials. The study delves into the challenges of fitting spectra under strong hybridization conditions and underscores the significance of proper calibration and stabilization. The detailed guide provided serves as a valuable resource for laboratories interested in exploring hybrid quantum systems through microwave resonators.

cond-mat.str-el↗

arXiv2023

Bond-dependent anisotropy and magnon decay in cobalt-based Kitaev triangular antiferromagnet

The Kitaev model, a honeycomb network of spins with bond-dependent anisotropic interactions, is a rare example of having a quantum spin liquid ground state. Although most Kitaev model candidate materials eventually order magnetically due to inevitable non-Kitaev terms, their bond-dependent anisotropy manifests in unusual spin dynamics. It has recently been suggested that bond-dependent anisotropy can stabilise novel magnetic phases and exotic spin dynamics on the geometrically frustrated triangular lattice. However, few materials have been identified with simultaneous geometric frustration and bond-dependent anisotropy. Here, we report a frustrated triangular lattice with bond-dependent anisotropy in the cobalt-based triangular van der Waals antiferromagnet CoI2. Its momentum and energy-resolved spin dynamics exhibit substantial magnon breakdown and complex level repulsion, as measured by inelastic neutron scattering. A thorough examination of excitations in both the paramagnetic and magnetically ordered states reveals that the bond-dependent anisotropy is the origin of the spiral order and the magnon breakdown found in CoI2. Our result paves the way toward a new research direction for the Kitaev model with geometrical frustration.

cond-mat.str-el↗

arXiv2023

Instabilities of heavy magnons in an anisotropic magnet

The search for new elementary particles is one of the most basic pursuits in physics, spanning from subatomic physics to quantum materials. Magnons are the ubiquitous elementary quasiparticle to describe the excitations of fully-ordered magnetic systems. But other possibilities exist, including fractional and multipolar excitations. Here, we demonstrate that strong quantum interactions exist between three flavors of elementary quasiparticles in the uniaxial spin-one magnet FeI2. Using neutron scattering in an applied magnetic field, we observe spontaneous decay between conventional and heavy magnons and the recombination of these quasiparticles into a super-heavy bound-state. Akin to other contemporary problems in quantum materials, the microscopic origin for new physics in FeI2 is the quasi-flat nature of excitation bands and the presence of Kitaev anisotropic magnetic exchange interactions.

cond-mat.str-el↗

arXiv2022

Chemical Design of Electronic and Magnetic Energy Scales in Tetravalent Praseodymium

Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the 4+ oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr4+ oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f1 configuration with ligand valence electrons, analogous to transition metals. The resulting competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr4+, which departs from the Jeff =1/2 limit and resembles that of high-valent actinides. Our results show that Pr4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials.

cond-mat.mtrl-sci↗