arXiv subjects

B. Normand

Publications and source records attributed to B. Normand.

At least 19 recordsLinked to original sources

arXiv2026

Optimized Tensor-Network Renormalization for Quantum Dynamics: Resolving the Spectral Function of $\mathrm{K_2Co(SeO_3)_2}$

Tensor-network methods have opened a powerful route for the study of dynamical spectral functions in two-dimensional quantum systems. However, existing approaches within the framework of infinite projected entangled-pair states construct the required renormalization tensors solely from the ground-state environment and can suffer from severe numerical instability. We identify the origin of this instability and introduce an excitation-tailored corner-transfer-matrix renormalization-group (ET-CTMRG) method to resolve it. By incorporating excitation tensors into the renormalization procedure, the method constructs a substantially more accurate effective Hamiltonian matrix and thereby yields reliable and well-converged excitation spectra. For Heisenberg antiferromagnets, it reduces truncation errors by orders of magnitude and for the particularly complex case of the supersolid phase in the triangular-lattice XXZ magnet $\mathrm{K_2Co(SeO_3)_2}$, it achieves excellent quantitative agreement with inelastic neutron-scattering measurements. ET-CTMRG therefore provides a robust framework for investigating the dynamical properties of strongly correlated quantum systems.

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arXiv2026

Field-induced quasi-bound state within the two-magnon continuum of a square-lattice Heisenberg antiferromagnet

Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF$_2$(D$_2$O)$_2$(pyz), we investigate the field-dependent spin dynamics of the $S = 1/2$ square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive ``shadow mode'' residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent $1/S$ spin-wave theory to deduce that the ``Larmor-shadow mode'' is a composite two-magnon resonance: a dispersing magnon at wavevector ${\bf Q}$ couples to the uniform Larmor precession at $\Gamma$, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field $(\pi,0)$ anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.

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arXiv2025

Dynamical Spectral Function of the Kagome Quantum Spin Liquid

Quantum spin liquids (QSLs) host exotic fractionalized magnetic and gauge-field excitations whose microscopic origins and experimental verification remain frustratingly elusive. In the absence of static magnetic order, the spin excitation spectrum constitutes the crucial probe of QSL behavior, but its theoretical computation is a serious challenge. Here we employ state-of-the-art tensor-network methods to obtain the full dynamical spectral function of the $J_1$-$J_2$ kagome Heisenberg model and benchmark our results by tracking their evolution across the magnetically ordered and QSL phases. Reducing $|J_2|/J_1$ causes increasingly strong spin-wave renormalization, flattening these modes then merging them into a continuum characteristic of deconfined spinons at all finite energies in the QSL. The low-energy continuum and the occurrence of gap closure at multiple high-symmetry points identify this gapless QSL as the U(1) Dirac spin liquid. These results establish a unified understanding of spin excitations in highly frustrated quantum magnets and provide clear spectral fingerprints for experimental detection in candidate kagome QSL materials.

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arXiv2025

Magnetic and phononic dynamics in the two-ladder quantum magnet (C5H9NH3)2CuBr4

In quantum magnetic materials it is common to observe both static and dynamic lattice effects on the magnetic excitation spectrum. Less common is to find that the magnetic correlations have a significant impact on the phonon spectrum. Can such an interplay occur in a structurally soft system with comparable elastic and magnetic energy scales? Here we study the metal-organic material (C5H9NH3)2CuBr4 (Cu-CPA), in which an explanation of the low-lying excitations depends crucially on a full understanding of both the spin and lattice subsystems. We report high-resolution neutron spectroscopy enabled by large, deuterated single-crystals that reveal how both sectors are affected by the recently discovered structural phase transition. By measuring over several Brillouin zones, we disentangle the vibrational contribution to the spectrum in order to obtain an accurate estimate of the quasi-one-dimensional magnetic signal. The low-energy magnetic excitations are dominated by two gaps, $\Delta$ b = 0.41 meV and $\Delta$ a = 0.55 meV, which contribute with equal intensity ratios, confirming that Cu-CPA realizes a two-ladder spin Hamiltonian, and we deduce the magnetic interaction parameters of both ladders. The phonon spectrum contains a highly localized mode at an anomalously low-energy around 2 meV. This characteristic frequency drops by approximately 5 percent as magnetic correlations become established with decreasing temperature, and we connect this behavior with the location and structure of the cyclopentylammonium rings.

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arXiv2025

Phonon spectrum in the spin-Peierls phase of CuGeO$_3$

CuGeO$_3$ has long been studied as a prototypical example of the spin-Peierls transition in a $S = 1/2$ Heisenberg chain. Despite intensive investigation of this quasi-one-dimensional material, systematic measurements and calculations of the phonon excitations in the dimerized phase have not to date been possible, leaving certain aspects of the spin-Peierls phenomenon unresolved. We perform state-of-the-art density functional theory (DFT) calculations to compute the electronic structure and phonon dynamics in the low-temperature dimerized phase. We also perform high-resolution neutron spectroscopy to measure the full phonon spectrum over multiple Brillouin zones. We find excellent agreement between our numerical and experimental results that extend to all measurement temperatures. Notable features of our phonon spectra include a number of steeply dispersive modes, nonmonotonic dispersion features, and specific phonon anticrossings, which we relate to the mode eigenvectors. By calculating the magnetic interactions within DFT and studying the effects of different phonon modes on the superexchange paths, we discuss the possibility of observing spin-phonon hybridization effects in experiments performed both in and out of equilibrium.

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arXiv2025

Pulsed Magnetophononics in Gapped Quantum Magnets

One route to the control of quantum magnetism at ultrafast timescales is magnetophononics, the modulation of magnetic interactions by coherently driven lattice excitations. Theoretical studies of a gapped quantum magnet subject to continuous, single-frequency driving of one strongly coupled phonon mode find intriguing phenomena including mutually repelling phonon-bitriplon excitations and global renormalization of the spin excitation spectrum. Because experiments are performed with ultrashort pulses that contain a wide range of driving frequencies, we investigate phonon-bitriplon physics under pulsed laser driving. We use the equations of motion to compute the transient response of the driven and dissipative spin-phonon system, which we characterize using the phonon displacement, phonon number, and triplon occupations. In the Fourier transforms of each quantity we discover a low-frequency energetic oscillation between the lattice and spin sectors, which is an intrinsically nonequilibrium collective mode, and demonstrate its origin as a beating between mutually repelling composite excitations. We introduce a phonon-bitriplon approximation that captures all the physics of hybridization, collective mode formation, and difference-frequency excitation, and show that sum-frequency phenomena also leave clear signatures in the repsonse. We model the appearance of such magnetophononic phenomena in the strongly-coupled spin-chain compound CuGeO$_3$, whose overlapping phonon and spin excitation spectra are well characterized, to deduce the criteria for their possible observation in quantum magnetic materials.

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arXiv2025

Confined and deconfined spinon excitations in the rectangular-lattice quantum antiferromagnet

Fractionalization remains one of the most fascinating manifestations of strong interactions in quantum many-body systems. In quantum magnetism, the existence of spinons -- collective magnetic excitations that behave as quasiparticles with fractional quantum numbers -- is proven in spin chains, but the criteria for their appearance in higher dimensions remain disputed. Motivated by experiments reporting the observation of spinons at high energies in the square-lattice Heisenberg antiferromagnet, we adopt the approach of extrapolating from where spinons are well defined. We study the dynamical properties of a Gutzwiller-projected wave function, the staggered-flux state, on a rectangular spin-1/2 Heisenberg lattice as a function of the spatial coupling ratio, $\gamma = J_y/J_x$. By studying the spectrum and the spinon separation distribution we show how, as the system evolves from one-dimensional (1D) towards 2D, the spinons become progressively more confined over most of reciprocal space, but remain deconfined at specific wave vectors.

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arXiv2024

Field-Induced Magnon Decay, Magnon Shadows, and Roton-like Excitations in the Honeycomb Antiferromagnet YbBr$_3$

Although the search for quantum many-body phenomena in magnetic materials has a strong focus on highly frustrated systems, even unfrustrated quantum magnets show a multitude of unconventional phenomena in their spin excitation spectra. YbBr$_3$ is an excellent realization of the $S = 1/2$ antiferromagnetic Heisenberg model on the honeycomb lattice, and we have performed detailed spectroscopic experiments with both unpolarized and polarized neutrons at all applied magnetic fields up to saturation. We observe extensive excitation continua, which cause strong renormalization and the decay of single magnons at higher fields, while coherent features include field-induced ``shadows'' of the single magnons and the spectacular emergence of a roton-like excitation. To guide and interpret our experiments, we performed systematic calculations by the method of cylinder matrix-product states that provide quantitative agreement with the neutron scattering data and a qualitative benchmark for the spectral signatures of strong quantum fluctuations even in the absence of magnetic frustration.

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arXiv2024

Multinode quantum spin liquids in extended Kitaev honeycomb models: the view from variational Monte Carlo

We discuss the discovery by variational Monte Carlo (VMC) methods of a series of multinode quantum spin liquids (QSLs) in extended Kitaev models on the honeycomb lattice. Like the gapless Kitaev spin liquid with its two nodes at K and K$^\prime$, these multinode QSLs are characterized by an emergent Z$_2$ gauge structure and a discrete number of symmetry-protected Majorana cones in their low-energy excitation spectrum. Because the cones are gapped by weak magnetic fields, nonzero Chern numbers are obtained and the ground state becomes one of many possible Abelian or non-Abelian chiral spin liquids. Here we focus on the projective symmetry group (PSG)-guided VMC approach to the Kitaev model with various symmetry-allowed extended interactions. Based on the VMC phase diagrams of these models, we propose a framework for the classification of nodal QSLs that includes the PSG, the chiralities of the cones, and the way in which the cones are symmetry-related. At present, the known candidate Kitaev materials seem to lie outside the parameter regimes of the multinode QSL phases. However, with more than 100 Z$_2$ PSGs for spin-orbit-coupled states on the honeycomb lattice, we anticipate that more than one multinode QSL will be realized experimentally in future work.

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arXiv2024

Spin waves and three-dimensionality in the high-pressure antiferromagnetic phase of SrCu$_2$(BO$_3$)$_2$

Quantum magnetic materials can provide explicit realizations of paradigm models in quantum many-body physics. In this context, SrCu$_2$(BO$_3$)$_2$ is a faithful realization of the Shastry-Sutherland model (SSM) for ideally frustrated spin dimers, even displaying several of its quantum magnetic phases as a function of pressure. We perform inelastic neutron scattering (INS) measurements on SrCu$_2$(BO$_3$)$_2$ at 5.5 GPa and 4.5 K, observing spin waves that characterize the high-pressure antiferromagnetic phase. The experimental spectra are well described by linear spin-wave calculations on a SSM with an inter-layer interaction, which is determined accurately as $J_c = 0.053(3)$ meV. The presence of $J_c$ indicates the need to account for the three-dimensional nature of SrCu$_2$(BO$_3$)$_2$ in theoretical models, also at lower pressures. We find that the ratio between in-plane interactions, $J'/J = 1.8(2)$, undergoes a dramatic change compared to lower pressures that we deduce is driven by a sharp drop in the dimer coupling, $J$. Our results underline the wide horizons opened by high-pressure INS experiments on quantum magnetic materials.

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arXiv2024

(C$_5$H$_9$NH$_3$)$_2$CuBr$_4$: a metal-organic two-ladder quantum magnet

Low-dimensional quantum magnets are a versatile materials platform for studying the emergent many-body physics and collective excitations that can arise even in systems with only short-range interactions. Understanding their low-temperature structure and spin Hamiltonian is key to explaining their magnetic properties, including unconventional quantum phases, phase transitions, and excited states. We study the metal-organic coordination compound (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$ and its deuterated counterpart, which upon its discovery was identified as a candidate two-leg quantum ($S = 1/2$) spin ladder in the strong-leg coupling regime. By growing large single crystals and probing them with both bulk and microscopic techniques, we deduce that two previously unknown structural phase transitions take place between 136 K and 113 K. The low-temperature structure has a monoclinic unit cell giving rise to two inequivalent spin ladders. We further confirm the absence of long-range magnetic order down to 30 mK and discuss the implications of this two-ladder structure for the magnetic properties of (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$.

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arXiv2024

Molecular intercalation in the van der Waals antiferromagnets FePS3 and NiPS3

We have performed electrochemical treatment of the van der Waals antiferromagnetic materials FePS$_3$ and NiPS$_3$ with the ionic liquid EMIM-BF$_4$, achieving significant molecular intercalation. Mass analysis of the intercalated compounds, EMIM$_x$-FePS$_3$ and EMIM$_x$-NiPS$_3$, indicated respective intercalation levels, $x$, of approximately 27\% and 37\%, and X-ray diffraction measurements demonstrated a massive (over 50\%) enhancement of the $c$-axis lattice parameters. To investigate the consequences of these changes for the magnetic properties, we performed magnetic susceptibility and $^{31}$P nuclear magnetic resonance (NMR) studies of both systems. For EMIM$_x$-FePS$_3$, intercalation reduces the magnetic ordering temperature from $T_N = 120$~K to 78~K, and we find a spin gap in the antiferromagnetic phase that drops from 45~K to 30~K. For EMIM$_x$-NiPS$_3$, the ordering temperature is almost unaffected (changing from 148~K to 145~K), but a change towards nearly isotropic spin fluctuations suggests an alteration of the magnetic Hamiltonian. Such relatively modest changes, given that the huge extension of the $c$ axes is expected to cause a very strong suppression any interlayer interactions, point unequivocally to the conclusion that the magnetic properties of both parent compounds are determined solely by two-dimensional (2D), intralayer physics. The changes in transition temperatures and low-temperature spin dynamics in both compounds therefore indicate that intercalation also results in a significant modulation of the intralayer magnetic interactions, which we propose is due to charge doping and localization on the P sites. Our study offers chemical intercalation with ionic liquids as an effective method to control not only the interlayer but also the intralayer interactions in quasi-2D magnetic materials.

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arXiv2023

Strong-coupling magnetophononics: Self-blocking, phonon-bitriplons, and spin-band engineering

Magnetophononics, the modulation of magnetic interactions by driving infrared-active lattice excitations, is emerging as a key mechanism for the ultrafast dynamical control of both semiclassical and quantum spin systems by coherent light. We demonstrate that, in a quantum magnet with strong spin-phonon coupling, resonances between the driven phonon and the spin excitation frequencies exhibit an intrinsic self-blocking effect, whereby only a fraction of the available laser power is absorbed by the phonon. Using the quantum master equations governing the nonequilibrium steady states of the coupled spin-lattice system, we show how self-blocking arises from the self-consistent alteration of the resonance frequencies. We link this to the appearance of mutually repelling collective spin-phonon states, which in the regime of strong hybridization become composites of a phonon and two triplons. We then identify the mechanism and optimal phonon frequencies by which to control a global nonequilibrium renormalization of the lattice-driven spin excitation spectrum and demonstrate that this effect should be observable in ultrafast THz experiments on a number of known quantum magnetic materials.

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arXiv2022

Investigating field-induced magnetic order in Han Purple by neutron scattering up to 25.9 T

BaCuSi$_2$O$_6$ is a quasi-two-dimensional (2D) quantum antiferromagnet containing three different types of stacked, square-lattice bilayer hosting spin-1/2 dimers. Although this compound has been studied extensively over the last two decades, the critical applied magnetic field required to close the dimer spin gap and induce magnetic order, which exceeds 23 T, has to date precluded any kind of neutron scattering investigation. However, the HFM/EXED instrument at the Helmholtz-Zentrum Berlin made this possible at magnetic fields up to 25.9 T. Thus we have used HFM/EXED to investigate the field-induced ordered phase, in particular to look for quasi-2D physics arising from the layered structure and from the different bilayer types. From neutron diffraction data, we determined the global dependence of the magnetic order parameter on both magnetic field and temperature, finding a form consistent with 3D quantum critical scaling; from this we deduce that the quasi-2D interactions and nonuniform layering of BaCuSi$_2$O$_6$ are not anisotropic enough to induce hallmarks of 2D physics. From neutron spectroscopy data, we measured the dispersion of the strongly Zeeman-split magnetic excitations, finding good agreement with the zero-field interaction parameters of BaCuSi$_2$O$_6$. We conclude that HFM/EXED allowed a significant extension in the application of neutron scattering techniques to the field range above 20 T and in particular opened new horizons in the study of field-induced magnetic quantum phase transitions.

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arXiv2022

Thermal Evolution of Dirac Magnons in the Honeycomb Ferromagnet CrBr$_3$

CrBr$_3$ is an excellent realization of the two-dimensional honeycomb ferromagnet, which offers a bosonic equivalent of graphene with Dirac magnons and topological character. We perform inelastic neutron scattering (INS) measurements using state-of-the-art instrumentation to update 50-year-old data, thereby enabling a definitive comparison both with recent experimental claims of a significant gap at the Dirac point and with theoretical predictions for thermal magnon renormalization. We demonstrate that CrBr$_3$ has next-neighbor $J_2$ and $J_3$ interactions approximately 5\% of $J_1$, an ideal Dirac magnon dispersion at the K point, and the associated signature of isospin winding. The magnon lifetime and the thermal band renormalization show the universal $T^2$ evolution expected from an interacting spin-wave treatment, but the measured dispersion lacks the predicted van Hove features, highlighting the need for a deeper theoretical analysis.

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arXiv2021

Giant Resonant Self-Blocking in Magnetophononically Driven Quantum Magnets

Magnetophononics, the modulation of magnetic interactions by driven infrared-active lattice excitations, is emerging as a key mechanism for the ultrafast dynamical control of both semiclassical and quantum spin systems by coherent light. We demonstrate that, in a quantum magnetic material with strong spin-phonon coupling, resonances between the driven phonon and the spin excitation frequencies exhibit a giant self-blocking effect. Instead of absorbing more energy, the spin system acts as a strong brake on the driven phonon, causing it to absorb only a tiny fraction of the power available from the laser. Using the quantum master equations governing the nonequilibrium steady states of the coupled spin-lattice system, we show how self-blocking dominates the dynamics, demonstrate the creation of mutually repelling hybrid spin-phonon states, and control the nonequilibrium renormalization of the lattice-driven spin excitation band.

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arXiv2021

Quantum Monte Carlo simulations in the trimer basis: first-order transitions and thermal critical points in frustrated trilayer magnets

The phase diagrams of highly frustrated quantum spin systems can exhibit first-order quantum phase transitions and thermal critical points even in the absence of any long-ranged magnetic order. However, all unbiased numerical techniques for investigating frustrated quantum magnets face significant challenges, and for generic quantum Monte Carlo methods the challenge is the sign problem. Here we report on a general quantum Monte Carlo approach with a loop-update scheme that operates in any basis, and we show that, with an appropriate choice of basis, it allows us to study a frustrated model of coupled spin-1/2 trimers: simulations of the trilayer Heisenberg antiferromagnet in the spin-trimer basis are sign-problem-free when the intertrimer couplings are fully frustrated. This model features a first-order quantum phase transition, from which a line of first-order transitions emerges at finite temperatures and terminates in a thermal critical point. The trimer unit cell hosts an internal degree of freedom that can be controlled to induce an extensive entropy jump at the quantum transition, which alters the shape of the first-order line. We explore the consequences for the thermal properties in the vicinity of the critical point, which include profound changes in the lines of maxima defined by the specific heat. Our findings reveal trimer quantum magnets as fundamental systems capturing in full the complex thermal physics of the strongly frustrated regime.

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arXiv2021

Field-Induced Spin Excitations in the Spin-1/2 Triangular-Lattice Antiferromagnet CsYbSe$_2$

A layered triangular lattice with spin-1/2 ions is an ideal platform to explore highly entangled exotic states like quantum spin liquid (QSL). Here, we report a systematic in-field neutron scattering study on a perfect two-dimensional triangular-lattice antiferromagnet, CsYbSe$_2$, a member of the large QSL candidate family rare-earth chalcogenides. The elastic neutron scattering measured down to 70 mK shows that there is a short-range 120$^{\circ}$ magnetic order at zero field. In the field-induced ordered states, the spin-spin correlation lengths along the $c$ axis are relatively short, although the heat capacity results indicate long-range magnetic orders at 3 T $-$ 5 T. The inelastic neutron scattering spectra evolve from highly damped continuum-like excitations at zero field to relatively sharp spin wave modes at the plateau phase. Our extensive large-cluster density-matrix renormalization group calculations with a Heisenberg triangular-lattice nearest-neighbor antiferromagnetic model reproduce the essential features of the experimental spectra, including continuum-like excitations at zero field, series of sharp magnons at the plateau phase as well as two-magnon excitations at high energy. This work presents comprehensive experimental and theoretical overview of the unconventional field-induced spin dynamics in triangular-lattice Heisenberg antiferromagnet and thus provides valuable insight into quantum many-body phenomena.

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