arXiv subjects

H. M. Rønnow

Publications and source records attributed to H. M. Rønnow.

At least 19 recordsLinked to original sources

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 $Γ$, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field $(π,0)$ 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.

cond-mat.str-el↗

arXiv2026

Magnetic Excitations of a Half-Filled Tl-based Cuprate

Strong electron correlations drive Mott insulator transitions. Yet, there exists no framework to classify Mott insulators by their degree of correlation. Cuprate superconductors, with their tunable doping and rich phase diagrams, offer a unique platform to investigate the evolution of these interactions. However, spectroscopic access to a clean half-filled Mott-insulating state is lacking in compounds with the highest superconducting onset temperature. To fill this gap, we introduce a pristine, half-filled thallium-based cuprate system, Tl$_2$Ba$_5$Cu$_4$O$_{x}$. Using high-resolution resonant inelastic x-ray scattering, we probe long-lived magnon excitations and uncover a pronounced kink in the magnon dispersion, marked by a simultaneous change in group velocity and lifetime broadening. Modeling the dispersion within a Hubbard-Heisenberg approach, we extract the interaction strength and compare it with other cuprate systems. Our results establish a cuprate universal relation between electron-electron interaction and magnon zone-boundary dispersion. Superconductivity seems to be optimal at intermediate correlation strength, suggesting an optimal balance between localization and itinerancy.

cond-mat.supr-con↗

arXiv2025

Impact of Electron Correlations on Infinite-Layer Cuprates and Nickelates

Optimization of unconventional superconductivity involves a balance of interaction strengths. Precise determination of correlation strength across different material families is therefore important. Here, we present a combined X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) study of infinite-layer PrNiO$_2$ and SrCuO$_2$ that enables fair comparison of their interaction strengths. For both compounds, we study the orbital and magnetic excitations and extract their dispersions along high-symmetry directions. Using a single-band Hubbard model and including higher-order exchange interactions, we derive the correlation factor $U/t$ for both compounds. A key finding is that despite a smaller Coulomb repulsion $U$, PrNiO$_2$ exhibits a correlation strength that is 20% stronger than that of its isostructural cuprate counterpart SrCuO$_2$. This indicates that a moderation of the correlation strength may further optimize superconductivity in nickelates.

cond-mat.supr-con↗

arXiv2025

Dynamic Competition between Cooper-Pair and Spin-Density-Wave Condensation

Quantum matter phases may co-exist microscopically even when they display competing tendencies. A fundamental question is whether such a competition can be avoided through the elimination of one phase while the other one condenses into the ground state. Here, we present a high-resolution neutron spectroscopy study of the low-energy spin excitations in the high-temperature superconductor La1.855Sr0.145CuO4. In the normal state, we find low-energy magnetic fluctuations at incommensurate reciprocal lattice positions where spin-density-wave order emerges at lower Sr concentration or at high magnetic fields. While these spin excitations are largely suppressed by the emergence of the superconducting spin gap, some low-energy magnetic fluctuations persist deep inside the superconducting state. We interpret this result in terms of a dynamic competition between superconductivity and magnetism, where superconductivity impedes the condensation of low-energy magnetic fluctuations through the formation of magnetically-mediated Cooper pairs.

cond-mat.supr-con↗

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, $γ= J_y/J_x$. 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.

cond-mat.str-el↗

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.

cond-mat.str-el↗

arXiv2024

Magnon interactions in a moderately correlated Mott insulator

Quantum fluctuations in low-dimensional systems and near quantum phase transitions have significant influences on material properties. Yet, it is difficult to experimentally gauge the strength and importance of quantum fluctuations. Here we provide a resonant inelastic x-ray scattering study of magnon excitations in Mott insulating cuprates. From the thin film of SrCuO$_2$, single- and bi-magnon dispersions are derived. Using an effective Heisenberg Hamiltonian generated from the Hubbard model, we show that the single-magnon dispersion is only described satisfactorily when including significant quantum corrections stemming from magnon-magnon interactions. Comparative results on La$_2$CuO$_4$ indicate that quantum fluctuations are much stronger in SrCuO$_2$ suggesting closer proximity to a magnetic quantum critical point. Monte Carlo calculations reveal that other magnetic orders may compete with the antiferromagnetic Néel order as the ground state. Our results indicate that SrCuO$_2$ - due to strong quantum fluctuations - is a unique starting point for the exploration of novel magnetic ground states.

cond-mat.str-el↗

arXiv2024

High-entropy magnetism of murunskite

Murunskite (K$_2$FeCu$_3$S$_4$) is a bridging compound between the only two known families of high-temperature superconductors. It is a semiconductor like the parent compounds of cuprates, yet isostructural to metallic iron-pnictides. Moreover, like both families, it has an antiferromagnetic (AF)-like response with an ordered phase occurring below $\approx$ 100 K. Through comprehensive neutron, Mössbauer, and XPS measurements on single crystals, we unveil AF with a nearly commensurate quarter-zone wave vector. Intriguingly, the only identifiable magnetic atoms, iron, are randomly distributed over one-quarter of available crystallographic sites in 2D planes, while the remaining sites are occupied by closed-shell copper. Notably, any interpretation in terms of a spin-density wave is challenging, in contrast to the metallic iron-pnictides where Fermi-surface nesting can occur. Our findings align with a disordered-alloy picture featuring magnetic interactions up to second neighbors. Moreover, in the paramagnetic state, iron ions are either in Fe$^{3+}$ or Fe$^{2+}$ oxidation states, associated with two distinct paramagnetic sites identified by Mössbauer spectroscopy. Upon decreasing the temperature below the appearance of magnetic interactions, these two signals merge completely into a third, implying an orbital transition. It completes the cascade of (local) transitions that transform iron atoms from fully orbitally and magnetically disordered to homogeneously ordered in inverse space, but still randomly distributed in real space.

cond-mat.str-el↗

arXiv2023

Orbital-selective metal skin induced by alkali-metal-dosing Mott-insulating Ca$_2$RuO$_4$

Doped Mott insulators are the starting point for interesting physics such as high temperature superconductivity and quantum spin liquids. For multi-band Mott insulators, orbital selective ground states have been envisioned. However, orbital selective metals and Mott insulators have been difficult to realize experimentally. Here we demonstrate by photoemission spectroscopy how Ca$_2$RuO$_4$, upon alkali-metal surface doping, develops a single-band metal skin. Our dynamical mean field theory calculations reveal that homogeneous electron doping of Ca$_2$RuO$_4$ results in a multi-band metal. All together, our results provide compelling evidence for an orbital-selective Mott insulator breakdown, which is unachievable via simple electron doping. Supported by a cluster model and cluster perturbation theory calculations, we demonstrate a novel type of skin metal-insulator transition induced by surface dopants that orbital-selectively hybridize with the bulk Mott state and in turn produce coherent in-gap states.

cond-mat.str-el↗

arXiv2023

Dynamics of K$_2$Ni$_2$(SO$_4$)$_3$ governed by proximity to a 3D spin liquid model

Quantum spin liquids (QSLs) have become a key area of research in magnetism due to their remarkable properties, such as long-range entanglement, fractional excitations, pinch-point singularities, and topologically protected phenomena. In recent years, the search for QSLs has expanded into the three-dimensional world, where promising features have been found in materials that form pyrochlore and hyper-kagome lattices, despite the suppression of quantum fluctuations due to high dimensionality. One such material is the $S = 1$ K$_2$Ni$_2$(SO$_4$)$_3$ compound, which belongs to the langbeinite family consisting of two interconnected trillium lattices. Although magnetically ordered, K$_2$Ni$_2$(SO$_4$)$_3$ has been found to exhibit a highly dynamical and correlated state which can be driven into a pure quantum spin liquid under magnetic fields of only $B \simeq 4$~T. In this article, we combine inelastic neutron scattering measurements with pseudo-fermion functional renormalization group (PFFRG) and classical Monte Carlo (cMC) calculations to study the magnetic properties of K$_2$Ni$_2$(SO$_4$)$_3$, revealing a high level of agreement between the experiment and theory. We further reveal the origin of the dynamical state in K$_2$Ni$_2$(SO$_4$)$_3$ by studying a larger set of exchange parameters, uncovering an `island of liquidity' around a focal point given by a magnetic network composed of tetrahedra on a trillium lattice.

cond-mat.str-el↗

arXiv2023

Investigation of role of antisite disorder in the pristine cage compound FeGa$_3$

The role of controlled disorder in the strong correlated narrow gap semiconductor candidate FeGa$_3$ has been investigated. Polycrystalline samples were synthesized by the combination of arc-melting furnace and successive annealing processes. Deviations of the occupation number of Fe and Ga sites from those expected in the pristine compound were quantified with X-ray analysis. Besides that, electrical transport and magnetization measurements reveal that hierarchy in Fe and Ga site disorder tunes the ground state of FeGa$_3$ from paramagnetic semiconducting to a magnetic metal. These findings are discussed within the framework of Anderson metal-insulator transitions and spin fluctuations.

cond-mat.mtrl-sci↗

arXiv2022

Spin wave spectra of single crystal CoPS$_3$

The spin waves in single crystals of the layered van der Waals antiferromagnet CoPS$_3$ have been measured using inelastic neutron scattering. The data show four distinct spin wave branches with large ($\gtrsim 14$ meV) energy gaps at the Brillouin zone center indicating significant anisotropy. The data were modelled using linear spin wave theory derived from a Heisenberg Hamiltonian. Exchange interactions up to the third nearest-neighbour in the layered planes were required to fit the data with ferromagnetic $J_1 = -1.37$ meV between first neighbours, antiferromagnetic $J_3 = 3.0$ meV between third neighbours, and a very small $J_2 = 0.09$ meV between second neighbours. A biaxial single-ion anisotropy was required, with a collinear term $D^x = -0.77$ meV for the axis parallel to the aligned moment direction and a coplanar term $D^z=6.07$ meV for an axis approximately normal to the layered crystal planes.

cond-mat.mtrl-sci↗

arXiv2022

Crossover of the high-energy spin fluctuations from collective triplons to localized magnetic excitations in doped Sr14-xCaxCu24O41 cuprate ladders

We studied the magnetic excitations in the quasi-one-dimensional (q-1D) ladder subsystem of Sr_(14-x) Ca_x Cu_24 O_41(SCCO) using Cu L_3-edge resonant inelastic X-ray scattering (RIXS). By comparing momentum-resolved RIXS spectra with (x=12.2) and without (x=0) high Ca content, we track the evolution of the magnetic excitations from collective two-triplon (2T) excitations (x=0) to weakly-dispersive gapped modes at an energy of 280 meV (x=12.2). Density matrix renormalization group (DMRG) calculations of the RIXS response in the doped ladders suggest that the flat magnetic dispersion and damped excitation profile observed at x=12.2 originates from enhanced hole localization. This interpretation is supported by polarization-dependent RIXS measurements, where we disentangle the spin-conserving ΔS=0 scattering from the predominant ΔS=1 spin-flip signal in the RIXS spectra. The results show that the low-energy weight in the ΔS=0 channel is depleted when Sr is replaced by Ca, consistent with a reduced carrier mobility. Our results demonstrate that off-ladder impurities can affect both the low-energy magnetic excitations and superconducting correlations in the CuO_4 plaquettes. Finally, our study characterizes the magnetic and charge fluctuations in the phase from which superconductivity emerges in SCCO at elevated pressures.

cond-mat.supr-con↗

arXiv2020

Vital role of anisotropy in cubic chiral skyrmion hosts

The impact of magnetic anisotropy on the skyrmion lattice (SkL) state in cubic chiral magnets has been overlooked for long, partly because a semi-quantitative description of the thermodynamically stable SkL phase pocket forming near the Curie temperature could be achieved without invoking anisotropy effects. However, there has been a range of phenomena reported recently in these materials, such as the formation of low-temperature tilted conical and SkL states as well as temperature-induced transformations of lattice geometry in metastable SkL states, where anisotropy was suspected to play a key role. To settle this issue on experimental basis, we quantified the cubic anisotropy in a series of CoZnMn-type cubic chiral magnets. We found that the strength of anisotropy is highly enhanced towards low temperatures in all the compounds, moreover, not only the magnitude but also the character of cubic anisotropy drastically varies upon changing the Co/Mn ratio. We correlate these changes with temperature- and composition-induced variations of the helical modulation vectors, the anharmonicity and structural rearrangements of the metastable SkLs and the spin relaxation rates. Similar systematic studies on magnetic anisotropy may not only pave the way for a quantitative and unified description of the stable and metastable modulated spin textures in cubic chiral magnets but would also help exploring further topological spin textures in this large class of skyrmion hosts.

cond-mat.str-el↗

arXiv2020

A quantum magnetic analogue to the critical point of water

At the familiar liquid-gas phase transition in water, the density jumps discontinuously at atmospheric pressure, but the line of these first-order transitions defined by increasing pressures terminates at the critical point, a concept ubiquitous in statistical thermodynamics. In correlated quantum materials, a critical point was predicted and measured terminating the line of Mott metal-insulator transitions, which are also first-order with a discontinuous charge density. In quantum spin systems, continuous quantum phase transitions (QPTs) have been investigated extensively, but discontinuous QPTs have received less attention. The frustrated quantum antiferromagnet SrCu$_2$(BO$_3$)$_2$ constitutes a near-exact realization of the paradigmatic Shastry-Sutherland model and displays exotic phenomena including magnetization plateaux, anomalous thermodynamics and discontinuous QPTs. We demonstrate by high-precision specific-heat measurements under pressure and applied magnetic field that, like water, the pressure-temperature phase diagram of SrCu$_2$(BO$_3$)$_2$ has an Ising critical point terminating a first-order transition line, which separates phases with different densities of magnetic particles (triplets). We achieve a quantitative explanation of our data by detailed numerical calculations using newly-developed finite-temperature tensor-network methods. These results open a new dimension in understanding the thermodynamics of quantum magnetic materials, where the anisotropic spin interactions producing topological properties for spintronic applications drive an increasing focus on first-order QPTs.

cond-mat.str-el↗

arXiv2020

Metastable skyrmion lattices governed by magnetic disorder and anisotropy in $β$-Mn-type chiral magnets

Magnetic skyrmions are vortex-like topological spin textures often observed in structurally chiral magnets with Dzyaloshinskii-Moriya interaction. Among them, Co-Zn-Mn alloys with a $β$-Mn-type chiral structure host skyrmions above room temperature. In this system, it has recently been found that skyrmions persist over a wide temperature and magnetic field region as a long-lived metastable state, and that the skyrmion lattice transforms from a triangular lattice to a square one. To obtain perspective on chiral magnetism in Co-Zn-Mn alloys and clarify how various properties related to the skyrmion vary with the composition, we performed systematic studies on Co$_{10}$Zn$_{10}$, Co$_9$Zn$_9$Mn$_2$, Co$_8$Zn$_8$Mn$_4$ and Co$_7$Zn$_7$Mn$_6$ in terms of magnetic susceptibility and small-angle neutron scattering measurements. The robust metastable skyrmions with extremely long lifetime are commonly observed in all the compounds. On the other hand, preferred orientation of a helimagnetic propagation vector and its temperature dependence dramatically change upon varying the Mn concentration. The robustness of the metastable skyrmions in these materials is attributed to topological nature of the skyrmions as affected by structural and magnetic disorder. Magnetocrystalline anisotropy as well as magnetic disorder due to the frustrated Mn spins play crucial roles in giving rise to the observed change in helical states and corresponding skyrmion lattice form.

cond-mat.str-el↗

arXiv2020

High-pressure specific heat technique to uncover novel states of quantum matter

AC-specific heat measurements remain as the foremost thermodynamic experimental method to underpin phase transitions in tiny samples. However, its performance under combined extreme conditions of high-pressure, very low temperature and intense magnetic fields needs to be broadly extended for investigation of quantum phase transition in strongly correlated electron systems. In this communication, we discuss the determination of specific heat on the quantum paramagnetic$-$insulator SrCu$_{2}$(BO$_{3}$)$_{2}$ by applying the AC-specific heat technique under extreme conditions. In order to apply this technique to insulating samples we sputtered a metallic thin film-heater and attached thermometer onto sample. Besides that, we performed full frequency scans with the aim to get quantitative specific heat data. Our results show that we can determine the sample heat capacity within 5$\%$ of accuracy respect to an adiabatic technique. This allows to uncover low energy scales that characterize the ground state of quantum spin entanglement in SrCu$_{2}$(BO$_{3}$)$_{2}$.

cond-mat.str-el↗

arXiv2020

Staggered-flux state for rectangular-lattice spin 1/2 Heisenberg antiferromagnet

We investigate the spin-1/2 Heisenberg model on a rectangular lattice, using the Gutzwiller projected variational wave function known as the staggered flux state. Using Monte Carlo techniques, the variational parameters and static spin-structure factor for different coupling anisotropies $γ=J_y/J_x$ are calculated. We observe a gradual evolution of the ground state energy towards a value which is very close to the 1D estimate provided by the Bethe ansatz and a good agreement between the finite size scaling of the energies. The spin-spin correlation functions exhibit a power-law decay with varying exponents for different anisotropies. Though the lack of Néel order makes the staggered flux state energetically unfavorable in the symmetric case $γ=1$, it appears to capture the essence of the system close to 1D. Hence we believe that the staggered flux state provides an interesting starting point to explore the crossover from quantum disordered chains to the Néel ordered 2D square lattices.

cond-mat.str-el↗