arXiv subjects

F. Orlandi

Publications and source records attributed to F. Orlandi.

At least 19 recordsLinked to original sources

arXiv2026

Melting upon cooling in a quantum magnet

Heating enhances thermal fluctuations and typically leads to melting of solids, but in exceptional cases, heating can also cause liquids to solidify. The paradigm of this counterintuitive phenomenon is solidification of liquid $^3$He upon increasing temperature, known as the Pomeranchuk effect. Here we show that such inverse melting also appears in quantum magnetism. We find that, on cooling, the Ising-like triangular-lattice antiferromagnet erbium heptatantalate first develops a three-sublattice long-range magnetic order -- analogous to a solid -- which then, unexpectedly, melts at even lower temperatures into a short-range correlated spin-stripe state -- analogous to a liquid. We propose that such an unprecedented ``spin Pomeranchuk effect" can generically arise from strong competition between spin-spin interactions in frustrated magnets, and provides a novel avenue to transformations between exotic magnetic phases.

cond-mat.str-el↗

arXiv2025

$\mathbb{Z}_2$ Vortex Crystal Candidate in the Triangular $S=1/2$ Quantum Antiferromagnet

The prospect of merging the paradigms of geometric frustration on a triangular lattice and bond anisotropies in the strong spin-orbit coupling limit holds tremendous promise in the ongoing hunt for exotic quantum materials. Here we identify a new candidate system to realize such physics, the organic quantum antiferromagnet (CD$_3$ND$_3$)$_2$NaRuCl$_6$. We report a combination of thermodynamic, magneto-elastic and neutron scattering experiments on single-crystals to determine the phase diagram in axial magnetic fields $\mathbf{H \parallel c}$ and propose a minimal model Hamiltonian. (CD$_3$ND$_3$)$_2$NaRuCl$_6$ displays an ideal triangular arrangement of Ru$^{3+}$ ions adopting the spin-orbital entangled $j_{\rm eff} = 1/2$ state. It hosts residual magnetic order below $T_{\rm N} = 0.23$ K and a highly unusual $H-T$ phase diagram including three different incommensurate states. Spin-waves in the high-field polarized regime are well described by a Heisenberg-like triangular lattice Hamiltonian with a potential sub-leading bond dependent anisotropy term $J_{\pm\pm}$. We discuss possible candidate magnetic structures in the various observed phases and propose two mechanisms that could explain the field-dependent incommensurability, requiring either a small ferromagnetic Kitaev term or a tiny magneto-elastic $J-J'$ isosceles distortion driven by pseudospin-lattice coupling. We argue that the multi-$\mathbf{q}$ ground state in zero magnetic field is a prime candidate for hosting the $\mathbb{Z}_2$ vortex crystal proposed on the triangular Heisenberg-Kitaev model. (CD$_3$ND$_3$)$_2$NaRuCl$_6$ is the first member in an extended family of quantum triangular lattice magnets, providing a new playground to study the interplay of geometric frustration and spin-orbit effects.

cond-mat.str-el↗

arXiv2025

Magnetic Ground State and Spin Excitations in the 2D Trimerized Collinear-II Lattice Antiferromagnet Li2Ni3P4O14

We report the magnetic ground state, spin excitations, and spin Hamiltonian of the 2D spin-1 trimerized Heisenberg antiferromagnet Li2Ni3P4O14. Below the magnetic ordering temperature TN = 14.5 K, the compound exhibits a canted long-range antiferromagnetic order with a propagation vector k = (0 0 0), consistent with the magnetic space group P21/c.1 (No. 14.75). The ground state magnetic structure consists of ferromagnetic spin-trimers of Ni2+ ions. The spin-trimers are coupled antiferromagnetically along the c-axis and ferromagnetically along the a-axis. Inelastic neutron scattering (INS) reveals gapped and dispersive magnon excitations below the TN, and gapless quasi-elastic scatterings at higher temperature. The linear spin-wave theory simulations reveal the essential features of the excitation spectrum; by a spin Hamiltonian composed of ferromagnetic intra-trimer exchange interaction J1 and inter-trimer exchange interactions J2 (FM) and J3(AFM) within the bc plane. The J2 and J3 along the b-axis and c-axis, respectively, with strengths of J2/J1=0.79 and J3/J1=-0.91. In addition, a weak inter planer ferromagnetic exchange interaction J4 (|J4/J1|~0.12) is found along the a-axis. The determined exchange constants reveal a 2D trimerized Collinear-II spin lattice within the bc-plane. The analysis of INS spectra by linear spin-wave theory also yields a moderate single-ion anisotropy (D/J1=0.48) which accounts for the observed spin gap below TN as well as the metamagnetic transition near 44 kOe in dc magnetization (M vs H) curves. These findings identify Li2Ni3P4O14 as a rare realization of a two-dimensional trimerized spin system and offer the direct experimental confirmation of theoretically predicted magnon excitations, unveiling the fundamental characteristics of the expected excitation spectrum.

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arXiv2025

Enhanced two-dimensional ferromagnetism in van der Waals $\beta$-UTe$_3$ monolayers

The discovery of local-moment magnetism in van der Waals (vdW) semiconductors down to the single-layer limit has led to a paradigm shift in the understanding of two-dimensional (2D) magnets and unleashed their potential for applications in microelectronic and optoelectronic devices. The incorporation of strong electronic and magnetic correlations in 2D vdW metals remains a sought-after platform not only to enable control of emergent quantum phases, such as superconductivity, but also to achieve more theoretically tractable microscopic models of complex materials. To date, however, there is limited success in the discovery of such metallic vdW platforms, and $f$-electron monolayers remain out of reach. Here we demonstrate that the actinide $\beta$-UTe$_3$ can be exfoliated to the monolayer limit. A sizable electronic specific heat coefficient provides the hallmark of strong correlations. Remarkably, $\beta$-UTe$_3$ remains ferromagnetic in the half-unit-cell limit with an enhanced ordering temperature of 35 K, a factor of two larger than its bulk counterpart. Our work establishes $\beta$-UTe$_3$ as a novel materials platform for investigating and modeling correlated behavior in the monolayer limit and opens numerous avenues for quantum control with, e.g., strain engineering.

cond-mat.str-el↗

arXiv2025

Magnetic properties of the zigzag ladder compound SrTb2O4

We report on the properties of SrTb2O4, a frustrated zigzag ladder antiferromagnet, studied by single crystal neutron diffraction (with polarised neutrons in zero field and unpolarised neutrons in an applied magnetic field), as well as by neutron spectroscopy on a polycrystalline sample. The neutron scattering results are supported by single crystal magnetisation and heat capacity measurements. In zero field, neutron diffraction data show no transition to a magnetically ordered state down to the lowest experimentally available temperature of 35 mK, and the material remains magnetically disordered down to this temperature. Polarised neutron diffraction measurements reveal the presence of a diffuse scattering signal suggesting only very weak spin-spin correlations in the ground state. For H // c (the easy magnetisation direction), we followed the magnetisation process using neutron diffraction measurements and observed the appearance of field-induced magnetic Bragg peaks with integer h and k indices in the (hk0) scattering plane. No magnetic peaks with a non-zero propagation vector were detected. The observed in-field data fit well to a simple two-sublattice model with magnetic moments aligned along the field direction but being significantly different in magnitude for the two inequivalent Tb3+ sites in the unit cell. Overall, the collected data point to a nonmagnetic ground state in SrTb2O4 despite the presence of strong interactions.

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arXiv2024

Competing charge and magnetic order in the candidate centrosymmetric skyrmion host EuGa$_2$Al$_2$

Eu(Ga$_{1-x}$Al$_x$)$_4$ are centrosymmetric systems that have recently been identified as candidates to stabilise topologically non-trivial magnetic phases, such as skyrmion lattices. In this Letter, we present a high-resolution resonant x-ray and neutron scattering study on EuAl2Ga2 that provides new details of the complex coupling between the electronic ordering phenomena. Our results unambiguously demonstrate that the system orders to form a spin density wave with moments aligned perpendicular to the direction of the propagation vector, and upon further cooling, a cycloid with moments in the ab plane, in contrast to what has been reported in the literature. We show that concomitant with the onset of the spin density wave is the suppression of the charge order, indicative of a coupling between the localised 4$f$ electrons and itinerant electron density. Furthermore we demonstrate that the charge density wave order breaks the four-fold symmetry present in the I4/mmm crystal structure, thus declassifying these systems as square-net magnets.

cond-mat.str-el↗

arXiv2024

Spontaneous spin chirality reversal and competing phases in the topological magnet EuAl$_4$

We demonstrate the spontaneous reversal of spin chirality in a single crystal sample of the intermetallic magnet EuAl$_4$. We solve the nanoscopic nature of each of the four magnetically phases of EuAl$_4$ using resonant magnetic x-ray scattering, and demonstrate all four phases order with single-k incommensurate magnetic modulation vectors. Below 15.4 K the system forms a spin density modulated spin structure where the spins are orientated in the ab plane perpendicular to the orientation of the magnetic propagation vector. Below 13.2 K a second spin density wave orders with moments aligned parallel to the c-axis, such that the two spin density wave orders coexist. Below 12.2 K a magnetic helix of a single chirality is stabilised across the entire sample. Below 10 K the chirality of the magnetic helix reverses, and the sample remains a single chiral domain. Concomitant with the establishment of the helical magnetic ordering is the lowering of the crystal symmetry to monoclinic, as evidenced the formation of uniaxial charge and spin strip domains. A group theoretical analysis demonstrates that below 12.2 K the symmetry lowers to polar monoclinic, which is necessary to explain the observed asymmetry in the chiral states of the magnetic helix and the spin chiral reversal. We find that in every magnetically ordered phase of EuAl4 the in-plane moment is perpendicular to the orientation of the magnetic propagation vector, which we demonstrate is favoured by magnetic dipolar interactions.

cond-mat.str-el↗

arXiv2024

Magnetic field-induced phases and spin Hamiltonian in Cs2CoBr4

Magnetic structures and spin excitations are studied across the phase diagram of the geometrically frustrated S = 3/2 quantum antiferromagnet Cs2CoBr4 in magnetic fields applied along the magnetic easy axis, using neutron diffraction, inelastic neutron scattering and THz absorption spectroscopy. The data are analyzed, where appropriate, using extended SU (4) linear spin wave theory. A minimal magnetic Hamiltonian is proposed based on measurements in the high field polarized state. It deviates considerably from the previously considered models. Additional dilatometry experiments highlight the importance of magnetoelastic coupling in this system.

cond-mat.str-el↗

arXiv2023

Unusual magnetism of the axion-insulator candidate Eu$_5$In$_2$Sb$_6$

Eu$_5$In$_2$Sb$_6$ is a member of a family of orthorhombic nonsymmorphic rare-earth intermetallics that combines large localized magnetic moments and itinerant exchange with a low carrier density and perpendicular glide planes. This may result in special topological crystalline (wallpaper fermion) or axion insulating phases. Recent studies of Eu$_5$In$_2$Sb$_6$ single crystals have revealed colossal negative magnetoresistance and multiple magnetic phase transitions. Here, we clarify this ordering process using neutron scattering, resonant elastic X-ray scattering, muon spin-rotation, and magnetometry. The nonsymmorphic and multisite character of Eu$_5$In$_2$Sb$_6$ results in coplanar noncollinear magnetic structure with an Ising-like net magnetization along the $a$ axis. A reordering transition, attributable to competing ferro- and antiferromagnetic couplings, manifests as the onset of a second commensurate Fourier component. In the absence of spatially resolved probes, the experimental evidence for this low-temperature state can be interpreted either as an unusual double-$q$ structure or in a phase separation scenario. The net magnetization produces variable anisotropic hysteretic effects which also couple to charge transport. The implied potential for functional domain physics and topological transport suggests that this structural family may be a promising platform to implement concepts of topological antiferromagnetic spintronics.

cond-mat.str-el↗

arXiv2023

Field-induced phase transitions and anisotropic magnetic properties of the Kiteav-Heisenberg compound Na$_2$Co$_2$TeO$_6$

Spin systems with honeycomb structures have recently attracted a great deal of attention in connection with the Kitaev quantum spin liquid state (QSL) predicted theoretically. One possible Kitaev QSL candidate is Na$_2$Co$_2$TeO$_6$ realizing a honeycomb lattice of pseudo-spin-1/2. Field-dependent single-crystal neutron diffraction technique allows us to determine the microscopic spin-spin correlations across the field induced phase transitions for H//a and H//a* in plane field directions. Our results reveal phase transitions, initially to a canted zigzag antiferromagnetic state at approximately 60 kOe, followed by a possible transition to a partially polarized state over the range of 90-120 kOe, and finally to a field-induced fully polarized state above 120 kOe. We observe distinct field dependencies of the magnetic peak intensities for H//a and H//a*. In addition, low-temperature electron spin resonance in magnetic fields H//c yields a complete softening for one of the antiferromagnetic resonances at ~ 40 kOe, revealing a field-induced phase transition. The present work, thus, provides new insights into the field evolution of the important Kitaev-Heisenberg spin system Na$_2$Co$_2$TeO$_6$.

cond-mat.str-el↗

arXiv2023

Negative Magnetization and Magnetic Ordering of Rare Earth and Transition Metal Sublattices in NdFe0.5Cr0.5O3

We investigate the effect of alloying at the 3d transition metal site of a rare-earth-transition metal oxide, by considering NdFe0.5Cr0.5O3 alloy with two equal and random distribution of 3d ions, Cr and Fe, interacting with an early 4f rare earth ion, Nd. Employing temperature- and field-dependent magnetization measurements, temperature-dependent x-ray diffraction, neutron powder diffraction, and Raman spectroscopy, we characterize its structural and magnetic properties. Our study reveals bipolar magnetic switching (arising from negative magnetization) and magnetocaloric effect which underline the potential of the studied alloy in device application. The neutron diffraction study shows the absence of spin reorientation transition over the entire temperature range of 1.5-320 K, although both parent compounds exhibit spin orientation transition. We discuss the microscopic origin of this curious behavior. The neutron diffraction results also reveal the ordering of Nd spins at an unusually high temperature of about 40 K, which is corroborated by Raman measurements.

cond-mat.mtrl-sci↗

arXiv2023

Incommensurate antiferromagnetism in UTe2 under pressure

The discovery of multiple superconducting phases in UTe2 boosted research on correlated-electron physics. This heavy-fermion paramagnet was rapidly identified as a reference compound to study the interplay between magnetism and unconventional superconductivity with multiple degrees of freedom. The proximity to a ferromagnetic quantum phase transition was initially proposed as a driving force to triplet-pairing superconductivity. However, we find here that long-range incommensurate antiferromagnetic order is established under pressure. The propagation vector km = (0.07,0.33,1) of the antiferromagnetic phase is close to a wavevector where antiferromagnetic fluctuations have previously been observed at ambient pressure. These elements support that UTe2 is a nearly-antiferromagnet at ambient pressure. Our work appeals for theories modelling the evolution of the magnetic interactions and electronic properties, driving a correlated paramagnetic regime at ambient pressure to a long-range antiferromagnetic order under pressure. A deeper understanding of itinerant-f-electrons magnetism in UTe2 will be a key for describing its unconventional superconducting phases.

cond-mat.str-el↗

arXiv2023

Magnetic structure, excitations and field induced transitions in the honeycomb lattice $\rm{Er_2Si_2O_7}$

We investigate the magnetic properties of the monoclinic D-type $\rm{Er_2Si_2O_7}$ with a distorted honeycomb lattice using powder and single crystal neutron scattering techniques, as well as single crystal magnetisation measurements. The powder neutron diffraction shows that below the ordering temperature, $T_{\rm N}=1.85$ K, the compound forms a ${\bf q}=0$ antiferromagnetic structure with four sublattices. For $H \! \parallel \! a$, magnetisation measurements reveal a narrow, but clearly visible plateau at one third of the magnetisation saturation value. The plateau's stabilisation is accompanied by a significant increase of the magnetic unit cell, as the magnetic peaks with fractional indices are observed in single crystal neutron diffraction experiments. At low-temperatures, the inelastic neutron scattering measurements reveal the presence of low-energy dispersionless excitations. Their spectrum is sensitive to the applied field, it significantly softens on the magnetisation plateau, and demonstrates the behaviour expected for a non-collinear Ising antiferromagnet away from the plateau.

cond-mat.str-el↗

arXiv2023

Strain control of a bandwidth-driven spin reorientation in Ca$_{3}$Ru$_{2}$O$_{7}$

The layered-ruthenate family of materials possess an intricate interplay of structural, electronic and magnetic degrees of freedom that yields a plethora of delicately balanced ground states. This is exemplified by Ca$_{3}$Ru$_{2}$O$_{7}$, which hosts a coupled transition in which the lattice parameters jump, the Fermi surface partially gaps and the spins undergo a $90^{\circ}$ in-plane reorientation. Here, we show how the transition is driven by a lattice strain that tunes the electronic bandwidth. We apply uniaxial stress to single crystals of Ca$_{3}$Ru$_{2}$O$_{7}$, using neutron and resonant x-ray scattering to simultaneously probe the structural and magnetic responses. These measurements demonstrate that the transition can be driven by externally induced strain, stimulating the development of a theoretical model in which an internal strain is generated self-consistently to lower the electronic energy. We understand the strain to act by modifying tilts and rotations of the RuO$_{6}$ octahedra, which directly influences the nearest-neighbour hopping. Our results offer a blueprint for uncovering the driving force behind coupled phase transitions, as well as a route to controlling them.

cond-mat.str-el↗

arXiv2023

Spin-density-wave order controlled by uniaxial stress in CeAuSb$_2$

The tetragonal heavy-fermion compound CeAuSb$_2$ (space group $P4/nmm$) exhibits incommensurate spin density wave (SDW) order below $T_{N}\approx6.5~K$ with the propagation vector $\mathbf{q}_A = (δ_A,δ_A,1/2)$. The application of uniaxial stress along the [010] direction induces a sudden change in the resistivity ratio $ρ_a/ρ_b$ at a compressive strain of $ε\approx -0.5$\%. Here we use neutron scattering to show that the uniaxial stress induces a first-order transition to a SDW state with a different propagation vector $(0,δ_B,1/2)$ with $δ_B=0.25$. The magnetic structure of the new (B) phase consists of Ce layers with ordered moments alternating with layers with zero moment stacked along the $c$-axis. The ordered layers have an up-up-down-down configuration along the $b$-axis. This is an unusual situation in which the loss of spatial inversion is driven by the magnetic order. We argue that the change in SDW wavevector leads to Fermi surface reconstruction and a concomitant change in the transport properties.

cond-mat.str-el↗

arXiv2023

The crystal and magnetic structure of cesium superoxide

CsO2 is a member of the family of alkali superoxides (formula AO2 with A= Na, K, Rb and Cs) that exhibit magnetic behavior arising from open $p$-shell electrons residing on O2- molecules. We use neutron diffraction to solve the crystal and magnetic structures of CsO2, and observe a complex series of structures on cooling from room temperature to 1.6 K. These include an incommensurate modulation along the a-axis of the structure at intermediate temperatures, which then locks into a commensurate modulation that doubles the unit cell compared to the previously supposed orthorhombic unit cell. In both incommensurate and commensurate phases our structural solution involves a staggering of the cesium ion positions along the b-axis, in contrast to studies of other alkali superoxides in which staggered tilts of the O2- dimers relative to the c-axis are seen. Below T ~ 10 K we observe magnetic Bragg reflections arising from an antiferromagnetically ordered structure with a wavevector of k = (0,0,0) (relative to the doubled crystallographic unit cell), with moments that point predominantly along the b-axis with a small component along the a-axis that hints at possible anisotropic exchange coupling (consistent with the crystal structure). Measurements of the magnetic Bragg reflections in an applied magnetic field suggest a spin-flop transition takes place between 2 T and 4 T in which moments likely flop to point along the crystallographic a-axis. Our measurements indicate that CsO2 is an interesting example of magnetic properties being inherently linked to the crystal structure, in that the staggered displacement of the cesium ions activates antisymmetric exchange which then permits the observed spin canting.

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arXiv2023

The Double-$Q$ Ground State with Topological Charge Stripes in the Skyrmion Candidate $\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$

$\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$ is a centrosymmetric magnet in which a skyrmion lattice has recently been discovered. Here, we investigate the magnetic structure of the zero field ground state using neutron diffraction on single crystal and polycrystalline $^{\text{160}}\text{GdRu}_{\text{2}}\text{Si}_{\text{2}}$. In addition to observing the principal propagation vectors $\mathbf{q}_{1}$ and $\mathbf{q}_{2}$, we discover higher order magnetic satellites, notably $\mathbf{q}_{1} + 2\mathbf{q}_{2}$. The appearance of these satellites are explained within the framework of a new double-$Q$ constant-moment solution. Using powder diffraction we implement a quantitative refinement of this model. This structure, which contains vortexlike motifs, is shown to have a one-dimensional topological charge density.

cond-mat.str-el↗

arXiv2022

Effective decoupling of ferromagnetic sublattices by frustration in Heusler alloys

Magnetic frustration in ferromagnetic metallic systems is unusual due to the long-range and symmetric nature of the exchange interactions. In this work we prove that it is possible to obtain a highly frustrated ferromagnetic phase in a multi-sublattices cubic structure through a fine tuning of the magnetic interactions. This peculiar state is achieved in Ni-Mn-(In, Sn) Heusler alloys and results in the effective decoupling of their two intertwined ferromagnetic sublattices. One sublattice is ferromagnetic long range ordered below the macroscopic Curie temperature (TC ) whereas the second one remains disordered until a crossover to a polarized state occurs at T << TC . This result points out that a fine engineering of the magnetic interactions in metallic systems can lead to interesting novel and emergent phenomena.

cond-mat.mtrl-sci↗