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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., Comment: Main text + supplemental material

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, M\"ossbauer, 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 M\"ossbauer 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., Comment: 17 pages, 8 figure, 2 tables (9 pages, 4 figures in the main text; 8 pages, 4 figures, 2 tables in the appendix)

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 N\'eel 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.

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., Comment: A revised version of this manuscript will appear in Communications Physics

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.

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., Comment: 11 pages, 6 figures, 3 tables

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.

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 {\Delta}S=0 scattering from the predominant {\Delta}S=1 spin-flip signal in the RIXS spectra. The results show that the low-energy weight in the {\Delta}S=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.

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.

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., Comment: 8+4 pages, 4+3 figures

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 $\beta$-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., Comment: 70 pages, 19 figures

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$_{3}$)$_{2}$., Comment: To be published in Journal of Physics: Conference Series

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 $\gamma=J_y/J_x$ 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 N\'eel order makes the staggered flux state energetically unfavorable in the symmetric case $\gamma=1$, 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 N\'eel ordered 2D square lattices.

It is well established that in the low-temperature limit, the two-dimensional quantum Heisenberg antiferromagnet on a square lattice (2DQHAFSL) exhibits an anomaly in its spectrum at short-wavelengths on the zone-boundary. In the vicinity of the $(\pi,0)$ point the pole in the one-magnon response exhibits a downward dispersion, is heavily damped and attenuated, giving way to an isotropic continuum of excitations extending to high energies. The origin of the anomaly and the presence of the continuum are of current theoretical interest, with suggestions focused around the idea that the latter evidences the existence of spinons in a two-dimensional system. Here we present the results of neutron inelastic scattering experiments and Quantum Monte Carlo calculations on the metallo-organic compound Cu(DCOO)$_2\cdot 4$D$_2$O (CFTD), an excellent physical realisation of the 2DQHAFSL, designed to investigate how the anomaly at $(\pi,0)$ evolves up to finite temperatures $T/J\sim2/3$. Our data reveal that on warming the anomaly survives the loss of long-range, three-dimensional order, and is thus a robust feature of the two-dimensional system. With further increase of temperature the zone-boundary response gradually softens and broadens, washing out the $(\pi,0)$ anomaly. This is confirmed by a comparison of our data with the results of finite-temperature Quantum Monte Carlo simulations where the two are found to be in good accord. At lower energies, in the vicinity of the antiferromagnetic zone centre, there was no significant softening of the magnetic excitations over the range of temperatures investigated., Comment: Dedicated to the life and work of Professor Roger Cowley. 22 pages, 8 figures

We use resonant inelastic x-ray scattering to investigate charge-stripe correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$. By differentiating elastic from inelastic scattering, it is demonstrated that charge-stripe correlations precede both the structural low-temperature tetragonal phase and the transport-defined pseudogap onset. The scattering peak amplitude from charge stripes decays approximately as $T^{-2}$ towards our detection limit. The in-plane integrated intensity, however, remains roughly temperature independent. Therefore, although the incommensurability shows a remarkably large increase at high temperature, our results are interpreted via a single scattering constituent. In fact, direct comparison to other stripe-ordered compounds (La$_{1.875}$Ba$_{0.125}$CuO$_4$, La$_{1.475}$Nd$_{0.4}$Sr$_{0.125}$CuO$_4$ and La$_{1.875}$Sr$_{0.125}$CuO$_4$) suggests a roughly constant integrated scattering intensity across all these compounds. Our results therefore provide a unifying picture for the charge-stripe ordering in La-based cuprates. As charge correlations in La$_{1.675}$Eu$_{0.2}$Sr$_{0.125}$CuO$_4$ extend beyond the low-temperature tetragonal and pseudogap phase, their emergence heralds a spontaneous symmetry breaking in this compound.

Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as the quantum spin liquids (QSLs) in real materials. In this work, we address exchange interactions in Sr2CuTe$_{1-x}$W$_{x}$O, a series of double perovskites that realize the spin-1/2 square lattice and were suggested to harbor a QSL ground state arising from random distribution of non-magnetic ions. Our {\it ab initio} multi-reference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor explained by the crucial role of unoccupied states of non-magnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the end compounds, as well as explain the magnetic excitations in Sr2CuTe$_{0.5}$W$_{0.5}$O as emerging from the bond-disordered exchange couplings. Our results provide crucial understanding of the role of non-magnetic cations in exchange interactions paving the way to further exploration of QSL phases in bond-disordered materials., Comment: Version accepted in Phys. Rev. Lett

We have used exact numerical diagonalization to study the excitation spectrum and the dynamic spin correlations in the $s=1/2$ next-next-nearest neighbor Heisenberg antiferromagnet on the square lattice, with additional 4-spin ring exchange from higher order terms in the Hubbard expansion. We have varied the ratio between Hubbard model parameters, $t/U$, to obtain different relative strengths of the exchange parameters, while keeping electrons localized. The Hubbard model parameters have been parametrized via an effective ring exchange coupling, $J_r$, which have been varied between 0$J$ and 1.5$J$. We find that ring exchange induces a quantum phase transition from the $(\pi, \pi)$ ordered Ne\`el state to a $(\pi/2, \pi/2)$ ordered state. This quantum critical point is reduced by quantum fluctuations from its mean field value of $J_r/J = 2$ to a value of $\sim 1.1$. At the quantum critical point, the dynamical correlation function shows a pseudo-continuum at $q$-values between the two competing ordering vectors.

Magnetic helices and skyrmions in noncentrosymmetric magnets are representative examples of chiral spin textures in solids. Their spin swirling direction, often termed as the magnetic helicity and defined as either left-handed or right-handed, is uniquely determined by the Dzyaloshinskii-Moriya interaction (DMI) in fixed chirality host crystals. Thus far, there have been relatively few investigations of the DMI in metallic magnets as compared with insulating counterparts. Here, we focus on the metallic magnets Co$_{8-x}$Fe$_x$Zn$_8$Mn$_4$ (0 $\leq$ $x$ $\leq$ 4.5) with a $\beta$-Mn-type chiral structure and find that as $x$ varies under a fixed crystal chirality, a reversal of magnetic helicity occurs at $x_\mathrm{c}$ $\sim$ 2.7. This experimental result is supported by a theory based on first-principles electronic structure calculations, demonstrating the DMI to depend critically on the electron band filling. Thus by composition tuning our work shows the sign change of the DMI with respect to a fixed crystal chirality to be a universal feature of metallic chiral magnets., Comment: 37 pages, 12 figures

Magnetic skyrmions are vortex-like topological spin textures often observed to form a triangular-lattice skyrmion crystal in structurally chiral magnets with Dzyaloshinskii-Moriya interaction. Recently $\beta$-Mn structure-type Co-Zn-Mn alloys were identified as a new class of chiral magnet to host such skyrmion crystal phases, while $\beta$-Mn itself is known as hosting an elemental geometrically frustrated spin liquid. Here we report the intermediate composition system Co$_7$Zn$_7$Mn$_6$ to be a unique host of two disconnected, thermal-equilibrium topological skyrmion phases; one is a conventional skyrmion crystal phase stabilized by thermal fluctuations and restricted to exist just below the magnetic transition temperature $T_\mathrm{c}$, and the other is a novel three-dimensionally disordered skyrmion phase that is stable well below $T_\mathrm{c}$. The stability of this new disordered skyrmion phase is due to a cooperative interplay between the chiral magnetism with Dzyaloshinskii-Moriya interaction and the frustrated magnetism inherent to $\beta$-Mn., Comment: 57 pages, 16 figures

Helimagnetic materials are identified as promising for novel spintronic applications. Since helical spin order is manifested as a compromise of competing magnetic exchange interactions, its emergence is limited by unique constraints imposed by the crystalline lattice and the interaction geometries, as exemplified by the multiferroic perovskite manganites with large orthorhombic distortion. Here we show that a simple cubic perovskite SrCoO$_3$ with room-temperature ferromagnetism has the potential to host helimagnetic order upon isotropic lattice expansion. Increasing the Ba content $x$ in Sr$_{1-x}$Ba$_x$CoO$_3$ continuously expands the cubic lattice, eventually suppressing the ferromagnetic order near $x$=0.4, where helimagnetic correlations are observed as incommensurate diffuse magnetic scattering by neutron diffraction measurements. The emergence of helimagnetism is semi-quantitatively reproduced by first-principles calculations, leading to the conjecture that a simple cubic lattice with strong $d$-$p$ hybridisation can exhibit a variety of novel magnetic phases originating from competing exchange interactions., Comment: 14 pages, 4 figures, To appear in Phys. Rev. Materials

Using small-angle neutron scattering (SANS), we investigate the deformation of the magnetic skyrmion lattice in bulk single-crystalline MnSi under electric current flow. A significant broadening of the skyrmion-lattice-reflection peaks was observed in the SANS pattern for current densities greater than a threshold value j_t ~ 1 MA/m^2 (10^6 A/m^2). We show this peak broadening to originate from a spatially inhomogeneous rotation of the skyrmion lattice, with an inverse rotation sense observed for opposite sample edges aligned with the direction of current flow. The peak broadening (and the corresponding skyrmion lattice rotations) remain finite even after switching off the electric current. These results indicate that skyrmion lattices under current flow experience significant friction near the sample edges, and plastic deformation due to pinning effects, these being important factors that must be considered for the anticipated skyrmion-based applications in chiral magnets at the nanoscale.

Due to their topological protection and nanometric size, magnetic skyrmions are anticipated to form components of new high-density memory technologies. In metallic systems skyrmion manipulation is achieved easily under a low density electric current flow, although the inevitable thermal dissipation ultimately limits the energy efficacy of potential applications. On the other hand, a near dissipation-free skyrmion and skyrmion phase manipulation is expected by using electric \emph{fields}, thus meeting better the demands of an energy-conscious society. In this work on an insulating chiral magnet Cu$_{2}$OSeO$_{3}$ with magnetoelectric coupling, we use neutron scattering to demonstrate directly i) the creation of metastable skyrmion states over an extended range in magnetic field and temperature, and ii) the in-situ electric field-driven switching between topologically distinct phases; the skyrmion phase and a competing non-topological cone phase. For our accessible electric field range, the phase switching is achieved in a high temperature regime, and the remnant (E=0) metastable skyrmion state is thermally volatile with an exponential lifetime on hour timescales. Nevertheless, by taking advantage of the demonstrably longer-lived metastable skyrmion states at lower temperatures, a truly non-volatile and near dissipation-free topological phase change memory function is promised in magnetoelectric chiral magnets.

The transition temperature $T_\textrm{c}$ of unconventional superconductivity is often tunable. For a monolayer of FeSe, for example, the sweet spot is uniquely bound to titanium-oxide substrates. By contrast for La$_{2-\mathrm{x}}$Sr$_\mathrm{x}$CuO$_4$ thin films, such substrates are sub-optimal and the highest $T_\textrm{c}$ is instead obtained using LaSrAlO$_4$. An outstanding challenge is thus to understand the optimal conditions for superconductivity in thin films: which microscopic parameters drive the change in $T_\mathrm{c}$ and how can we tune them? Here we demonstrate, by a combination of x-ray absorption and resonant inelastic x-ray scattering spectroscopy, how the Coulomb and magnetic-exchange interaction of La$_2$CuO$_4$ thin films can be enhanced by compressive strain. Our experiments and theoretical calculations establish that the substrate producing the largest $T_\textrm{c}$ under doping also generates the largest nearest neighbour hopping integral, Coulomb and magnetic-exchange interaction. We hence suggest optimising the parent Mott state as a strategy for enhancing the superconducting transition temperature in cuprates., Comment: 15 pages, 7 figures and 2 tables (including Supplementary Information)

Ferroic magnetic quadrupole order exhibiting macroscopic magnetoelectric activity is discovered in the novel compound $A$(TiO)Cu$_4$(PO$_4$)$_4$ with $A$ = Pb, which is in contrast with antiferroic quadrupole order observed in the isostructural compounds with $A$ = Ba and Sr. Unlike the famous lone-pair stereochemical activity which often triggers ferroelectricity as in PbTiO$_3$, the Pb$^{2+}$ cation in Pb(TiO)Cu$_4$(PO$_4$)$_4$ is stereochemically inactive but dramatically alters specific magnetic interactions and consequently switches the quadrupole order from antiferroic to ferroic. Our first-principles calculations uncover a positive correlation between the degree of $A$-O bond covalency and a stability of the ferroic quadrupole order., Comment: 7 pages, 4 figures

One-dimensional (1D) magnetic insulators have attracted significant interest as a platform for studying emergent phenomena such as quasiparticle fractionalization and quantum criticality. The antiferromagnetic Heisenberg chain of spins-1/2 is an important reference system; its elementary excitations are spin-1/2 quasiparticles called spinons that are always created in pairs. However, while inelastic neutron scattering (INS) experiments routinely observe the excitation continuum associated with two-spinon states, the presence of more complex dynamics associated with four-spinon states has only been inferred from comparison with theory. Here, we show that resonant inelastic x-ray scattering (RIXS) is capable of accessing the four-spinon excitations directly, in a spectroscopic region separated from the two-spinon continuum. Our results provide the first direct measurement of four-spinon excitations, which is made possible by the fundamentally different correlation functions probed by RIXS compared to INS. This advance holds great promise as a tool in the search for novel quantum states, in particular quantum spin liquids.

The strongly correlated insulator Ca$_{2}$RuO$_4$ is considered as a paradigmatic realization of both spin-orbital physics and a band-Mott insulating phase, characterized by orbitally selective coexistence of a band and a Mott gap. We present a high-resolution oxygen $K$-edge resonant inelastic X-ray scattering study of the antiferromagnetic Mott insulating state of Ca$_{2}$RuO$_4$. A set of low-energy ($\sim$80 and 400 meV) and high-energy ($\sim$1.3 and 2.2 eV) excitations are reported that show strong incident light polarization dependence. Our results strongly support a spin-orbit coupled band-Mott scenario and explore in detail the nature of its exotic excitations. Guided by theoretical modelling, we interpret the low-energy excitations as a result of composite spin-orbital excitations. Their nature unveil the intricate interplay of crystal-field splitting and spin-orbit coupling in the band-Mott scenario. The high-energy excitations correspond to intra-atomic singlet-triplet transitions at an energy scale set by the Hund's coupling. Our findings give a unifying picture of the spin and orbital excitations in the band-Mott insulator Ca$_{2}$RuO$_4$., Comment: accepted for publication in Physical Review X

The antiferromagnetic compound Ba(TiO)Cu$_4$(PO$_4$)$_4$ contains square cupola of corner-sharing CuO$_4$ plaquettes, which were proposed to form effective quadrupolar order. To identify the magnetic structure, we have performed spherical neutron polarimetry measurements. Based on symmetry analysis and careful measurements we conclude that the orientation of the Cu$^{2+}$ spins form a non-collinear in-out structure with spins approximately perpendicular to the CuO$_4$ motif. Strong Dzyaloshinskii-Moriya interaction naturally lends itself to explain this phenomenon. The identification of the ground state magnetic structure should serve well for future theoretical and experimental studies into this and closely related compounds., Comment: 9 pages, 4 figures

We report that in a $\beta$-Mn-type chiral magnet Co$_9$Zn$_9$Mn$_2$, skyrmions are realized as a metastable state over a wide temperature range, including room temperature, via field-cooling through the thermodynamic equilibrium skyrmion phase that exists below a transition temperature $T_\mathrm{c}$ $\sim$ 400 K. The once-created metastable skyrmions survive at zero magnetic field both at and above room temperature. Such robust skyrmions in a wide temperature and magnetic field region demonstrate the key role of topology, and provide a significant step toward technological applications of skyrmions in bulk chiral magnets.

We use resonant inelastic x-ray scattering (RIXS) at the Cu L$_3$ edge to measure the charge and spin excitations in the "half-stuffed" Cu--O planes of the cuprate antiferromagnet Ba$_2$Cu$_3$O$_4$Cl$_2$. The RIXS line shape reveals distinct contributions to the $dd$ excitations from the two structurally inequivalent Cu sites, which have different out-of-plane coordinations. The low-energy response exhibits magnetic excitations. We find a spin-wave branch whose dispersion follows the symmetry of a CuO$_2$ sublattice, similar to the case of the "fully-stuffed" planes of tetragonal CuO (T-CuO). Its bandwidth is closer to that of a typical cuprate material, such as Sr$_2$CuO$_2$Cl$_2$, than it is to that of T-CuO. We interpret this result as arising from the absence of the effective four-spin inter-sublattice interactions that act to reduce the bandwidth in T-CuO., Comment: 10 pages, 8 figures

We demonstrate that light-induced heat pulses of different duration and energy can write skyrmions in a broad range of temperatures and magnetic field in FeGe. Using a combination of camera-rate and pump-probe cryo-Lorentz Transmission Electron Microscopy, we directly resolve the spatio-temporal evolution of the magnetization ensuing optical excitation. The skyrmion lattice was found to maintain its structural properties during the laser-induced demagnetization, and its recovery to the initial state happened in the sub-{\mu}s to {\mu}s range, depending on the cooling rate of the system.

A combined resistivity and hard x-ray diffraction study of superconductivity and charge ordering in $\mathrm{Ir_{1-x}Pt_xTe_2}$, as a function of Pt substitution and externally applied hydrostatic pressure, is presented. Experiments are focused on samples near the critical composition $x_c\sim 0.045$ where competition and switching between charge order and superconductivity is established. We show that charge order as a function of pressure in $\mathrm{Ir_{0.95}Pt_{0.05}Te_{2}}$ is preempted - and hence triggered - by a structural transition. Charge ordering appears uniaxially along the short crystallographic (1,0,1) domain axis with a $\mathrm{(\frac{1}{5},0,\frac{1}{5})}$ modulation. Based on these results we draw a charge-order phase diagram and discuss the relation between stripe ordering and superconductivity., Comment: 8 pages, 4 figures: Accepted in Scientific Reports

We report magnetic and thermodynamic properties of a $4d^1$ (Mo$^{5+}$) magnetic insulator MoOPO$_4$ single crystal, which realizes a $J_1$-$J_2$ Heisenberg spin-$1/2$ model on a stacked square lattice. The specific-heat measurements show a magnetic transition at 16 K which is also confirmed by magnetic susceptibility, ESR, and neutron diffraction measurements. Magnetic entropy deduced from the specific heat corresponds to a two-level degree of freedom per Mo$^{5+}$ ion, and the effective moment from the susceptibility corresponds to the spin-only value. Using {\it ab initio} quantum chemistry calculations we demonstrate that the Mo$^{5+}$ ion hosts a purely spin-$1/2$ magnetic moment, indicating negligible effects of spin-orbit interaction. The quenched orbital moments originate from the large displacement of Mo ions inside the MoO$_6$ octahedra along the apical direction. The ground state is shown by neutron diffraction to support a collinear N\'eel-type magnetic order, and a spin-flop transition is observed around an applied magnetic field of 3.5 T. The magnetic phase diagram is reproduced by a mean-field calculation assuming a small easy-axis anisotropy in the exchange interactions. Our results suggest $4d$ molybdates as an alternative playground to search for model quantum magnets., Comment: 9 pages, 7 figures

We report detailed neutron scattering studies on Ba$_2$Cu$_3$O$_4$Cl$_2$. The compound consists of two interpenetrating sublattices of Cu, labeled as Cu$_{\rm A}$ and Cu$_{\rm B}$, each of which forms a square-lattice Heisenberg antiferromagnet. The two sublattices order at different temperatures and effective exchange couplings within the sublattices differ by an order of magnitude. This yields an inelastic neutron spectrum of the Cu$_{\rm A}$ sublattice extending up to 300 meV and a much weaker dispersion of Cu$_{\rm B}$ going up to around 20 meV. Using a single-band Hubbard model we derive an effective spin Hamiltonian. From this, we find that linear spin-wave theory gives a good description to the magnetic spectrum. In addition, a magnetic field of 10 T is found to produce effects on the Cu$_{\rm B}$ dispersion that cannot be explained by conventional spin-wave theory., Comment: 13 pages, 9 figures

Magnetic skyrmions are topologically protected spin-whirl quasiparticles currently considered as promising components for ultra-dense memory devices. In the bulk they form lattices that are stable over just a few Kelvin below the ordering temperature. This narrow stability range presents a key challenge for applications, and finding ways to tune the SkL stability over a wider phase space is a pressing issue. Here we show experimentally that the skyrmion phase in the magnetoelectric insulator ${\text{Cu}_2 \text{O} \text{Se} \text{O}_3}$ can either expand or shrink substantially depending on the polarity of a moderate applied electric field. The data are well-described by an expanded mean-field model with fluctuations that show how the electric field provides a direct control of the free energy difference between the skyrmion and the surrounding conical phase. Our finding of the direct electric field control of the skyrmion phase stability offers enormous potential for skyrmionic applications based on a magnetoelectric coupling., Comment: 7 pages, 3 figures

A resonant inelastic x-ray scattering (RIXS) study of overdamped spin-excitations in slightly underdoped La$_{2-x}$Sr$_{x}$CuO$_4$ (LSCO) with $x=0.12$ and $0.145$ is presented. Three high-symmetry directions have been investigated: (1) the antinodal $(0,0)\rightarrow (1/2,0)$, (2) the nodal $(0,0)\rightarrow (1/4,1/4)$ and (3) the zone boundary direction $(1/2,0)\rightarrow (1/4,1/4)$ connecting these two. The overdamped excitations exhibit strong dispersions along (1) and (3), whereas a much more modest dispersion is found along (2). This is in strong contrast to the undoped compound La$_{2}$CuO$_4$ (LCO) for which the strongest dispersions are found along (1) and (2). The $t-t^{\prime}-t^{\prime\prime}-U$ Hubbard model used to explain the excitation spectrum of LCO predicts $-$ for constant $U/t$ $-$ that the dispersion along (3) scales with $(t^{\prime}/t)^2$. However, the diagonal hopping $t^{\prime}$ extracted on LSCO using single-band models is low ($t^{\prime}/t\sim-0.16$) and decreasing with doping. We therefore invoked a two-orbital ($d_{x^2-y^2}$ and $d_{z^2}$) model which implies that $t^{\prime}$ is enhanced. This effect acts to enhance the zone-boundary dispersion within the Hubbard model. We thus conclude that hybridization of $d_{x^2-y^2}$ and $d_{z^2}$ states has a significant impact on the zone-boundary dispersion in LSCO., Comment: 10 pages, 7 figures

We present a systematic study of the phase diagram of LiHo$_x$Y$_{1-x}$F$_4$ ($0.25

We report the structural and magnetic properties of the 4}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Rh) based and 5}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Ir) based systems Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ (nominally $x$ = 0.5, 1). The studied compositions were found to crystallize in a hexagonal structure with the centrosymmetric space group }$P6_{3}/mmc$.\textcolor{black}{{} The structures comprise of A$_{2}$O$_{9}$ polyhedra (with the A site (possibly) statistically occupied by M and Ti) in which pairs of transition metal ions are stacked along the crystallographic }\textit{\textcolor{black}{c}}\textcolor{black}{-axis. These pairs form triangular bilayers in the $ab$-plane. The magnetic Rh and Ir ions occupy these bilayers, diluted by Ti ions even for $x$ = 1. These bilayers are separated by a triangular layer which is dominantly occupied by Ti ions. From magnetization measurements we infer strong antiferromagnetic couplings for all of the materials but the absence of any spin-freezing or spin-ordering down to 2~K. Further, specific heat measurements down to 0.35~K show no sign of a phase transition for any of the compounds. Based on these thermodynamic measurements we propose the emergence of a quantum spin liquid ground state for Ba$_{3}$Rh$_{0.5}$Ti$_{2.5}$O$_{9}$, and Ba$_{3}$Ir$_{0.5}$Ti$_{2.5}$O$_{9}$, in addition to the already reported Ba$_{3}$IrTi$_{2}$O$_{9}$. }, Comment: 12 pages, 11 figures, accepted in Phys. Rev. B (regular article)

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu$_4$(PO$_4$)$_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements., Comment: 4 figures

A paradigmatic case of multi-band Mott physics including spin-orbit and Hund's coupling is realised in Ca$_2$RuO$_4$. Progress in understanding the nature of this Mott insulating phase has been impeded by the lack of knowledge about the low-energy electronic structure. Here we provide -- using angle-resolved photoemission electron spectroscopy -- the band structure of the paramagnetic insulating phase of Ca$_2$RuO$_4$ and show how it features several distinct energy scales. Comparison to a simple analysis of atomic multiplets provides a quantitative estimate of the Hund's coupling $J=0.4$ eV. Furthermore, the experimental spectra are in good agreement with electronic structure calculations performed with Dynamical Mean-Field Theory. The crystal field stabilisation of the d$_{xy}$ orbital due to $c$-axis contraction is shown to be important in explaining the nature of the insulating state. It is thus a combination of multiband physics, Coulomb interaction and Hund's coupling that generates the Mott insulating state of Ca$_2$RuO$_4$. These results underscore the importance of Hund's coupling in the ruthenates and related multiband materials.

We have used inelastic neutron scattering to measure the magnetic excitation spectrum along the high-symmetry directions of the first Brillouin zone of the magnetic skyrmion hosting compound Cu$_2$OSeO$_3$. The majority of our scattering data are consistent with the expectations of a recently proposed model for the magnetic excitations in Cu$_2$OSeO$_3$, and we report best-fit parameters for the dominant exchange interactions. Important differences exist, however, between our experimental findings and the model expectations. These include the identification of two energy scales that likely arise due to neglected anisotropic interactions. This feature of our work suggests that anisotropy should be considered in future theoretical work aimed at the full microscopic understanding of the emergence of the skyrmion state in this material., Comment: 5 pages, 6 figures

We report the synthesis of single crystals of a novel layered iridate Ba$_{21}$Ir$_9$O$_{43}$, and present the crystallographic, transport and magnetic properties of this material. The compound has a hexagonal structure with two iridium oxide layers stacked along the $c$ direction. One layer consists of a triangular arrangement of Ir$_2$O$_9$ dimers while the other layer comprises two regular octahedra and one triangular pyramid, forming inter-penetrated triangular lattices. The resistivity as a function of temperature exhibits an insulating behavior, with a peculiar $T^{-3}$ behavior. Magnetic susceptibility shows antiferromagnetic Curie-Weiss behavior with $\Theta_\mathrm{CW} \simeq -$90 K while a magnetic transition occurs at substantially lower temperature of 9 K. We discuss possible valence states and effective magnetic moments on Ir ions in different local environments, and argue that the Ir ions in a unique triangular-pyramidal configuration likely carry unusually large magnetic moments., Comment: 5 pages, 3 figures

We present direct local-probe evidence for strongly hybridized nuclear-electronic spin states of an Ising ferromagnet LiHoF$_4$ in a transverse magnetic field. The nuclear-electronic states are addressed via a magnetic resonance in the GHz frequency range using coplanar resonators and a vector network analyzer. The magnetic resonance spectrum is successfully traced over the entire field-temperature phase diagram, which is remarkably well reproduced by mean-field calculations. Our method can be directly applied to a broad class of materials containing rare-earth ions for probing the substantially mixed nature of the nuclear and electronic moments., Comment: 6 pages, 5 figures

Skyrmions, topologically-protected nanometric spin vortices, are being investigated extensively in various magnets. Among them, many of structurally-chiral cubic magnets host the triangular-lattice skyrmion crystal (SkX) as the thermodynamic equilibrium state. However, this state exists only in a narrow temperature and magnetic-field region just below the magnetic transition temperature $T_\mathrm{c}$, while a helical or conical magnetic state prevails at lower temperatures. Here we describe that for a room-temperature skyrmion material, $\beta$-Mn-type Co$_8$Zn$_8$Mn$_4$, a field-cooling via the equilibrium SkX state can suppress the transition to the helical or conical state, instead realizing robust metastable SkX states that survive over a very wide temperature and magnetic-field region, including down to zero temperature and up to the critical magnetic field of the ferromagnetic transition. Furthermore, the lattice form of the metastable SkX is found to undergo reversible transitions between a conventional triangular lattice and a novel square lattice upon varying the temperature and magnetic field. These findings exemplify the topological robustness of the once-created skyrmions, and establish metastable skyrmion phases as a fertile ground for technological applications.

Sr$_2$CuTeO$_6$ presents an opportunity for exploring low-dimensional magnetism on a square lattice of $S=1/2$ Cu$^{2+}$ ions. We employ ab initio multi-reference configuration interaction calculations to unravel the Cu$^{2+}$ electronic structure and to evaluate exchange interactions in Sr$_2$CuTeO$_6$. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr$_2$CuTeO$_6$ is an almost realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV., Comment: 10 pages, 7 figures

We report ac susceptibility, specific heat, and neutron scattering measurements on a dipolar-coupled antiferromagnet LiYbF$_4$. For the thermal transition, the order-parameter critical exponent is found to be 0.20(1) and the specific-heat critical exponent -0.25(1). The exponents agree with the 2D XY/h$_4$ universality class despite the lack of apparent two-dimensionality in the structure. The order-parameter exponent for the quantum phase transitions is found to be 0.35(1) corresponding to (2+1)D. These results are in line with those found for LiErF$_4$ which has the same crystal structure, but largely different T$_N$, crystal field environment and hyperfine interactions. Our results therefore experimentally establish that the dimensional reduction is universal to quantum dipolar antiferromagnets on a distorted diamond lattice., Comment: 9 pages, 7 figures

The heavy fermion compound Ce$_{3}$Pd$_{20}$Si$_{6}$ displays unconventional quantum criticality as the lower of two consecutive phase transitions is fully suppressed by magnetic field. Here we report on the effects of pressure as additional tuning parameter. Specific heat and electrical resistivity measurements reveal a converse effect of pressure on the two transitions, leading to the merging of both transitions at 6.2 kbar. The field-induced quantum criticality is robust under pressure tuning. We rationalize our findings within an extended version of the global phase diagram for antiferromagnetic heavy fermion quantum criticality., Comment: accepted for publication in Phys. Rev. B

The recent discovery of magnetic skyrmion lattices initiated a surge of interest in the scientific community. Several novel phenomena have been shown to emerge from the interaction of conducting electrons with the skyrmion lattice, such as a topological Hall-effect and a spin-transfer torque at ultra-low current densities. In the insulating compound Cu2OSeO3, magneto-electric coupling enables control of the skyrmion lattice via electric fields, promising a dissipation-less route towards novel spintronic devices. One of the outstanding fundamental issues is related to the thermodynamic stability of the skyrmion lattice. To date, the skyrmion lattice in bulk materials has been found only in a narrow temperature region just below the order-disorder transition. If this narrow stability is unavoidable, it would severely limit applications. Here we present the discovery that applying just moderate pressure on Cu2OSeO3 substantially increases the absolute size of the skyrmion pocket. This insight demonstrates directly that tuning the electronic structure can lead to a significant enhancement of the skyrmion lattice stability. We interpret the discovery by extending the previously employed Ginzburg-Landau approach and conclude that change in the anisotropy is the main driver for control of the size of the skyrmion pocket. This realization provides an important guide for tuning the properties of future skyrmion hosting materials., Comment: submitted to Scientific Reports