Institut Laue-Langevin
The effective electron neutrino mass can be determined by analyzing the endpoint region of the 163^{163}Ho electron capture spectrum, provided a measurement with high energy resolution and high statistics using calorimetric techniques. Here, the Electron Capture in 163^{163}Ho collaboration, ECHo, presents an analysis of the most precise 163^{163}Ho spectrum currently available, obtained with the ECHo-1k experiment and comprising about 200 million events. A very low background rate of B=9.1(1.3)×106B=9.1(1.3)\times 10^{-6} /eV/pixel/day was achieved allowing for a reliable analysis of the endpoint region. The derived endpoint energy Q=2862(4)Q = 2862(4) eV is in excellent agreement with the one independently determined via Penning-trap mass spectrometry of Q=2863.2(6)Q=2863.2(6) eV [1]. The upper limit of the effective electron neutrino mass is improved by almost a factor 2 compared to the lowest current value [2], reaching m_{\nu_\mathrm{e}} < 15 eV/c2{^2} (90\% credible interval).
Discrepancies between theory and recent qBounce data have prompted renewed scrutiny of how boundary conditions are implemented for ultracold neutrons bouncing above a mirror in Earth's gravity. We apply the theory of self-adjoint extensions to the linear gravitational potential on the half-line and derive the most general boundary condition that renders the Hamiltonian self-adjoint. This introduces a single real self-adjoint parameter λ\lambda that continuously interpolates between the Dirichlet case and more general (Robin-type) reflecting surfaces. Building on this framework, we provide analytical expressions for the energy spectrum, eigenfunctions, relevant matrix elements, and a set of sum rules valid for arbitrary λ\lambda. We show how nontrivial boundary conditions can bias measurements of gg and can mimic or mask putative short-range ''fifth-force''. Our results emphasize that enforcing self-adjointness-and modeling the correct boundary physics-is essential for quantitative predictions in gravitational quantum states. Beyond neutron quantum bounces, the approach is broadly applicable to systems where boundaries and self-adjointness govern the observable spectra and dynamics.
We present the result of an experiment to measure the electric dipole moment (EDM) of the neutron at the Paul Scherrer Institute using Ramsey's method of separated oscillating magnetic fields with ultracold neutrons (UCN). Our measurement stands in the long history of EDM experiments probing physics violating time reversal invariance. The salient features of this experiment were the use of a Hg-199 co-magnetometer and an array of optically pumped cesium vapor magnetometers to cancel and correct for magnetic field changes. The statistical analysis was performed on blinded datasets by two separate groups while the estimation of systematic effects profited from an unprecedented knowledge of the magnetic field. The measured value of the neutron EDM is dn=(0.0±1.1stat±0.2sys)×1026ecmd_{\rm n} = (0.0\pm1.1_{\rm stat}\pm0.2_{\rm sys})\times10^{-26}e\,{\rm cm}.
Spin-nematic and spin-smectic phases have been reported in magnetic materials, which break rotational symmetry while preserving translational symmetry along certain directions. However, until now the analogy to liquid crystals remained incomplete because no magnetic analog of cholesteric order was known. Here we show that the bilayer perovskite Sr3_3Fe2_2O7_7, previously believed to adopt a simple single-q\mathbf{q} spin-helical order, hosts two distinct types of multi-q\mathbf{q} spin textures and the first "spin-cholesteric". Its ground state represents a novel multi-q\mathbf{q} spin texture with unequally intense spin modulations at the two ordering vectors. This is followed in temperature by the new "spin-cholesteric" phase with spontaneously broken chiral symmetry, in which the translational symmetry is broken only along one of the crystal directions while the weaker orthogonal modulation melts, giving rise to intense short-range dynamical fluctuations. Shortly before the transition to the paramagnetic state, vortex-crystal order spanned by two equivalent q\mathbf{q} vectors emerges. The "spin-cholesteric" phase completes the spin analogy with liquid crystals and renders Sr3_3Fe2_2O7_7 a touchstone for studying transitions among multiple-q\mathbf{q} spin textures in a centrosymmetric host.
Disorder in frustrated quantum systems can critically influence their magnetic ground states and drive exotic correlated behavior. In the S=12S = \frac{1}{2} system ktenasite, Cu2.7_\text{2.7}Zn2.3_\text{2.3}(SO4_\text{4})2_\text{2}(OH)6_\text{6}\cdot6H2_\text{2}O, we show that structural disorder drives an unexpected dimensional crossover and stabilizes a rare coexistence of distinct magnetic states. Neutron diffraction reveals significant Cu/Zn mixing at the Cu2 site, which tunes the Cu2+^{2+} sublattice from a two-dimensional scalene-distorted triangular lattice into a one-dimensional spin-chain network. Magnetic susceptibility, neutron diffraction, ac susceptibility, and specific heat measurements collectively indicate magnetic duality: a coexistence of incommensurate long-range magnetic order below TN=4T_\text{N} = 4\,K and a cluster spin-glass state with Tf=3.28T_\text{f} = 3.28\,K at ν=10\nu = 10\,Hz. Our findings highlight ktenasite as a rare platform where structural disorder tunes the effective dimensionality and stabilizes coexisting ordered and glassy magnetic phases, offering a unique opportunity to explore the interplay of frustration, disorder, and dimensional crossover in quantum magnets.
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 (CD3_3ND3_3)2_2NaRuCl6_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 Hc\mathbf{H \parallel c} and propose a minimal model Hamiltonian. (CD3_3ND3_3)2_2NaRuCl6_6 displays an ideal triangular arrangement of Ru3+^{3+} ions adopting the spin-orbital entangled jeff=1/2j_{\rm eff} = 1/2 state. It hosts residual magnetic order below TN=0.23T_{\rm N} = 0.23 K and a highly unusual HTH-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. 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 JJJ-J' isosceles distortion driven by pseudospin-lattice coupling. We argue that the multi-q\mathbf{q} ground state in zero magnetic field is a prime candidate for hosting the Z2\mathbb{Z}_2 vortex crystal proposed on the triangular Heisenberg-Kitaev model. (CD3_3ND3_3)2_2NaRuCl6_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.
The Raman scattering response of the biaxial antiferromagnet CoPS3_3 has been investigated as a function of both magnetic field and temperature. The peaks observed in the low-frequency spectral range (90--200~cm1^{-1}) have been identified as hybrid magnon--phonon excitations. The energies of the bare magnon and phonon modes, as well as the effective coupling strengths between different excitation pairs, have been determined. The strong and selective magnon--phonon interaction largely accounts for the pronounced splitting of two phonon-like modes observed at 152~cm1^{-1} and 158~cm1^{-1} in the antiferromagnetic phase of CoPS3_3. Based on the identification of bare magnon excitations and their magnetic-field dependence, we propose an updated set of parameters for the effective exchange (Jeff=9.9J_{\mathrm{eff}} = 9.9~meV) and biaxial magnetic anisotropy (D=4.3D = 4.3~meV and E=0.7E = -0.7~meV) and advocate for an apparent anisotropic gg-factor (gx=gy=2g_x = g_y = 2, gz=4g_z = 4) in the CoPS3_3 antiferromagnet.
High-resolution neutron spectroscopy on Ce2_2Hf2_2O7_7 reveals a correlated state characterized by distinct dipolar scattering signals -- quasi-elastic and inelastic contributions consistent with `photon' and `spinon' excitations in quantum spin ice. These signals coexist with weak octupolar scattering. Fits of thermodynamic data using numerical methods indicate a dominant octupolar exchange, JxJ_{x} or JyJ_{y}, with substantial dipolar JzJ_{z} and minute dipole-octupole JxzJ_{xz} couplings. The JxzJ_{xz} value is corroborated by an independent fit of the neutron scattering amplitude balance between dipolar and octupolar `photon' contributions, highlighting its importance to understand neutron scattering results in this family. Ce2_2Hf2_2O7_7 enriches the landscape of dipole-octupole pyrochlore physics, and reveals a `quantum multipolar liquid' where hybrid correlations involve multiple terms in moment series expansion, opening questions on their intertwining and hierarchy in quantum phases.
Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discovered subterahertz collective modes, dubbed 'skyrons', which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. Momentum-resolved time-domain measurements of diffuse scattering revealed an avoided crossing in the dispersion relation of skyrons. We further demonstrated that the amplitude and dispersion of skyrons can be controlled by sample temperature and electric-field bias. Atomistic simulations and dynamical phase-field modeling provided microscopic insights into the three-dimensional crystallographic and polarization dynamics. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.
Interfacial interactions significantly alter the fundamental properties of water confined in mesoporous structures, with crucial implications for geological, physicochemical, and biological processes. Herein, we focused on the effect of changing the surface ionic charge of nanopores with comparable pore size (3.5-3.8 nm) on the dynamics of confined liquid water. The control of the pore surface ionicity was achieved by using two periodic mesoporous organosilicas (PMOs) containing either neutral or charged forms of a chemically similar bridging unit. The effect on the dynamics of water at the nanoscale was investigated in the temperature range of 245 -300 K, encompassing the glass transition by incoherent quasielastic neutron scattering (QENS), For both types of PMOs, the water dynamics revealed two distinct types of molecular motions: rapid local movements and translational jump diffusion. While the neutral PMO induces a moderate confinement effect, we show that the charged PMO drastically slows down water dynamics, reducing translational diffusion by a factor of four and increasing residence time by an order of magnitude. Notably, by changing the pore filling values, we demonstrate that for charged pore this effect extends beyond the interfacial layer of surface-bound water molecules to encompass the entire pore volume. Thus, our observation indicates a dramatic change in the long-range character of the interaction of water confined in nanopores with surface ionic charge compared to a simple change in hydrophilicity. This is relevant for the understanding of a broad variety of applications in (nano)technological phenomena and processes, such as nanofiltration and membrane design.
Structural and magnetic chiralities are found to coexist in a small group of materials in which they produce intriguing phenomenologies such as the recently discovered skyrmion phases. Here, we describe a previously unknown manifestation of this interplay in MnSb2O6, a trigonal oxide with a chiral crystal structure. Unlike all other known cases, the MnSb2O6 magnetic structure is based on co-rotating cycloids rather than helices. The coupling to the structural chirality is provided by a magnetic axial vector, related to the so-called vector chirality. We show that this unique arrangement is the magnetic ground state of the symmetric-exchange Hamiltonian, based on ab-initio theoretical calculations of the Heisenberg exchange interactions, and is stabilised by out-of-plane anisotropy. MnSb2O6 is predicted to be multiferroic with a unique ferroelectric switching mechanism.
The Ricochet experiment aims to measure the coherent elastic neutrino-nucleus scattering process from antineutrinos emitted by a research nuclear reactor operated by the Institut Laue-Langevin (Grenoble, France). This article presents a description of the Ricochet experimental installation and the detector performance achieved during its commissioning with a mini-CryoCube module consisting of three 42-gram germanium cryogenic calorimeters. The baseline resolutions and background levels are reported both during reactor-on and reactor-off periods, and as noise mitigation techniques were improved. A baseline resolution of 40 eV electron equivalent was achieved for the ionization channel after setup improvements, and the phonon channel resolutions ranged from 50 to 80 eV of total phonon energy. In the energy region from 2 to 7 keV, a nuclear recoil rate of 15(2) events/(kg day keV) is measured during the reactor-off period selecting events in coincidence with muon veto signals. This rate is in agreement with the cosmogenic neutron rate calculated from GEANT4 simulations. After the rejection of events in coincidence with signals in the muon veto detectors, a combined 90% C.L. limit on the nuclear recoil background of < 9 events/(kg day keV) is obtained in that energy region during the reactor-on period, which is compatible with our GEANT4 model calculation corresponding to a total rate of 5 events/(kg day keV). The sensitivity of this analysis was however found to be limited by a surface event contamination which is currently being addressed by the Ricochet Collaboration with upgraded detectors.
Longitudinal magnons are a novel class of multipolar quantum excitations in magnetic materials with large spins S1S\ge 1 and strong easy-axis anisotropy. These excitations have angular momentum Sz=±2SS^z = \pm 2S and can be viewed as propagating spin reversals. We study a simple model for longitudinal magnons: a square lattice of spins SS coupled by the neareast-neighbor exchange, ferro- or antiferromagnetic, in the presence of a single-ion anisotropy. We calculate the excitation spectra in the large-DD limit by using a strong-coupling expansion. In the specific case of S=1S=1 we compare the results for several analytical approaches that include the linked-cluster expansion, the multiboson representation of spin operators, and also, for a ferromagnetic ground state, the exact solution of the two-particle bound states. Among these different approaches, the multiboson theory gives the decay rate of longitudinal magnons and describes the evolution of the excitation spectra from strong to moderate and weak anisotropy.
RuO2_2 was considered for a long time to be a paramagnetic metal with an ideal rutile-type structure down to low temperatures, but recent studies on single-crystals claimed evidence for antiferromagnetic order and some symmetry breaking in the crystal structure. We have grown single-crystals of RuO2 by vapor transport using either O2_2 or TeCl4_4 as transport medium. These crystals exhibit metallic behavior following a T2T^2 low-temperature relation and a small paramagnetic susceptibility that can be attributed to Pauli paramagnetism. Neither the conductance nor the susceptibility measurements yield any evidence for a magnetic or a structural transition between 300K and \sim4 K. Comprehensive single-crystal diffraction studies with neutron and X-ray radiation reveal the rutile structure to persist until 2K in our crystals, and show nearly perfect stoichiometry. Previous observations of symmetry forbidden reflections can be attributed to multiple diffraction. Polarized single-crystal neutron diffraction experiments at 1.6K exclude the proposed antiferromagnetic structures with ordered moments larger than 0.01 Bohr magnetons.
Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce2_2Hf2_2O7_7 down to a temperature of T=0.02T = 0.02 K are reported. These show a two-peaked structure, with a Schottky-like peak at T10.065T_1 \sim 0.065 K, similar to what is observed in its sister Ce-pyrochlores Ce2_2Zr2_2O7_7 and Ce2_2Sn2_2O7_7. However, a second sharper peak is observed at T20.025T_2 \sim 0.025 K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to CP=0C_P=0 at T=0T = 0 K fully accounts for the Rln(2)R\ln(2) entropy associated with the pseudospin-1/2 doublet for Ce3+^{3+} in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in CPC_P at much higher temperatures than the measured T2T_2 for expectations from an all-in all-out ground state of the XYZ Hamiltonian for Ce2_2Hf2_2O7_7. The sharp low-temperature peak could also signify a cross-over from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured CPC_P with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below T0.25T \sim 0.25 K. The diffuse magnetic neutron scattering observed from Ce2_2Hf2_2O7_7 at low temperatures between T2T_2 and T1T_1 resembles that observed from Ce2_2Zr2_2O7_7, which is well established as a π\pi-flux quantum spin ice (QSI). Together with the peak in the heat capacity at T2T_2, this diffuse scattering from Ce2_2Hf2_2O7_7 is suggestive of a classical spin liquid regime above T2T_2 that is distinct from the zero-entropy quantum ground state below T2T_2.
The frustrated magnet Bi2Fe4O9 has been reported to exhibit complex spin dynamics coexisting with conventional spin wave excitations. The magnetic Fe3+ (S = 5/2) ions are arranged into a distorted two-dimensional Cairo pentagonal lattice with weak couplings between the layers, developing long-ranged non-collinear antiferromagnetic order below 245 K. In order to enable studies and modelling of the complex dynamics close to TN, we have reexamined the magnetic excitations across the complete energy scale (0 < E < 90 meV) at 10 K. We discover two distinct gaps, which can be explained by introducing, respectively, easy axis and easy plane anisotropy on the two unequivalent Fe-sites. We develop a refined spin Hamiltonian that accurately accounts for the dispersion of essentially all spin-wave branches across the full spectral range, except around 40 meV, where a splitting and dispersion are observed. We propose that this mode is derived from phonon hybridization. Polarisation analysis shows that the system has magnetic anisotropic fluctuations, consistent with our model. A continuum of scattering is observed above the spin wave branches and is found to principally be explained by an instrumental resolution effect. The full experimental mapping of the excitation spectrum and the refined spin Hamiltonian provides a foundation for future quantitative studies of spin waves coexisting with unconventional magnetic fluctuations in this frustrated magnet found at higher temperatures.
A strange metal is an exotic state of correlated quantum matter; intensive efforts are ongoing to decipher its nature. Here we explore whether the quantum Fisher information (QFI), a concept from quantum metrology, can provide new insight. We use inelastic neutron scattering and quantum Monte Carlo simulations to study a Kondo destruction quantum critical point, where strange metallicity is associated with fluctuations beyond a Landau order parameter. We find that the QFI probed away from magnetic Bragg peaks, where the effect of magnetic ordering is minimized, increases strongly and without a characteristic scale as the strange metal forms with decreasing temperature, evidencing its unusual entanglement properties. Our work opens a new direction for studies across strange metal platforms.
Co2+^{2+} ions in an octahedral crystal field, stabilise a jeff_{eff} = 1/2 ground state with an orbital degree of freedom and have been recently put forward for realising Kitaev interactions, a prediction we have tested by investigating spin dynamics in two cobalt honeycomb lattice compounds, Na2_2Co2_2TeO6_6 and Na3_3Co2_2SbO6_6, using inelastic neutron scattering. We used linear spin wave theory to show that the magnetic spectra can be reproduced with a spin Hamiltonian including a dominant Kitaev nearest-neighbour interaction, weaker Heisenberg interactions up to the third neighbour and bond-dependent off-diagonal exchange interactions. Beyond the Kitaev interaction that alone would induce a quantum spin liquid state, the presence of these additional couplings is responsible for the zigzag-type long-range magnetic ordering observed at low temperature in both compounds. These results provide evidence for the realization of Kitaev-type coupling in cobalt-based materials, despite hosting a weaker spin-orbit coupling than their 4d and 5d counterparts.
Vacancy defects in isotropic noncollinear antiferromagnets produce long-range spin textures. By developing a "magnetic elasticity theory", we demonstrate that a vacancy-induced readjustment in the spin configuration decays algebraically with distance. The power law exponent depends on the multipole moment of a local spin deformation, which in turn is determined by the lattice symmetry and an equilibrium spin configuration in the absence of defects. The role of these two factors is highlighted for the J1-J2 Heisenberg model on a kagome lattice. A vacancy in this model generates spin deformations that decay as 1/r^2 for the q=0 ground state and as a 1/r for the sqrt{3} x sqrt{3} magnetic structure. The analytic conclusions are confirmed by extensive numerical simulations. We also compute the fractional magnetic moments associated with vacancies and other lattice defects. Our results shed light on relative fragility of different magnetic structures with respect to spin glass formation at higher doping levels.
Quantum magnetic materials can provide explicit realizations of paradigm models in quantum many-body physics. In this context, SrCu2_2(BO3_3)2_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 SrCu2_2(BO3_3)2_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 Jc=0.053(3)J_c = 0.053(3) meV. The presence of JcJ_c indicates the need to account for the three-dimensional nature of SrCu2_2(BO3_3)2_2 in theoretical models, also at lower pressures. We find that the ratio between in-plane interactions, J/J=1.8(2)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, JJ. Our results underline the wide horizons opened by high-pressure INS experiments on quantum magnetic materials.
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