Perovskite manganites are quantum materials exhibiting competing interactions inducing colossal magnetoresistance (CMR). The prevailing theory of CMR highlights the essential role of electron-phonon coupling (EPC), but mounting evidence suggests the underlying mechanism is more complicated. Here, we investigate phonons and spin-phonon coupling in ferromagnetic CMR manganites La_1-xSr_xMnO_3 (x=0.2,0.3) with relatively small CMR associated with melting of the magnetic order above room temperature. High-resolution neutron scattering experiments combined with density functional theory (DFT) show that the low-temperature ferromagnetic phase is conventional: neutron scattering from phonons agrees with DFT predictions and magnons follow sinusoidal dispersions. Fluctuating magnetic moments and low-energy phonons remain conventional in the high temperature paramagnetic phase, indicating the Mn and La/Sr sublattices are not strongly perturbed by melting of ferromagnetism. In contrast, the Jahn-Teller-active optical oxygen vibrations collapse entirely above the Curie temperature, despite low CMR in these compositions, with some of the lost spectral weight reappearing as quasielastic scattering. We attribute this highly anomalous behavior to giant EPC in the charge and/or orbital channel. It drives cooperative diffusive motion of quasistatic carrier-trapping oxygen sublattice distortions once ferromagnetism disappears. We hypothesize the magnitude of magnetoresistance correlates with the rate of diffusion rather than with the strength of Jahn-Teller EPC.
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 noncollinear antiferromagnetic order below 245 K. In order to enable studies and modeling of the complex dynamics close to TN, we have reexamined the magnetic excitations across the complete energy scale (0 < homega < 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. Polarization 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.
As a nontrivial state of solid, Schwarz crystal manifests itself in extremely refined nanograins and triply periodic minimal surface (TPMS) grain boundaries, and therefore exceptional thermal and mechanical stability. However, it remains unexploited how the structural units interact and thermal transport is influenced by such complex atomic structures. Here, we investigate Schwarz crystals of Cu and Pt using neutron scattering and thermal transport measurements. Pair distribution function analysis reveals the coexistence of compressed grains and expanded TPMS grain-boundary regions, forming a spatially confined atomic environment. This leads to an unusual phonon hardening suggested by inelastic neutron scattering. As bulk materials, Schwarz crystals exhibit a quasilinear temperature dependence of thermal conductivity, which was previously only observed in low-dimensional materials. This contrast indicates that the spatial confinement of the Schwarz crystals plays a crucial role in determining the unique thermal conductivity, which also provides an emergent route to regulate thermal properties in bulk materials.
Lattice vibrations can carry angular momentum and magnetic moments under broken inversion or time-reversal symmetry, forming so-called chiral phonons. While such excitations have been explored in nonmagnetic systems via optical probes, their direct detection in magnetic materials and coupling to spin excitations remain largely unexplored. Here, using neutron spectroscopy, sensitive to both nuclear and magnetic scattering, we reveal the magnetic signature of chiral phonons in ferrimagnetic Fe_{1.75}Zn_{0.25}Mo_{3}O_{8} with Curie temperature T_{C}∼49 K. Below T_{C}, we observe enhanced magnetic scattering of phonons at small momenta, arising from strong magnon-phonon coupling. In addition, out-of-plane intensity modulation, phonon mode splitting, and field-induced Zeeman shifts are observed, all closely associated with the ferrimagnetic order. These features vanish above T_{C}, where phonon spectra are dominated by nuclear scattering. These observations demonstrate the existence of chiral phonons carrying substantial magnetic moments that directly contribute to magnetic scattering, and establish neutron spectroscopy as a powerful, momentum-resolved probe of their magnetic character.
CoxTaS2 (x approximate to 1/3) exhibits a spontaneous Hall effect from spin texture in antiferromagnets, with a tetrahedral triple-Q(3Q) order and uniform spin scalar chirality. Upon Co overdoping (x> 1/3), it undergoes a shift in magnetic ordering vectors from Q(m) = (1/2, 0, 0) to (1/3, 0, 0). Interestingly, the spontaneous Hall effect disappeared in the overdoped regime, which was originally attributed to the loss of 3Q order. However, a question remains whether a new type of 3Q order can exist with alternating chirality in the overdoped regime. To address this, we investigated Co0.336TaS2 using inelastic neutron scattering (INS), neutron diffraction, and optical dichroism, and found that INS data and spin-wave simulations support a 3Q order with alternating chirality. Moreover, neutron diffraction data show field-independent Bragg peaks, while linear dichroism detects no in-plane anisotropy, consistent with threefold rotation symmetry. Our data support the scenario of an alternating-chirality 3Q order in Co0.336TaS2, canceling the spontaneous Hall effect. This study highlights a combined neutron-optical approach to identify complex spin textures.
Perovskite manganites are quantum materials exhibiting competing interactions inducing colossal magnetoresistance (CMR). The prevailing theory of CMR highlights the essential role of electron-phonon coupling (EPC), but mounting evidence suggests the underlying mechanism is more complicated. Here, we investigate phonons and spin-phonon coupling in ferromagnetic CMR manganites La1-xSrxMnO3 (x=0.2,0.3) with relatively small CMR associated with melting of the magnetic order above room temperature. High-resolution neutron scattering experiments combined with density functional theory (DFT) show that the low-temperature ferromagnetic phase is conventional: neutron scattering from phonons agrees with DFT predictions and magnons follow sinusoidal dispersions. Fluctuating magnetic moments and low-energy phonons remain conventional in the high-temperature paramagnetic phase, indicating the Mn and La/Sr sublattices are not strongly perturbed by melting of ferromagnetism. In contrast, the Jahn-Teller-active optical oxygen vibrations collapse entirely above the Curie temperature, despite low CMR in these compositions, with some of the lost spectral weight reappearing as quasielastic scattering. We attribute this highly anomalous behavior to giant EPC in the charge and/or orbital channel. It drives cooperative diffusive motion of quasistatic carrier-trapping oxygen sublattice distortions once ferromagnetism disappears. We hypothesize the magnitude of magnetoresistance correlates with the rate of diffusion rather than with the strength of Jahn-Teller EPC.
We present a combined experimental and theoretical investigation of the spin dynamics in the iron-based superconductor Ba0.75K0.25Fe2As2. Time-of-flight inelastic neutron scattering measurements reveal the threedimensional (3D) nature of the spin fluctuations, manifested as out-of-plane modulations of the low-energy magnetic intensity. As the energy increases, this 3D-like modulation gradually fades away, leading to a more two-dimensional (2D) profile-a clear signature of a 3D-to-2D crossover in the spin dynamics. By incorporating a realistic 3D electronic band structure derived from density functional theory (DFT), we reproduce the experimentally observed features of the spin susceptibility, including the pronounced out-of-plane modulation at low energies and its gradual evolution into a more 2D character at higher energies. The calculated susceptibility exhibits a peak at the experimental ordering wave vector qAFM= (0.5, 0.5, 1), demonstrating that the DFT-derived 3D model accurately captures the tendency toward out-of-plane antiferromagnetic (AFM) order. Notably, electronic states away from the Fermi level play a crucial role in shaping the susceptibility peak at qAFM, highlighting the limitations of the Fermi surface nesting picture in explaining the out-of-plane AFM instability. The demonstrated agreement between experiment and theory serves as a benchmark for validating the DFT-derived model as a realistic description of the material-specific electronic structure.
Two-dimensional hybrid organic-inorganic perovskites (HOIPs) have emerged as promising materials for light-emitting diode applications. In this study, by using time-of-flight neutron spectroscopy we identified and quantitatively separated the lattice vibrational and molecular rotational dynamics of two perovskites, butylammonium lead iodide (BA)$_{2}$PbI$_{4}$ and phenethyl-ammonium lead iodide (PEA)$_{2}$PbI$_{4}$. By examining the corresponding temperature dependence, we found that the lattice vibrations, as evidenced by neutron spectra, are consistent with the lattice dynamics obtained from Raman scattering. We revealed that the rotational dynamics of organic molecules in these materials tend to suppress their photoluminescence quantum yield (PLQY) while the vibrational dynamics did not show predominant correlations with the same. Additionally, we observed photoluminescence emission peak splitting for both systems, which becomes prominent above certain critical temperatures where the suppression of PLQY begins. This study suggests that the rotational motions of polarized molecules may lead to a reduction in exciton binding energy or the breaking of degeneracy in exciton binding energy levels, enhancing non-radiative recombination rates, and consequently reducing photoluminescence yield. These findings offer a deeper understanding of fundamental interactions in 2D HOIPs and could guide the design of more efficient light-emitting materials for advanced technological applications.
The pursuit of quantum spin liquid (QSL) states in condensed matter physics has drawn attention to kagome antiferromagnets (AFM) where a two-dimensional corner-sharing network of triangles frustrates conventional magnetic orders. While quantum kagome AFMs based on Cu2+ (3d9, s = ½) ions have been extensively studied, there is so far little work beyond copper-based systems. Here we present our bulk magnetization, specific heat and neutron scattering studies on single crystals of a new titanium fluorides Cs8RbK3Ti12F48 where Ti3+ (3d1, s = ½) ions form a modulated quantum kagome antiferromagnet that does not order magnetically down to 1.5 K. Our comprehensive map of the dynamic response function S ( Q , ℏ ω ) acquired at 1.5 K where the heat capacity is T-linear reveals a dispersive continuum emanating from soft lines that extend along (100). The data indicate fractionalized spinon-like excitations with quasi-one-dimensional dispersion within a quasi-two-dimensional spin system.
Fractionalized quasiparticles and their confinement into emergent bound states lie at the heart of modern quantum magnetism. While the evolution into magnonic bound states has been well characterized, experimental insight into the analogous transition to triplons remains limited. Here, using high-resolution neutron spectroscopy and state-of-the-art spin dynamics simulations, we uncover the transformation from weakly interacting spinons to tightly bound triplons in the spin-Peierls compound CuGeO3. Quantitative comparisons between the measured spectra and tensor network simulations reveal substantial next-nearest-neighbor frustration and weak external dimerization, placing the system deep within the spontaneously dimerized regime and near the exactly solvable Majumdar-Ghosh point. We further show an energy- and temperature-dependent evolution between two contrasting quasiparticle regimes: deconfined spinons with markedly suppressed interactions by frustration, and coherent triplonic bound states with no observable spinon degrees of freedom. Remarkably, triplon character persists into the two-particle regime, forming a structured two-triplon continuum with a spectral feature associated with a van Hove singularity at its lower boundary. These findings challenge the conventional view that robust triplons require strong external dimerization and demonstrate how the interplay between frustration and dimerization can reshape fractionalization and confinement.
Magnetic orders of non-Heisenberg Tsai-type 1/1 approximant crystals (ACs) in the Au-Ga-Dy system were studied through bulk magnetization, neutron diffraction, and inelastic neutron scattering techniques. The results uncovered noncoplanar, ferromagnetic (FM) and antiferromagnetic (AFM) spin configurations whirling along [111] crystallographic axis, which is analogous to those observed in the Tb- and Ho-contained counterparts. The crystal electric field excitations similar to those in the Tb-based counterpart are also observed indicating the strong Ising-like magnetic anisotropy. These comprehensive experiments and analyses have revealed the existence of a universal mechanism that stabilizes noncoplanar FM and AFM structures in non-Heisenberg Tsai-type ACs, independent of the rare-earth species (Tb, Dy, Ho); FM intra-cluster interactions and strong Ising-like anisotropy.
Multi-Q magnetic structures on two-dimensional (2D) lattices provide a key route to realizing topological physics in 2D magnetism. A major experimental challenge is to unambiguously confirm their formation by excluding the possibility of topologically trivial multidomain single- or double-Q magnetic orders, which cannot be distinguished using conventional diffraction techniques. Here, we propose that long-wavelength spin dynamics offers a universal diagnostic for triangular lattices: Triple-Q orders that preserve rotational symmetry and single- or double-Q orders that break it exhibit qualitatively distinct anisotropies in their Goldstone-mode velocities, stemming from fundamental differences in their underlying spin configurations. We validate this concept using the metallic triangular-lattice antiferromagnet Co_{0.325}TaS_{2}, which hosts both a stripe-type single-Q state and a triple-Q tetrahedral ordering at different temperatures. Using inelastic neutron-scattering and spin dynamics simulations, we first refine the spin Hamiltonian by fitting the paramagnetic excitation spectra, allowing us to develop an unbiased model independent of magnetic ordering. We then show that the observed velocity profiles of the Goldstone modes agree with the high-temperature model’s predictions: markedly anisotropic for the single-Q phase and near isotropic for the triple-Q phase. Importantly, this contrast persists across various exchange parameters, highlighting its model-independent nature and suggesting potential applicability to other 2D lattice systems. Beyond the long-wavelength regime, we present a substantial discrepancy between the measured and simulated magnon spectra exclusively in the triple-Q phase. We attribute this discrepancy to magnon energy renormalization arising from order-of-magnitude-enhanced magnon-magnon interactions in the triple-Q phase, due to its noncollinear configuration. This work provides universal insight into the dynamical properties of topological multi-Q magnetic orderings in 2D lattice structures, offering a broadly applicable diagnostic to distinguishing them from topologically trivial single- or double-Q counterparts. The unequivocal confirmation of the triple-Q structure in Co_{0.325}TaS_{2} further establishes it as a prominent material platform for exploring topological spin textures in the genuine 2D limit.
We performed inelastic x-ray and neutron scattering (IXS and INS) experiments for (Ba, Ca)TiO3 single crystals to elucidate the effect of Ca doping on the atomic dynamics. Dispersion relations of transverse phonons in BaTiO3, (Ba0.9Ca0.1)TiO3, and (Ba0.8Ca0.2)TiO3 were determined. The A-site-O vibrational mode as well as the acoustic mode were observed both by IXS and INS, whereas the Ti-O soft mode was detected only by INS. It was found that the A-site-O vibration exhibits significant softening with increasing Ca concentration, while the Ti-O soft mode is almost unaffected by the Ca doping. This finding is discussed in comparison with the polarization hysteresis loops and piezoelectric coefficients of (Ba, Ca)TiO3. It is indicated that the softening of the A-site-O vibration contributes to the enhancement of the piezoelectricity of Ca-doped BaTiO3-based materials.
Antiferromagnetic van der Waals family M P X 3 ( M = Fe , Mn , Co , and Ni; X = S and Se) have attracted significant research attention due to the possibility of realizing long-range magnetic order down to the monolayer limit. Here, we perform inelastic neutron scattering measurements on single -crystal samples of MnPSe 3 , a member of the M P X 3 family, to study the spin dynamics and determine the effective spin model. The excited magnon bands are well characterized by a spin model, which includes a Heisenberg term with three intraplane exchange parameters ( J 1 = - 0 . 73 meV, J 2 = - 0 . 014 meV, J 3 = - 0 . 43 meV) and one interplane parameter ( J c = - 0 . 054 meV), and an easy -plane single -ion anisotropy term ( D = - 0 . 035 meV). Additionally, we observe the intersection of the magnon and phonon bands but no anomalous spectral features induced by the formation of magnon-phonon hybrid excitations at the intersecting region. We discuss possible reasons for the absence of such hybrid excitations in MnPSe 3 .
TbMn6Sn6 is a correlated topological magnet with a Mn-based kagome lattice, in which a Chern gap opens at the Dirac point at low temperatures. The magnetic moment direction of the ferrimagnetic order changes from in the kagome plane to out-of-plane upon cooling, which is essential for generating the Chern gap, but the underlying mechanism for the spin reorientation remains elusive. Here, we investigate the spin-reorientation transition in TbMn6Sn6 using neutron scattering. We provide direct evidence for the spin-reorientation transition and unveil the coexistence of two Tb modes at 200 K. To account for these results, we put forward a model based on SU(N) spin-wave theory, in which there is a temperature evolution of the ground state Tb 4 f orbitals, driven by the crystalline electric field, single-ion anisotropy, and exchange interactions between Tb and Mn ions. Our findings shed light on the complex magnetism of TbMn6Sn6, despite its relatively simple ground state magnetic structure, and provide insights into the mechanisms for tuning magnetic topological materials.
Spontaneous Hall conductivity has recently been reported in the triangular lattice antiferromagnet Co1/3TaS2 under a zero magnetic field. This phenomenon originates from the distinctive noncoplanar triple -Q magnetic ground state, possessing uniform real -space Berry curvature characterized by scalar spin chirality. We investigated the physical properties of Co1/3TaS2 by judiciously controlling the composition, revealing a drastic change in its bulk properties, even by slight variations in cobalt composition, despite the same crystal structure. For 0.299 <= x <= 0.325, CoxTaS2 keeps all the characteristics of the ground state consistent with the previous studies-two antiferromagnetic phase transitions at T-N1 and T-N2 (< T-N1), a large spontaneous Hall conductivity [sigma(xy)(H = 0)], and a weak ferromagnetic moment along the c axis. However, samples with x >= 0.330 exhibit distinct bulk properties, including the absence of both sigma xy(H = 0) and the weak ferromagnetic moment. Our neutron diffraction data reveal that CoxTaS2 with x >= 0.330 develops coplanar helical magnetic order with q(m1) =(1/3, 0, 0). This is entirely different from what has been seen in x <= 0.325, explaining the observed composition dependence.
The understanding of the lattice dynamics is essential for engineering the thermal transport properties in quantum materials. Based on the canonical point of view, acoustic phonons are believed to be the principal thermal carriers in heat flow. Here, in this work, optical phonons are elucidated to play a pivotal role in determining the lattice thermal conductivity in thermoelectric material SnS by using the state-of-the-art inelastic neutron scattering technique combined with first-principles calculations. Additionally, in contrast to acoustic phonons, optical phonons are observed to exhibit pronounced softening and broadening with temperature. Our observations not only shed light on the significance of the optical phonons in thermal transport but also provide a vital clue to suppress the propagation of optical phonons to optimize the thermoelectric performance of SnS.
Magnon polarons are novel elementary excitations possessing hybrid magnonic and phononic signatures, and are responsible for many exotic spintronic and magnonic phenomena. Despite long-term sustained experimental efforts in chasing for magnon polarons, direct spectroscopic evidence of their existence is hardly observed. Here, we report the direct observation of magnon polarons using neutron spectroscopy on a multiferroic Fe2Mo3O8 possessing strong magnon-phonon coupling. Specifically, below the magnetic ordering temperature, a gap opens at the nominal intersection of the original magnon and phonon bands, leading to two separated magnon-polaron bands. Each of the bands undergoes mixing, interconverting and reversing between its magnonic and phononic components. We attribute the formation of magnon polarons to the strong magnon-phonon coupling induced by Dzyaloshinskii-Moriya interaction. Intriguingly, we find that the band-inverted magnon polarons are topologically nontrivial. These results uncover exotic elementary excitations arising from the magnon-phonon coupling, and offer a new route to topological states by considering hybridizations between different types of fundamental excitations.
The triangular lattice antiferromagnet (TLAF) has been the standard paradigm of frustrated magnetism for several decades. The most common magnetic ordering in insulating TLAFs is the 120° structure. However, a new triple- Q chiral ordering can emerge in metallic TLAFs, representing the short wavelength limit of magnetic skyrmion crystals. We report the metallic TLAF Co 1/3 TaS 2 as the first example of tetrahedral triple- Q magnetic ordering with the associated topological Hall effect (non-zero σ xy ( H = 0)). We also present a theoretical framework that describes the emergence of this magnetic ground state, which is further supported by the electronic structure measured by angle-resolved photoemission spectroscopy. Additionally, our measurements of the inelastic neutron scattering cross section are consistent with the calculated dynamical structure factor of the tetrahedral triple- Q state.