SearcharxivSearch

arXiv subjects

Mitsutaka Nakamura

Publications and source records attributed to Mitsutaka Nakamura.

At least 19 recordsLinked to original sources

Local magnon modes studied by dynamic magnetic pair-density function analysis

The dynamic magnetic pair-density function (DymPDF) $D_{\rm M}(r, E)$ is obtained via the Fourier transform of the dynamic magnetic structure factor, $S_{\rm M}(Q, E)$, which is measured using nonpolarized inelastic neutron scattering. While there is a long history of magnetic excitation studies with $S_{\rm M}(Q, E)$, there are no reports on $D_{\rm M}(r, E)$. In this study, we examine simple magnet models and representative magnet examples, such as FeTiO$_{3}$ and YBa$_{2}$Cu$_{3}$O$_{6}$, to investigate the real-space dynamics of $D_{\rm M}(r, E)$. We derive the $D_{\rm M}(r, E)$ equations for simple magnet models in a low energy limit. By comparing these equations to the simulations, we demonstrate the characteristic energy dependence of real-space local magnon modes, including the transition of the magnon mode from acoustic to optical. Our novel analysis reveals the local magnon modes accompanied by a sign change in each spin-pair correlation at a given energy in nanoscale real space even under non-periodic conditions. This method is unique for studying local magnetic dynamics.

cond-mat.str-el

Magnetic Signature of Chiral Phonons Revealed by Neutron Spectroscopy in Ferrimagnetic Fe$_{1.75}$Zn$_{0.25}$Mo$_3$O$_8$

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 $T_{\rm C}\sim49$ K. Below $T_{\rm C}$, 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 $T_{\rm C}$, 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.

cond-mat.str-el

Refined spin Hamiltonian on the Cairo pentagonal lattice of Bi2Fe4O9

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.

cond-mat.str-el

From weakly interacting spinons to tightly bound triplons in the frustrated quantum spin-Peierls chain

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.

cond-mat.str-el

Nematic quantum disordered state in FeSe

The unusual quantum-disordered magnetic ground state intertwined with superconductivity and electronic nematicity in FeSe has been a research focus in iron-based superconductors. However, the intrinsic spin excitations across the entire Brillouin zone in detwinned FeSe, which forms the basis for a microscopic understanding of the magnetic state and superconductivity, remain to be determined. Here, we use inelastic neutron scattering to map out the spin excitations of FeSe dewtinned with a uniaxial-strain device. We find that the stripe spin excitations (Q=(1, 0)/(0, 1)) exhibit the $C_2$ symmetry up to $E\approx120$ meV, while the N{é}el spin excitations (Q=(1, 1)) retain their $C_4$ symmetry in the nematic state. The temperature dependence of the difference in the spin excitations at Q=(1, 0) and (0, 1) for temperatures above the structural phase transition unambiguously shows the establishment of the nematic quantum disordered state. The similarity of the Néel excitations in FeSe and NaFeAs suggests that the Néel excitations are driven by the enhanced electron correlations in the $3d_{xy}$ orbital. By determining the key features of the stripe excitations and fitting their dispersions using a Heisenberg Hamiltonian with biquadratic interaction ($J_1$-$K$-$J_2$), we establish a spin-interaction phase diagram and conclude that FeSe is close to a crossover region between the antiferroquadrupolar, Néel, and stripe ordering regimes. The results provide an experimental basis for establishing a microscopic theoretical model to describe the origin and intertwining of the emergent orders in iron-based superconductors.

cond-mat.supr-con

The influence of Structural Dynamics in Two-Dimensional Hybrid Organic-Inorganic Perovskites on their Photoluminescence Efficiency -- Neutron scattering analysis

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.

cond-mat.mtrl-sci

Gapless dispersive continuum in a modulated quantum kagome antiferromagnet

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 Cu$^{2+}$ (3d$^9$, $s=\frac{1}{2}$) 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 fluoride Cs$_8$RbK$_3$Ti$_{12}$F$_{48}$ where Ti$^{3+}$ (3d$^1$, $s = \frac{1}{2}$) 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 $S(Q,\hbarω)$ 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.

cond-mat.str-el

Direct observation of topological magnon polarons in a multiferroic material

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 Fe$_{2}$Mo$_{3}$O$_{8}$ 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.

cond-mat.str-el

Single crystal growths and magnetic properties of hexagonal polar semimetals RAuGe (R = Y, Gd-Tm, and Lu)

We study structural and magnetic properties of rare-earth based semimetals RAuGe (R = Y, Gd-Tm, and Lu) using flux-grown single crystals. These compounds belong to the noncentrosymmetric polar space group P63mc. We confirm the systematic structural evolution at room temperature as a function of ionic radius of rare earths to clarify the isopointal crossover between two polar structures: three-dimensional LiGaGe-type and quasi-two-dimensional NdPtSb-type. Magnetism shows a characteristic anisotropy in reasonable agreement with the crystal electric field (CEF) theory; the easy-plane-type anisotropy for R = Tb and Dy turns into the Ising-type anisotropy for R = Er and Tm. We evaluate the CEF parameters based on the Stevens operators to reasonably reproduce the temperature dependence of magnetic susceptibilities and specific heat for RAuGe (R = Tb-Tm). The estimated energy scale of the Ising gap (~ 11 meV) in TmAuGe is consistent with an excitation observed in an inelastic neutron scattering experiment. These findings suggest an opportunity for interplay between conduction electrons and nontrivial spin structures in the family of magnetic polar semimetals RAuGe.

cond-mat.mtrl-sci

The $ω^3$ scaling of the vibrational density of states in quasi-2D nanoconfined solids

Atomic vibrations play a vital role in the functions of various physical, chemical, and biological systems. The vibrational properties and the specific heat of crystalline bulk materials are well described by Debye theory, which successfully predicts the quadratic $ω^{2}$ low-frequency scaling of the vibrational density of states (VDOS) in bulk ordered solids from few fundamental assumptions. However, the analogous framework for nanoconfined materials with fewer degrees of freedom has been far less well explored. Using inelastic neutron scattering, we characterize the VDOS of amorphous ice confined to a thickness of $\approx 1$ nm inside graphene oxide membranes and we observe a crossover from the Debye $ω^2$ scaling to an anomalous $ω^3$ behaviour upon reducing the confinement size $L$. Additionally, using molecular dynamics simulations, we confirm the experimental findings and also prove that such a scaling of the VDOS appears in both crystalline and amorphous solids under slab-confinement. We theoretically demonstrate that this low-frequency $ω^3$ law results from the geometric constraints on the momentum phase space induced by confinement along one spatial direction. Finally, we predict that the Debye scaling reappears at a characteristic frequency $ω_\times= v L/2π$, with $v$ the speed of sound of the material, and we confirm this quantitative estimate with simulations. This new physical phenomenon, revealed by combining theoretical, experimental and simulations results, is relevant to a myriad of systems both in synthetic and biological contexts and it could impact various technological applications for systems under confinement such as nano-devices or thin films.

cond-mat.mtrl-sci

Q Dependence of Magnetic Resonance Mode on FeTe$_{0.5}$Se$_{0.5}$ Studied by Inelastic Neutron Scattering

Inelastic neutron scattering measurements have been performed on a superconducting single crystal FeTe$_{0.5}$Se$_{0.5}$ to examine the ${\bf Q}$-dependent enhancement of the dynamical structure factor, $S({\bf Q},E)$, from ${\bf Q}$ = (0, 0) to ($π$, $π$), including ($π$, 0) in the superconducting state. In most of iron-based superconductors, $S({\bf Q},E)$ is enhanced at ${\bf Q}$ = ($π$, 0), where the "magnetic resonance mode" is commonly observed in the unfolded Brillouin zone. Constant-$E$ cuts of $S({\bf Q},E)$ suggest that the enhancement is not uniform in the magnetic excitation, and limited around ${\bf Q}$ = ($π$, 0). This result is consistent with the theoretical simulation of the magnetic resonance mode due to the Bardeen$-$Cooper$-$Schrieffer coherence factor with the sign-reversing order parameter of s$_{\pm}$ wave.

cond-mat.supr-con

Magnetic excitations of Sr$_3$Ir$_2$O$_7$ observed by inelastic neutron scattering measurement

In this short note, we report on the first inelastic neutron scattering (INS) study on high-energy magnetic excitations in Sr$_3$Ir$_2$O$_7$. We observed excitations between $\sim$80 meV and $\sim$180 meV. The peak position of the excitations is consistent with the dispersion of a single magnon determined by resonant inelastic X-ray scattering (RIXS) measurement. Thus, our results demonstrate that INS and RIXS observe identical excitations in iridate oxides, as in La$_2$CuO$_4$.

cond-mat.str-el

Temporally-decoherent and spatially-coherent vibrations in metal halide perovskite

The long carrier lifetime and defect tolerance in metal halide perovskites (MHPs) are major contributors to the superb performance of MHP optoelectronic devices. Large polarons were reported to be responsible for the long carrier lifetime. Yet microscopic mechanisms of the large polaron formation including the so-called phonon melting, are still under debate. Here, time-of-flight (TOF) inelastic neutron scattering (INS) experiments and first-principles density-functional theory (DFT) calculations were employed to investigate the lattice vibrations (or phonon dynamics) in methylammonium lead iodide ($\rm{MAPbI_3}$), a prototypical example of MHPs. Our findings are that optical phonons lose temporal coherence gradually with increasing temperature which vanishes at the orthorhombic-to-tetragonal structural phase transition. Surprisingly, however, we found that the spatial coherence is still retained throughout the decoherence process. We argue that the temporally decoherent and spatially coherent vibrations contribute to the formation of large polarons in this metal halide perovskite.

cond-mat.mtrl-sci

Spin dynamics of a magnetic Weyl semimetal Sr$_{1-x}$Mn$_{1-y}$Sb$_2$

Dirac matters provide a platform for exploring the interplay of their carriers with other quantum phenomena. Sr$_{1-x}$Mn$_{1-y}$Sb$_2$ has been proposed to be a magnetic Weyl semimetal and provides an excellent platform to study the coupling between Weyl fermions and magnons. Here, we report comprehensive inelastic neutron scattering (INS) measurements on single crystals of Sr$_{1-x}$Mn$_{1-y}$Sb$_2$, which have been well characterized by magnetization and magnetotransport measurements, both of which demonstrate that the material is a topologically nontrivial semimetal. The INS spectra clearly show a spin gap of $\sim6$ meV. The dispersion in the magnetic Mn layer extends up to about 76 meV, while that between the layers has a narrow band width of 6 meV. We find that the linear spin-wave theory using a Heisenberg spin Hamiltonian can reproduce the experimental spectra with the following parameters: a nearest-neighbor ($SJ_1\sim28.0$ meV) and next-nearest-neighbor in-plane exchange interaction ($SJ_2\sim9.3$ meV) , interlayer exchange coupling ($SJ_c\sim-0.1$ meV), and spin anisotropy constant ($SD\sim-0.07$ meV). Despite the coexistence of Weyl fermions and magnons, we find no clear evidence that the magnetic dynamics are influenced by the Weyl fermions in Sr$_{1-x}$Mn$_{1-y}$Sb$_2$, possibly because that the Weyl fermions and magnons reside in the Sb and Mn layers separately, and the interlayer coupling is weak due to the quasi-two-dimensional nature of the material, as also evident from the small $SJ_c$ of -0.1 meV.

cond-mat.mtrl-sci

Emergent spin-$1$ Haldane gap and ferroelectricity in a frustrated spin-$1/2$ ladder

We report experimental and theoretical evidence that Rb$_2$Cu$_2$Mo$_3$O$_{12}$ has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin-$1/2$ chains and exhibits a Haldane spin gap of emergent spin-1 pairs. Three spin excitations split from the spin-1 triplet by a Dzyaloshinskii-Moriya interaction are identified in inelastic neutron-scattering and electron spin resonance spectra. A tiny magnetic field generates ferroelectricity without closing the spin gap, indicating a novel class of ferroelectricity induced by a vector spin chirality order.

cond-mat.str-el

Energy Resolution and Neutron Flux of the 4SEASONS Spectrometer Revisited

The elastic energy resolution, integrated intensity, and peak intensity of the direct-geometry neutron chopper spectrometer 4SEASONS at Japan Proton Accelerator Research Complex (J-PARC) were re-investigated. This was done with respect to the incident energy and the rotation speed of the Fermi chopper using incoherent scattering of vanadium and simple analytical formulas. The model calculations reproduced the observed values satisfactorily. The present work should be useful for estimating in instrument performance in experiments.

physics.ins-det

Quantum dynamics of hydrogen in iron-based superconductor LaFeAsO0.9D0.1 measured with inelastic neutron spectroscopy

Inelastic neutron scattering was performed for an iron-based superconductor LaFeAsO0.9D0.1, where most of D (deuterium) replaces oxygen, while a tiny amount goes into interstitial sites. By first-principle calculation, we characterize the interstitial sites for D (and for H slightly mixed) with four equivalent potential minima. Below the superconducting transition temperature Tc = 26 K,new excitations emerge in the range 5-15 meV, while they are absent in the reference system LaFeAsO0.9F0.1. The strong excitations at 14.5 meV and 11.1 meV broaden rapidly around 15 K and 20 K, respectively, where each energy becomes comparable to twice of the superconducting gap. The strong excitations are ascribed to a quantum rattling, or a band motion of hydrogen, which arises only if the number of potential minima is larger than two.

cond-mat.supr-con

High-energy spin fluctuation in low-$T_{\rm c}$ iron-based superconductor LaFePO$_{0.9}$

Spin fluctuations are widely believed to play an important role in the superconducting mechanisms of unconventional high-temperature superconductors. Spin fluctuations have been observed in iron-based superconductors as well. However, in some iron-based superconductors such as LaFePO$_{0.9}$, they have not been observed by inelastic neutron scattering (INS). LaFePO$_{0.9}$ is an iron-based superconductor with a low superconducting transition temperature ($T_{\rm c}$= 5 K), where line nodes are observed in the superconducting gap function. The line-node symmetry typically originates from sign reversal of the order parameter in spin-fluctuation-mediated superconductivity. This contradiction has been a long-standing mystery of this superconductor. Herein, spin fluctuations were found at high energies such as 30$-$50 meV with comparable intensities to an optimally doped LaFeAs(O,F). Based on this finding, the line-node symmetry can be explained naturally as spin-fluctuation-mediated superconductivity.

cond-mat.supr-con