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Jun Sugiyama

Publications and source records attributed to Jun Sugiyama.

At least 19 recordsLinked to original sources

Topological Metal-Insulator Transition within the Ferromagnetic state

A major challenge in condensed matter physics is integrating topological phenomena with correlated electron physics to leverage both types of states for next-generation quantum devices. Metal-insulator transitions (MITs) are central to bridging these two domains while simultaneously serving as 'on-off' switches for electronic states. Here, we demonstrate how the prototypical material of K2Cr8O16 undergoes a ferromagnetic MIT accompanied by a change in band topology. Through inelastic x-ray and neutron scattering experiments combined with first-principles theoretical calculations, we demonstrate that this transition is not driven by a Peierls mechanism, given the lack of phonon softening. Instead, we establish the transition as a topological MIT within the ferromagnetic phase (topological-FM-MIT) with potential axionic properties, where electron correlations play a key role in stabilizing the insulating state. This work pioneers the discovery of a topological-FM-MIT and represents a fundamentally new class of topological phase transitions, revealing a unique pathway through which magnetism, topology, and electronic correlations interact.

cond-mat.str-el

Characterization of Nuclear and Magnetic Structures of Wolframite-Type MgReO4 and ZnReO4

We utilized high-pressure methods to synthesize the oxides AReO$4$ (A=Zn, Mg) and characterized their crystal structures as monoclinic wolframite-type. By combining muon spin spectroscopy ($μ^+$SR) with DFT calculations for muon stopping sites, we identify two possible magnetic spin structures for both compounds: $Γ_3$ with the propagation vector $\mathbf{k} = (0,1/2,0)$ and $Γ_4$ with $\mathbf{k} = (0,0,0)$. In both cases, the magnetic moments are canted from the principal axes within the $ac$-plane. The ordered moment of the proposed structures is $\mathbf{0.29(5)~μ\mathrm{B}}$ for $Γ_3$ and $\mathbf{0.25(8)~μ_\mathrm{B}}$ for $Γ_4$. The low moment is consistent with the absence of a magnetic contribution to the neutron powder diffraction (NPD) spectra. Bond valence sum (BVS) analysis supports the oxidation state of Re being Re$^{6+}$ in the compounds, and we suggest that a combination of $t_\mathrm{2g}$ orbital splitting due to spin-orbit coupling (SOC) and $d$-$p$ orbital hybridization is responsible for the strongly suppressed ordered magnetic moment.

cond-mat.mtrl-sci

Magnetic hysteresis control in thin film Fe/Si multilayers by incorporation of B4C

Magnetic hysteresis properties in Fe/Si multilayers have been studied as a function of the B4C content to control magnetization amplitude, coercivity, and hysteresis tilt, properties that are beneficial to tune for advancing applications in e.g. data storage, spintronics, and sensors. With an ion-assisted magnetron sputtering technique, 35 distinct thin film multilayer samples were prepared and their magnetic and structural properties were characterized by vibrating sample magnetometry, X-ray photoelectron spectroscopy, near edge X-ray absorption fine structure spectroscopy, and X-ray and neutron scattering methods. Key findings indicate that adding B4C lowers the coercivity and can decrease the saturation magnetization, demonstrating the tunability of magnetic responses based on composition. For samples with =30Å periodicity, 10-15% of B4C addition produces antiferromagnetically (AF) coupled multilayers, and such AF coupling strength increases with the B4C content. Our findings reveal that B atoms do not chemically bind within the Fe atoms but instead occupy interstitial positions, disrupting medium- to long-range crystallinity thereby inducing the amorphization. Thereon, the observed effects on magnetic properties are directly attributed to this amorphization process caused by the presence of B4C. The demonstrated ability to finely adjust magnetic properties by varying the B4C content offers a promising approach to overcome challenges in magnetic device performance and efficiency.

cond-mat.mtrl-sci

Diminished spin-flip reflectivity in stacked multilayers with varying period thicknesses of Fe/Si by incorporating 11B4C

This study investigates the effects of 11B4C co-sputtering on the structural and optical properties of Fe/Si stacked multilayers, with a focus on neutron supermirror applications. X-ray and neutron reflectivity techniques reveal that 11B4C incorporation improves interface sharpness, reduces roughness, and enhances reflectivity for all multilayer periods. Neutron reflectivity measurements show reduced spin-flip intensities, while wafer-curvature measurements indicate a 50% reduction in internal stress, allowing for higher mechanical stability of the multilayers. These improvements are attributed to the amorphization of Fe layers, which also suppress the formation of structural and magnetic domains responsible for stress and spin-flip scattering. In contrast, the pure Fe/Si sample exhibits a persistent half-order Bragg peak, indicating residual antiferromagnetic coupling. The results demonstrate that 11B4C enhances neutron optics by reducing spin-flip effects, increasing reflectivity and polarization, and alleviating stress, enabling the use of polarizers at reduced external fields compared to pure Fe/Si multilayers. These findings establish 11B4C as a transformative material for advancing neutron supermirror technology, paving the way for more efficient, stable, and high-performance polarizers in next-generation neutron optics.

cond-mat.mtrl-sci

Magnetic Properties of Multifunctional $^7$LiFePO$_4$ under Hydrostatic Pressure

LiFePO$_4$ (LFPO) is an archetypical and well-known cathode material for rechargeable Li-ion batteries. However, its quasi-one-dimensional (Q1D) structure along with the Fe ions, LFPO also displays interesting low-temperature magnetic properties. Our team has previously utilized the muon spin rotation ($μ^+$SR) technique to investigate both magnetic spin order as well as Li-ion diffusion in LFPO. In this initial study we extend our investigation and make use of high-pressure $μ^+$SR to investigate effects on the low-$T$ magnetic order. Contrary to theoretical predictions we find that the magnetic ordering temperature as well as the ordered magnetic moment increase at high pressure (compressive strain).

cond-mat.str-el

Revised Magnetic Structure and Tricritical Behavior of the CMR Compound NaCr$_2$O$_4$ Investigated with High Resolution Neutron Diffraction and $μ^+$SR

The mixed valence Cr compound NaCr$_2$O$_4$, synthesized using a high-pressure technique, offers a unique playground for investigating unconventional physical properties in condensed matter. In the present study, muon spin rotation/relaxation ($μ^+$SR) and high-resolution neutron powder diffraction (NPD) measurements were carried out to clarify the true magnetic ground state of this interesting compound. Our detailed study brings new insight, allowing us to confirm the existence of a commensurate antiferromagnetic order (C-AFM) and to extract its ordered Cr moment $μ^{\rm C}_{\rm Cr}=(4.30\pm0.01)μ_B$. Such a value of the ordered moment is in fact compatible with the existence of high-spin Cr sites. Further, the value of the canting angle of the Cr spin axial vector is refined as $θ_{\rm c}=(8.8\pm0.5)^{\circ}$. Employing high-quality samples in combination with time-of-flight NPD, a novel magnetic supercell was also revealed. Such supercell display an incommensurate (IC)-AFM propagation vector (0~0~${\textstyle \frac{1}{2}-}δ$), having an ordered moment $μ^{\rm IC}_{\rm Cr}=(2.20\pm0.03)μ_B$. It is suggested that the C-AFM and IC-AFM modulations are due to itinerant and localized contributions to the magnetic moment, respectively. Finally, the direct measurement of the magnetic order parameter provided a value of the critical exponent $β= 0.245 \approx \frac{1}{4}$, suggesting a non conventional critical behavior for the magnetic phase transition in NaCr$_2$O$_4$.

cond-mat.str-el

Na-ion Dynamics in the Solid Solution Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$ Studied by Muon Spin Rotation and Neutron Diffraction

In this work we present systematic set of measurements carried out by muon spin rotation/relaxation ($μ^+$SR) and neutron powder diffraction (NPD) on the solid solution Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$. This study investigates Na-ion dynamics in the quasi-1D (Q1D) diffusion channels created by the honeycomb-like arrangement of CrO$_6$ octahedra, in the presence of defects introduced by Ca doping. With increasing Ca content, the size of the diffusion channels is enlarged, however, this effect does not enhance the Na ion mobility. Instead the overall diffusivity is hampered by the local defects and the Na hopping probability is lowered. The diffusion mechanism in Na$_{\rm x}$Ca$_{1- \rm x}$Cr$_2$O$_4$ was found to be interstitial and the activation energy as well as diffusion coefficient were determined for all the members of the solid solution.

cond-mat.mtrl-sci

Refined magnetic structure of VI$_3$

The van der Waals ferromagnet (FM), VI$_3$, was studied by muon spin relaxation ($μ^+$SR) and first principle calculations based on density functional theory (DFT). Temperature dependent zero field muon spin relaxation ($μ^+$SR) measurements confirm the onset of long range FM order and the time spectra exhibits clear muon spin precession frequencies for $T<T_{\rm C}=50.03(1)$~K. The calculated internal magnetic fields at the predicted muon sites, based on the established magnetic structure from neutron diffraction, is inconsistent with the measured one. This inconsistency is because of strong incoherent neutron scattering and absorption originating from the elements V and I. Instead, a new and a more accurate magnetic structure is derived based on a combined study using $μ^+$SR and DFT. These results suggest strong contritions from orbital angular momentum, providing experimental evidence for the existence of unquenched orbital angular momentum of V$^{3+}$ in VI$_3$. Finally, an unusual form of a short range ordering is present above $T_{\rm C}$. Its temperature dependence is unlike previously reported cases in other layered compounds and its microscopic origin is discussed.

cond-mat.str-el

Magnetic nature of wolframite MgReO$_4$

Rhenium oxides belonging to the family $A$ReO$_4$ where $A$ is a metal cation, exhibit interesting electronic and magnetic properties. In this study we have utilized the muon spin rotation/relaxation ($μ^+$SR) technique to study the magnetic properties of the MgReO$_4$ compound. To the best of our knowledge, this is the first investigation reported on this interesting material, that is stabilized in a wolframite crystal structure using a special high-pressure synthesis technique. Bulk magnetic studies show the onset of an antiferromagnetic (AF) long range order, or a possible singlet spin state at $T_{\rm C1}\approx90$~K, with a subtle second high-temperature transition at $T_{\rm C2}\approx280$~K. Both transitions are also confirmed by heat capacity ($C_p$) measurements. From our $μ^+$SR measurements, it is clear that the sample enters an AF order below $T_{\rm C1}=T_{\rm N}\approx85$~K. We find no evidence of magnetic signal above $T_{\rm N}$, which indicates that $T_{\rm C2}$ is likely linked to a structural transition. Further, via sensitive zero field (ZF) $μ^+$SR measurements we find evidence of a spin reorientation at $T_{\rm Cant}\approx65$~K. This points towards a transition from a collinear AF into a canted AF order at low temperature, which is proposed to be driven by competing magnetic interactions.

cond-mat.str-el

Influence of the Magnetic Sub-Lattices in the Double Perovskite Compound LaCaNiReO$_6$

The magnetism of double perovskites is a complex phenomenon, determined from intra- or interatomic magnetic moment interactions, and strongly influenced by geometry. We take advantage of the complementary length and time scales of the muon spin rotation, relaxation and resonance ($μ^+$SR) microscopic technique and bulk AC/DC magnetic susceptibility measurements to study the magnetic phases of the LaCaNiReO$_6$ double perovskite. As a result we are able to discern and report a newly found dynamic phase transition and the formation of magnetic domains below and above the known magnetic transition of this compound at T$_N$ = 103 K. $μ^+$SR, serving as a local probe at crystallographic interstitial sites, reveals a transition from a metastable ferrimagnetic ordering below T = 103 K to a stable one below T = 30 K. The fast and slow collective dynamic state of this system are investigated. Between 103 K < T < 230 K, the following two magnetic environments appear, a dense spin region and a static-dilute spin region. The paramagnetic state is obtained only above T > 270 K. An evolution of the interaction between Ni and Re magnetic sublattices in this geometrically frustrated fcc perovskite structure, is revealed as a function of temperature and magnetic field, through the critical behaviour and thermal evolution of microscopic and macroscopic physical quantities.

cond-mat.str-el

Li-ion diffusion in single crystal LiFePO$_4$ measured by muon spin spectroscopy

Muon spin spectroscopy ($μ^+$SR) is now an established method to measure atomic scale diffusion coefficients of ions in oxides. This is achieved via the ion hopping rate, which causes periodic change in the local magnetic field at the muon site(s). We present here the first systematic study on a single crystalline sample. The highly anisotropic diffusion of Li-ions in the battery cathode material LiFePO$_4$, combined with the extensive investigation of this material with $μ^+$SR and other techniques make it a perfect model compound for this study. With this experiment we can confirm that Li diffusion in the bulk LiFePO$_4$ is measurable with $μ^+$SR. Hence, surface/interface effects, which might play a crucial role in case of powders/nano crystals, are less significant for macroscopic single crystals where bulk diffusion is in fact present. We observe that the internal magnetic field fluctuations caused by the diffusing Li-ions are different depending on the crystal orientation. This is not obviously expected based on theoretical considerations. Such fluctuation rates were used to estimate the diffusion coefficient, which agrees well with values estimated by first principle calculations considering anisotropic diffusion.

cond-mat.mtrl-sci

Pressure driven magnetic order in Sr$_{1-x}$Ca$_x$Co$_2$P$_2$

The magnetic phase diagram of Sr$_{1-x}$Ca$_x$Co$_2$P$_2$ as a function of hydrostatic pressure and temperature is investigated by means of high pressure muon spin rotation, relaxation and resonance ($μ^+$SR). The weak pressure dependence for the $x\neq1$ compounds suggests that the rich phase diagram of Sr$_{1-x}$Ca$_x$Co$_2$P$_2$ as a function of $x$ at ambient pressure may not only be attributed to solely chemical pressure effects. The $x=1$ compound on the other hand reveals a high pressure dependence, where the long range magnetic order is fully suppressed at $p_{\rm c2}\approx9.8$~kbar, which seem to be a first order transition. In addition, an intermediate phase consisting of dilute ferromagnetic islands (FMI) is formed above $p_{\rm c1}\approx8$~kbar where they co-exist with a magnetically disordered state. Moreover, such FMI phase seems to consist of an high- (FMI-\textcircled{\small{1}}) and low-temperature (FMI-\textcircled{\small{2}}) region, respectively, separated by a phase boundary at $T_{\rm i}\approx20$~K.

cond-mat.str-el

Charge Order Stabilized Quantum Spin Liquid in Hollandite K$_2$V$_8$O$_{16}$

Quantum spin liquid is an elusive state that display strong many-body entanglement with potential applications in future quantum computing. This study reports muon spin relaxation ($μ^+$SR) measurements on a novel high-pressure synthesized material, the Hollandite K$_{2}$V$_8$O$_{16}$. In this quasi-one-dimensional compound, charge ordering (CO) at $T_{\rm MIT}\approx160$~K effectively isolates half of the vanadium chains and model-like Heisenberg spin-1/2 chains are realized. Our zero field $μ^+$SR measurements show exponential like relaxation down to the lowest temperature $T=100$~mK and the absence of long range ordering is confirmed. The relaxation rate is found to be temperature independent below $T_{\rm QSL}\approx2$~K and measurements in longitudinal field confirms a highly dynamic ground state. These results represents the first confirmation of quantum spin liquid (QSL) behavior within the Hollandite family, stabilized by the CO. Finally, the presence of strong local electron correlation and one dimensional Fermi surface suggest this QSL to be a gapless Tomonaga-Luttinger liquid (TLL), which here uniquely presents itself in a stoichiometric compound under zero applied magnetic field and at ambient pressure.

cond-mat.str-el

Spin dynamics in the Van der Waals magnet CrCl$_3$

The magnetic nature of low dimensional compound, CrCl$_3$, was investigated by muon spin rotation, relaxation and resonance ($μ^+$SR). The $μ^+$SR measurements revealed three distinct phases as a function of temperature: an antiferromagnetic state (AF) for $T\leq T_{\rm N}=14.32(6)$~K, a ferromagnetic short range ordered state (FM-SRO) for $T_{\rm N}<T<\sim18$~K and a paramagnetic phase (PM) above $\sim18$~K. Moreover, the AF state exhibits appreciable spin dynamics, which increases with decreasing temperature below $T_{\rm N}$. These dynamics originate from out of plane fluctuations, which seem to settle for $9.5$~K$\leq T\leq T_{\rm N}$, evidenced from measurements in ZF and complementary local field calculations. Moreover, the presented muon Knight shift measurements just above $T_{\rm N}$ represent a clear microscopic evidence for the absence of the previously speculated long range quasi-2D FM order.

cond-mat.str-el

Co-existence of short- and long-range magnetic order in LaCo$_2$P$_2$

The ferromagnetic (FM) nature of the metallic LaCo$_2$P$_2$ was investigated with the positive muon spin rotation, relaxation and resonance ($μ^+$SR) technique. Transverse and zero field $μ^+$SR measurements revealed that the compound enters a long range FM ground state at $T_{\rm C}=130.91(65)$~K, consistent with previous studies. Based on the reported FM structure, the internal magnetic field was computed at the muon sites, which were predicted with first principles calculations. The computed result agree well with the experimental data. Moreover, although LaCo$_2$P$_2$ is a paramagnet at higher temperatures $T>160$~K, it enters a short range ordered (SRO) magnetic phase for $T_{\rm C}<T\leq160$~K. Measurements below the vicinity of $T_{\rm C}$ revealed that the SRO phase co-exists with the long range FM order at temperatures $124\leq T\leq T_{\rm C}$. Such co-existence is an intrinsic property and stems from competition between the 2D and 3D interactions/fluctuations.

cond-mat.str-el

Intertwined Magnetic Sub-Lattices in the Double Perovskite Compound LaSrNiReO6

We report a muon spin rotation ($μ^{+}$SR) study of the magnetic properties of the double perovskite compound LaSrNiReO$_{6}$. Using the unique length and time scales of the $μ^{+}$SR technique, we successfully clarify the magnetic ground state of LaSrNiReO$_{6}$, which was previously deemed as a spin glass state. Instead, our $μ^{+}$SR results point towards a long-range dynamically ordered ground state below $T_{\rm C}= 23$ K, for which a static limit is foreseen at $T=0$. Furthermore, between 23 K$ 250$ K) state. Our results reveal how two separate, yet intertwined magnetic lattices interact within the unique double perovskite structure and the importance of using complementary experimental techniques to obtain a complete understanding of the microscopic magnetic properties of complex materials.

cond-mat.str-el

Investigation of Ionic and Anomalous Magnetic Behavior in CrSe$_2$ Using $^8$Li $β$-NMR

We have studied a mosaic of 1T-CrSe$_2$ single crystals using $β$-detected nuclear magnetic resonance of $^{8}$Li from 4 to 300 K. We identify two broad resonances that show no evidence of quadrupolar splitting, indicating two magnetically distinct environments for the implanted ion. We observe stretched exponential spin lattice relaxation and a corresponding rate ($1/T_1$) that increases monotonically above 200 K, consistent with the onset of ionic diffusion. A pronounced maximum in $1/T_1$ is observed at the low temperature magnetic transition near 20 K. Between these limits, $1/T_1$ instead exhibits a broad minimum with a remarkable absence of strong features in the vicinity of structural and magnetic transitions between 150 and 200 K. Together, the results suggest $^{8}$Li$^{+}$ site occupation within the van der Waals gap between CrSe$_2$ trilayers. Possible origins of the two environments are discussed.

cond-mat.mtrl-sci

Magnetic moment of rare earth elements in R2Fe14B estimated with μ^+SR

The ferromagnetic (FM) nature of Nd2Fe14B has been investigated with muon spin rotation and relaxation (μ^+SR) measurements on an aligned, sintered plate-shaped sample. A clear muon spin precession frequency (f_{FM}) corresponding to the static internal FM field at the muon site showed an order parameter-like temperature dependence and disappeared above around 582 K (~T_C). This indicated that the implanted muons are static in the Nd2Fe14B lattice even at temperatures above around 600 K. Using the predicted muon site and local spin densities predicted by DFT calculations, the ordered Nd moment (M_{Nd}) was estimated to be 3.31 μ_B at 5 K, when both M_{Fe} and M_{Nd} are parallel to the c-axis and M_{Fe} = 2.1 μ_B. Furthermore, M_R in R2Fe14B with R = Y, Ce, Pr, Sm, Gd, Tb, Dy, Ho, Er, and Tm was estimated from f_μ values reported in earlier μ+SR work, using the FM structure proposed by neutron scattering and the same muon site and local spin density as in Nd2Fe14B. Such estimations yielded M_R values consistent with those obtained by the other methods.

cond-mat.mtrl-sci