arXiv subjects

Hiroyuki Nojiri

Publications and source records attributed to Hiroyuki Nojiri.

At least 19 recordsLinked to original sources

arXiv2026

Multistage spin correlations in the $s$ = 1/2 stuffed hyper-star lattice Li$_{2}$Cu$_{2}$(MoO$_{4}$)$_{3}$

Star lattice, which can be visualized as a honeycomb network with each vertex replaced by a triangle, provides a rare platform for realizing exotic quantum states such as quantum spin liquids and disorder-driven random-singlet (RS) states. Herein, we investigate the ground-state properties of the three-dimensional (3D) stuffed hyper-star lattice Li$_2$Cu$_2$(MoO$_4$)$_3$, which exhibits a crossover from short-range spin correlations to a disorder-driven RS-like state below $T^{*}\sim$15.8 K. Thermodynamic and microscopic measurements capture this crossover through a change in the power-law behavior of various observables, from $\sim T^{0.25}$ for $T > T^{*}$ to $\sim T^{-0.50}$ for $T < T^{*}$. Upon further cooling, a quasi-frozen state emerges near $T_{\rm f} = 0.32$ K, likely associated with weakly coupled spin chains within the hyper-star spin network. Our results underscore the crucial role of orphan spins and weak residual interactions in stabilizing a disorder-driven quantum-disordered state in 3D.

cond-mat.str-el↗

arXiv2025

Spin dynamics in natural multiferroic pyroxene NaFeSi$_2$O$_6$

Spin dynamics in the natural mineral aegirine, NaFeSi$_2$O$_6$, a member of the pyroxene family, was studied by elastic and inelastic neutron scattering. Magnetization and specific heat measurements as well as single-crystal neutron diffraction maps, taken in the temperature range 2 - 20 K, confirm two successive magnetic transitions at 8.8 and 5.8 K, consistent with previous studies. The observed spin-wave excitations emerge from the incommensurate magnetic Bragg peaks corresponding to the propagation vector $k_{\rm ICM} = (0, 0.77, 0)$, and extend up to energies of about 1.5 meV. In the low-temperature helical phase, the spin dynamics of the Fe$^{3+}$ ions is well described by a simple linear spin-wave model. The observed excitations can be modeled using a spin Hamiltonian that includes three primary exchange interactions - intrachain coupling $J=0.142(2)$ meV, interchain couplings $J_1=0.083(1)$ meV and $J_2=0.186(1)$ meV - and an easy-plane anisotropy $D=0.020(6)$ meV. Our results show that no single exchange interaction dominates the spin dynamics. The similar strengths of the intrachain and interchain couplings point to the fact that the magnetic interactions in aegirine are three-dimensional rather than confined along one direction. As a result, the system cannot be considered quasi-one-dimensional, as previously suggested, and calls for further investigations.

cond-mat.str-el↗

arXiv2025

Unconventional Temperature Dependence of Exciton Diamagnetism in 2D Ruddlesden-Popper Lead Halide Perovskites

Layered hybrid perovskites containing larger organic cations have demonstrated superior environmental stability, but the presence of these insulating spacers also strengthens the exciton binding energy, which contributes to reduced carrier separation. The consequences of increased binding energy on device efficiency are still not fully documented, and binding energy measurements are often conducted at cryogenic temperatures where linewidths are decreased and a series of hydrogen-like bound states can be identified, but not under ambient conditions where devices are expected to operate. In contrast to the quenching observed in 3D perovskites such as methylammonium lead iodide, where exciton binding energies are thought to decrease at higher temperatures, we present evidence for a smaller excitonic radius at higher temperatures in the $n=5$ member of butylammonium-spaced methylammonium lead iodide, (BA)$_2$(MA)$_{n-1}$Pb$_n$I$_{3n+1}$. We measured the temperature-dependent diamagnetic shift coefficient in magnetic fields up to 40\,T, which is one-third as large at room temperature as those at cryogenic temperatures. In both the ideal 2D and 3D hydrogen models, this trend would indicate that the exciton binding energy more than triples at room temperature.

cond-mat.mtrl-sci↗

arXiv2025

Bullet pressure-cell design for neutron scattering experiments with horizontal magnetic fields and dilution temperatures

The simultaneous application of high magnetic fields and high pressures for controlling magnetic ground states is important for testing our understanding of many-body quantum theory. However, the implementation for neutron scattering experiments presents a technical challenge. To overcome this challenge we present an optimized pressure-cell design with a novel bullet shape, which is compatible with horizontal-field magnets, in particular the high-field magnet operating at the Helmholtz-Zentrum Berlin. The cell enabled neutron diffraction and spectroscopy measurements with the combination of three extreme conditions: high pressures, high magnetic fields, and dilution temperatures, simultaneously reaching 0.7 GPa, 25.9 T, and 200 mK. Our results demonstrate the utility of informed material choices and the efficiency of finite-element analysis for future pressure-cell designs to be used in combination with magnetic fields and dilution temperatures for neutron scattering purposes.

cond-mat.str-el↗

arXiv2024

Zeeman polaritons as a platform for probing Dicke physics in condensed matter

The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd$_3$Ga$_5$O$_{12}$. The electron paramagnetic resonance of Gd$^{3+}$ ions is tuned by a magnetic field into resonance with a Fabry--Pérot cavity mode, resulting in the formation of spin--photon hybrid states, or Zeeman polaritons. We observe that the light--matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids.

quant-ph↗

arXiv2024

Angle-resolved photoemission spectroscopy with an $\textit{in situ}$ tunable magnetic field

Angle-resolved photoemission spectroscopy (ARPES) is a powerful tool for probing the momentum-resolved single-particle spectral function of materials. Historically, $\textit{in situ}$ magnetic fields have been carefully avoided as they are detrimental to the control of photoelectron trajectory during the photoelectron detection process. However, magnetic field is an important experimental knob for both probing and tuning symmetry-breaking phases and electronic topology in quantum materials. In this paper, we introduce an easily implementable method for realizing an $\textit{in situ}$ tunable magnetic field at the sample position in an ARPES experiment and analyze magnetic field induced artifacts in ARPES data. Specifically, we identified and quantified three distinct extrinsic effects of a magnetic field: Fermi surface rotation, momentum shrinking, and momentum broadening. We examined these effects in three prototypical quantum materials, i.e., a topological insulator (Bi$_2$Se$_3$), an iron-based superconductor (LiFeAs), and a cuprate superconductor (Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$), and demonstrate the feasibility of ARPES measurements in the presence of a controllable magnetic field. Our studies lay the foundation for the future development of the technique and interpretation of ARPES measurements of field-tunable quantum phases.

cond-mat.str-el↗

arXiv2024

Higher-magnesium-doping effects on the singlet ground state of the Shastry-Sutherland SrCu2(BO3)2

Doping of quantum antiferromagnets is an established approach to investigate the robustness of their ground state against the competing phases. Predictions of doping effects on the ground state of the Shastry-Sutherland dimer model are here verified experimentally on Mg-doped SrCu2(BO3)2. A partial incorporation of Mg2+ on the Cu2+-site in the SrCu2(BO3)2 structure leads to a subtle but systematic lattice expansion with the increasing Mg-doping concentration, which is accompanied by a concomitant decrease in the spin gap, the Curie-Weiss temperature and the peak temperature of the susceptibility. These findings indicate a doping-induced breaking of Cu2+ spin-1/2 dimers which is also corroborated by X-band EPR spectroscopy that points to a systematic increase in intensity of free Cu2+ sites with increasing Mg-doping concentration. Extending the Mg-doping up to nominal x = 0.10 or SrCu1.9Mg0.1(BO3)2, in the magnetisation measurements taken up to 35 T, a suppression of the pseudo-1/8 plateau is found along with a clear presence of an anomaly at an onset critical field H'C0 ~ 9 T. The latter, absent in pure SrCu2(BO3)2, emerges due to the coupling of liberated Cu2+ spin-1/2 entities in the vicinity of Mg-doping induced impurities.

cond-mat.str-el↗

arXiv2024

Pressure-tuned quantum criticality in the large-$D$ antiferromagnet DTN

Strongly correlated spin systems can be driven to quantum critical points via various routes. In particular, gapped quantum antiferromagnets can undergo phase transitions into a magnetically ordered state with applied pressure or magnetic field, acting as tuning parameters. These transitions are characterized by $z=1$ or $z=2$ dynamical critical exponents, determined by the linear and quadratic low-energy dispersion of spin excitations, respectively. Employing high-frequency susceptibility and ultrasound techniques, we demonstrate that the tetragonal easy-plane quantum antiferromagnet NiCl$_{2}\cdot$4SC(NH$_2$)$_2$ (aka DTN) undergoes a spin-gap closure transition at about $4.2$ kbar, resulting in a pressure-induced magnetic ordering. The studies are complemented by high-pressure-electron spin-resonance measurements confirming the proposed scenario. Powder neutron diffraction measurements revealed that no lattice distortion occurs at this pressure and the high spin symmetry is preserved, establishing DTN as a perfect platform to investigate $z=1$ quantum critical phenomena. The experimental observations are supported by DMRG calculations, allowing us to quantitatively describe the pressure-driven evolution of critical fields and spin-Hamiltonian parameters in DTN.

cond-mat.str-el↗

arXiv2024

Observation of the Magnonic Dicke Superradiant Phase Transition

Two-level atoms coupled with single-mode cavity photons are predicted to exhibit a quantum phase transition when the coupling strength exceeds a critical value, entering a phase in which atomic polarization and photonic field are finite even at zero temperature and without external driving. However, this phenomenon, the superradiant phase transition (SRPT), is forbidden by a no-go theorem due to the existence of the diamagnetic term in the Hamiltonian. Here, we present spectroscopic evidence for a magnonic SRPT in ErFeO$_3$, where the role of the photonic mode (two-level atoms) in the photonic SRPT is played by an Fe$^{3+}$ magnon mode (Er$^{3+}$ spins). The absence of the diamagnetic term in the Fe$^{3+}$-Er$^{3+}$ exchange coupling ensures that the no-go theorem does not apply. Terahertz and gigahertz magnetospectroscopy experiments revealed the signatures of the SRPT -- a kink and a softening, respectively, of two spin-magnon hybridized modes at the critical point.

quant-ph↗

arXiv2023

One-ninth magnetization plateau stabilized by spin entanglement in a kagome antiferromagnet

The spin-1/2 antiferromagnetic Heisenberg model on a Kagome lattice is geometrically frustrated, which is expected to promote the formation of many-body quantum entangled states. The most sought-after among these is the quantum spin liquid phase, but magnetic analogs of liquid, solid, and supersolid phases may also occur, producing fractional plateaus in the magnetization. Here, we investigate the experimental realization of these predicted phases in the Kagome material YCu3(OD)6+xBr3-x (x=0.5). By combining thermodynamic and Raman spectroscopic techniques, we provide evidence for fractionalized spinon excitations and observe the emergence of a 1/9 magnetization plateau. These observations establish YCu3(OD)6+xBr3-x as a model material for exploring the 1/9 plateau phase.

cond-mat.str-el↗

arXiv2023

Terahertz cavity magnon polaritons

Hybrid light-matter coupled states, or polaritons, in magnetic materials have attracted significant attention due to their potential for enabling novel applications in spintronics and quantum information processing. However, most studies to date have been carried out for ferromagnetic materials with magnon excitations at gigahertz frequencies. Here, we have investigated strong resonant photon-magnon coupling at frequencies above 1 terahertz for the first time in a prototypical room-temperature antiferromagnetic insulator, NiO, inside a Fabry-Pérot cavity. The cavity was formed by the crystal itself when it was thinned down to an optimized thickness. By using terahertz time-domain spectroscopy in high magnetic fields up to 25 T, we swept the magnon frequency through Fabry-Pérot cavity modes and observed photon-magnon anticrossing behavior, demonstrating clear vacuum Rabi splittings exceeding the polariton linewidths. These results show that NiO is a promising platform for exploring antiferromagnetic spintronics and cavity magnonics in the terahertz frequency range.

physics.optics↗

arXiv2023

Field-induced bound-state condensation and spin-nematic phase in SrCu$_2$(BO$_3$)$_2$ revealed by neutron scattering up to 25.9 T

Bose-Einstein condensation (BEC) underpins exotic forms of order ranging from superconductivity to superfluid 4 He. In quantum magnetic materials, ordered phases induced by an applied magnetic field can be described as the BEC of magnon excitations. With sufficiently strong magnetic frustration, exemplified by the system SrCu$_2$(BO$_3$)$_2$ , no clear magnon BEC is observed and the complex spectrum of multi-magnon bound states may allow a different type of condensation, but the high fields required to probe this physics have remained a barrier to detailed investigation. Here we exploit the first purpose-built high-field neutron scattering facility to measure the spin excitations of SrCu$_2$(BO$_3$)$_2$ up to 25.9 T and use cylinder matrix-product-states (MPS) calculations to reproduce the experimental spectra with high accuracy. Multiple unconventional features point to a condensation of $S = 2$ bound states into a spin-nematic phase, including the gradients of the one-magnon branches, the presence of many novel composite two- and three-triplon excitations and the persistence of a one-magnon spin gap. This gap reflects a direct analogy with superconductivity, suggesting that the spin-nematic phase in SrCu$_2$(BO$_3$)$_2$ is best understood as a condensate of bosonic Cooper pairs. Our results underline the wealth of unconventional states yet to be found in frustrated quantum magnetic materials under extreme conditions.

cond-mat.str-el↗

arXiv2023

Chiral Phonons with Giant Magnetic Moments in a Topological Crystalline Insulator

We have studied the magnetic response of transverse optical phonons in Pb$_{1-x}$Sn$_{x}$Te films. Polarization-dependent terahertz magnetospectroscopy measurements revealed Zeeman splittings and diamagnetic shifts, demonstrating that these phonon modes become chiral in magnetic fields. Films in the topological crystalline insulator phase ($x > 0.32$) exhibited magnetic moment values that are larger than those for topologically trivial films ($x < 0.32$) by two orders of magnitude. Furthermore, the sign of the effective $g$-factor was opposite in the two phases, which can be explained by our theoretical model. These results strongly indicate the existence of interplay between the magnetic properties of chiral phonons and the topology of electronic band structure.

cond-mat.mes-hall↗

arXiv2022

Magnetically Tuned Continuous Transition from Weak to Strong Coupling in Terahertz Magnon Polaritons

Depending on the relative rates of coupling and dissipation, a light-matter coupled system is either in the weak- or strong-coupling regime. Here, we present a unique system where the coupling rate continuously increases with an externally applied magnetic field while the dissipation rate remains constant, allowing us to monitor a weak-to-strong coupling transition as a function of magnetic field. We observed a Rabi splitting of a terahertz magnon mode in yttrium orthoferrite above a threshold magnetic field of ~14 T. Based on a microscopic theoretical model, we show that with increasing magnetic field the magnons transition into magnon polaritons through an exceptional point, which will open up new opportunities for in situ control of non-Hermitian systems.

cond-mat.mes-hall↗

arXiv2022

Magnetic Control of Soft Chiral Phonons in PbTe

PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term. In magnetic fields up to 25T, the phonon mode split into two modes with opposite handedness, exhibiting circular dichroism. Their frequencies displayed Zeeman splitting together with an overall diamagnetic shift with increasing magnetic field. Using a group-theoretical approach, we demonstrate that these observations are results of magnetic field-induced morphic changes in the crystal symmetries through the Lorentz force exerted on the lattice ions. This study thus reveals a novel process of controlling phonon properties in a soft ionic lattice by a strong magnetic field.

physics.optics↗

arXiv2021

Combination of Optical Transitions of Polarons with Rashba Effect in Methylammonium Lead Tri-halide Perovskites under High Magnetic Fields

We investigate photoluminescence (PL) transitions of MAPbX$_{3}$ (X = I, Br and Cl) organic-inorganic hybrid perovskite single crystals under magnetic fields of up to 60 T. In these materials, sharp free-exciton transition peaks emerge at a low temperature (4.2 K). Under strong magnetic fields, the free-exciton PL transitions of three different halogens show dramatic differences. The free-exciton transitions of the MAPbCl$_{3}$ crystal undergo negative energy shifts, while those of the MAPbBr$_{3}$ crystal show normal diamagnetic shifts. To obtain the variation from Cl to Br, we attempt to measure PL transitions of MAPbCl$_{x}$Br$_{3-x}$. For MAPbI$_{3}$, the transition-energy shifts for both $σ^{+}$ and $σ^{-}$ transitions at 4.2 K exhibit a power-law dependence on the magnetic field. Such inconsistent magnetic-field effects on different halogens make it difficult to understand the transition-energy behavior through a unified model. We propose a possible mechanism for the field effects that is based on a combination of the Rashba effect induced by strong spin-orbit coupling and the polaron effect caused by the polar nature of the inorganic elements.

cond-mat.mtrl-sci↗

arXiv2021

Soft X-ray absorption spectroscopy and magnetic circular dichroism under pulsed high magnetic field of Ni-Co-Mn-In metamagnetic shape memory alloy

In this study, X-ray absorption spectroscopy (XAS) experiments for Ni45Co5Mn36.7In13.3 metamagnetic shape memory alloy were performed under high magnetic fields up to 12 T using a pulsed magnet. Field-induced reverse transformation to austenite phase caused considerable changes in the magnetic circular dichroism (MCD) signals and the magnetic moments of the ferromagnetic coupling between Mn, Ni, and Co were determined. The spin magnetic moment, Mspin, and orbital magnetic moment, Morb, of Mn atom in the induced austenite ferromagnetic phase, estimated based on the magneto-optical sum rule, were 3.2 and 0.13 μB, respectively, resulting in an Morb / Mspin ratio of 0.04. In the element-specific magnetization curves recorded at 150 K, metamagnetic behavior associated with the field-induced reverse transformation is clearly observed and reverse transformation finishing magnetic field and martensitic transformation starting magnetic field are detected. There was almost no difference in the magnetically averaged XAS spectrum for Mn-L2,3 edges between in the martensite and in the magnetic field-induced austenite phases, however, it was visible for Ni, indicating that Ni 3d-electrons mainly contribute to martensitic transformation.

cond-mat.mtrl-sci↗

arXiv2021

Ultrastrong Magnon-Magnon Coupling Dominated by Antiresonant Interactions

Exotic quantum vacuum phenomena are predicted in cavity quantum electrodynamics (QED) systems with ultrastrong light-matter interactions. Their ground states are predicted to be vacuum squeezed states with suppressed quantum fluctuations. The source of such phenomena are antiresonant terms in the Hamiltonian, yet antiresonant interactions are typically negligible compared to resonant interactions in light-matter systems. We report an unusual coupled matter-matter system of magnons that can simulate a unique cavity QED Hamiltonian with coupling strengths that are easily tunable into the ultrastrong coupling regime and with dominant antiresonant terms. We found a novel regime where vacuum Bloch-Siegert shifts, the hallmark of antiresonant interactions, greatly exceed analogous frequency shifts from resonant interactions. Further, we theoretically explored the system's ground state and calculated up to 5.9 dB of quantum fluctuation suppression. These observations demonstrate that magnonic systems provide an ideal platform for simulating exotic quantum vacuum phenomena predicted in ultrastrongly coupled light-matter systems.

quant-ph↗