arXiv subjects

Shintaro Kobayashi

Publications and source records attributed to Shintaro Kobayashi.

7 recordsLinked to original sources

arXiv2026

Time-Temperature-Transformation (TTT) Diagrams to rationalize the nucleation and quenchability of metastable $α$-Li$_3$PS$_4$

$α$-Li$_3$PS$_4$ is a promising solid-state electrolyte with the highest ionic conductivity among its polymorphs. However, its formation presents a thermodynamic paradox: the $α$-phase is the equilibrium phase at high temperature and transforms to the stable $γ$-Li$_3$PS$_4$ polymorph when cooled to room temperature; however, $α$-Li$_3$PS$_4$ can be synthesized and quenched in a metastable state via rapid heating at relatively low temperatures. The origin of this synthesizability and anomalous stability has remained elusive. Here, we resolve this paradox by establishing a comprehensive time-temperature-transformation (TTT) diagram, constructed from a computational temperature-size phase diagram and experimental high-time-resolution isothermal measurements. Our density functional theory calculations reveal that at the nanoscale, the $α$-phase is stabilized by its low surface energy, which drastically lowers the nucleation barrier across a wide temperature range. This size-dependent stabilization is directly visualized using in-situ synchrotron X-ray diffraction and electron microscopy, capturing the rapid nucleation of nano-sized $α$-phase and its subsequent slow transformation. This work presents a generalizable framework that integrates thermodynamic and kinetic factors for understanding nucleation and phase transformation mechanisms, providing a rational strategy for the targeted synthesis of functional metastable materials.

cond-mat.mtrl-sci↗

arXiv2025

Control of Covalent Bond Enables Efficient Magnetic Cooling

Magnetic cooling, harnessing the temperature change in matter when exposed to a magnetic field, presents an energy-efficient and climate-friendly alternative to traditional vapor-compression refrigeration systems, with a significantly lower global warming potential. The advancement of this technology would be accelerated if irreversible losses arising from hysteresis in magnetocaloric materials were minimized. Despite extensive efforts to manipulate crystal lattice constants at the unit-cell level, mitigating hysteresis often compromises cooling performance. Herein, we address this persistent challenge by forming Sn(Ge)3/Sn(Ge)3 bonds within the unit cell of the Gd5Ge4 compound. Our approach enables an energetically favorable phase transition, leading to the elimination of thermal hysteresis. Consequently, we achieve a synergistic improvement of two key magnetocaloric figures of merit: a larger magnetic entropy change and a twofold increase in the reversible adiabatic temperature change (from 3.8 to 8 K) in the Gd5Sn2Ge2 compound. Such synergies can be extended over a wide temperature range. This study demonstrates a paradigm shift in mastering hysteresis toward simultaneously achieving exceptional magnetocaloric metrics and opens up promising avenues for gas liquefaction applications in the longstanding pursuit of sustainable energy solutions.

cond-mat.mtrl-sci↗

arXiv2025

Impact of in-plane disorders on the thermal conductivity of AgCrSe$_2$

Superionic conductors have recently attracted renewed attention for their use as thermoelectric materials due to their extremely low lattice thermal conductivity. Of central interest is why the superionic conductors exhibit such low thermal conductivity, and competing mechanisms have been proposed thus far. In this study, we investigate the effects of Cu and Au substitution for Ag site on the crystal structure and thermal properties of AgCrSe$_2$, which exhibits superionic conduction of Ag ions. We show that Au substitution significantly reduces the lattice thermal conductivity of AgCrSe$_2$. Powder structure analysis using synchrotron x-ray diffraction reveals that Au substitution increases the anisotropic atomic displacement parameter of Ag ions along the $a$ and $b$ axes. This result indicates that the amplitude of in-plane vibrations is enhanced, which is attributed to increased anharmonicity in the potential energy around Ag ions. The enhanced vibrational amplitude also suggests a reduction in the force constants between Ag ions. Consequently, the enhanced anharmonicity not only shortens the phonon lifetime ($τ$) by increasing phonon-phonon scattering, but also increases the number of low-energy phonons, which further contributes to the reduction of $τ$. This anharmonicity mechanism is applicable to other superionic conductors exhibiting ultra-low thermal conductivity, promoting their widespread use as thermoelectric materials.

cond-mat.mtrl-sci↗

arXiv2023

Pressure-induced structural phase transition and new superconducting phase in UTe2

We report on the crystal structure and electronic properties of the heavy fermion superconductor UTe2 at high pressure up to 11 GPa, as investigated by X-ray diffraction and electrical resistivity experiments. The X-ray diffraction measurements under high pressure using a synchrotron light source reveal anisotropic linear compressibility of the unit cell up to 3.5 GPa, while a pressure-induced structural phase transition is observed above 3.5-4GPa at room temperature, where the body-centered orthorhombic crystal structure with the space group Immm changes into a body-centered tetragonal structure with the space group I4/mmm. The molar volume drops abruptly at the critical pressure, while the distance between the first-nearest neighbor of U atoms increases, implying a switch from the heavy electronic states to the weakly correlated electronic states. Surprisingly, a new superconducting phase at pressures higher than 7 GPa was detected at Tsc above 2K with a relatively low upper-critical field, Hc2(0). The resistivity above 3.5GPa, thus, in the high-pressure tetragonal phase, shows a large drop below 230 K, which may also be related to a considerable change from the heavy electronic states to the weakly correlated electronic states.

cond-mat.str-el↗

arXiv2021

Slow dynamics of disordered zigzag chain molecules in layered LiVS2 under electron irradiation

Electronic instabilities in transition metal compounds often spontaneously form orbital molecules, which consist of orbital-coupled metal ions at low temperature. Recent local structural studies utilizing the pair distribution function revealed that preformed orbital molecules appear disordered even in the high-temperature paramagnetic phase. However, it is unclear whether preformed orbital molecules are dynamic or static. Here, we provide clear experimental evidence of the slow dynamics of disordered orbital molecules realized in the high-temperature paramagnetic phase of LiVS2, which exhibits vanadium trimerization upon cooling below 314 K. Unexpectedly, the preformed orbital molecules appear as a disordered zigzag chain that fluctuate in both time and space under electron irradiation. Our findings should advance studies on soft matter physics realized in an inorganic material due to disordered orbital molecules.

cond-mat.str-el↗

arXiv2020

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↗

arXiv2019

Effect of Cu intercalation and pressure on excitonic interaction in 1T-TiSe2

1T-TiSe2 has a semimetallic band structure at room temperature and undergoes phase transition to a triple-q charge density wave (CDW) state with a commensurate superlattice structure (2a * 2a * 2c) below Tc ~ 200 K at ambient pressure. This phase transition is caused by cooperative phenomena involving electron-phonon and electron-hole (excitonic) interactions, and cannot be described by a standard CDW framework. By Cu intercalation or the application of pressure, this phase transition temperature is suppressed and superconductivity (SC) appears. However, it is not clear what kind of order parameters are affected by these two procedures. We investigated the crystal structure of CuxTiSe2 and pressurized 1T-TiSe2 around the SC state by synchrotron x-ray diffraction on single crystals. In the high-temperature phase, the variation of structural parameters for the case of Cu intercalation and application of pressure are considerably different. Moreover, the relationship between the critical points of the CDW phase transition and the SC dome are also different for the two cases. The excitonic interaction appears to play an important role in the P-T phase diagram of 1T-TiSe2, but not in the x-T phase diagram.

cond-mat.str-el↗