arXiv subjects

Hiroko Tokoro

Publications and source records attributed to Hiroko Tokoro.

8 recordsLinked to original sources

arXiv2026

Thermally quenched metastability in metal-insulator transitions via elemental substitution

Thermal quenching inhibits equilibration toward the thermodynamic ground state during phase transitions, revealing metastable phases such as structural glasses and quenched alloys. Whether such thermally quenched metastability can be realized in metal-insulator transitions has remained an open question because these transformations are governed by collective electronic reorganization rather than atomic diffusion. We demonstrate that rapid cooling exceeding 10$^9$ K s$^{-1}$ kinetically avoids the metal-insulator transition, stabilizing a long-lived metastable metallic phase in tungsten-substituted VO$_2$. Temperature-dependent relaxation reveals nucleation-dominated kinetics with a thermal activation barrier introduced by tungsten substitution. Our results establish elemental substitution as a route to thermally quenched metastability in metal-insulator transitions, expanding metastable phase control to electronic phases.

cond-mat.str-el↗

arXiv2026

Two pathways to break the insulating state in a correlated transition metal oxide

Correlated transition metal oxides present exciting prospects as switches or memory and storage devices owing to the possibility to control electronic properties using various external stimuli. While their complex behaviour is known to stem from interplay between electronic correlations, atomic structure and orbital physics, they remain poorly understood on the microscopic level. Here, we investigate such origins as a function of temperature and pressure in the transition metal oxide Ti3O5. We find that the insulating room-temperature phase is characterized by one-dimensional zig-zag chains composed by two types of titanium dimers forming orbital selective valence bonds. At the thermal phase transition, one type of titanium dimer breaks up, resulting in an insulator to metal transition with a large orbital repopulation between the two states. Moreover, optical spectroscopy reveals that an additional pressure-driven insulator to metal transition occurs in Ti3O5 at room temperature. The phenomenology of this novel pressure-induced metallic transition is completely different from the insofar studied transitions and results from a competition between intra- and inter-dimer hopping. Our combined results suggest that Ti3O5 is a prototypical correlated transition metal oxide, where both correlations as well as orbital interactions need to be considered to fully understand the evolution of the electronic states.

cond-mat.str-el↗

arXiv2020

Landau Theory for Non-Symmetry-Breaking Electronic Instability Coupled to Symmetry-Breaking Applied to Prussian Blue Analogue

Different types of ordering phenomena may occur during phase transitions, described within the universal framework of the Landau theory through the evolution of one, or several, symmetry-breaking order parameter h. In addition, many systems undergo phase transitions related to an electronic instability, in the absence of a symmetry-breaking and eventually described through the evolution of a totally symmetric order parameter q linearly coupled to volume change. Analyzing the coupling of a non-symmetry-breaking electronic instability, responsible for volume strain, to symmetry-breaking phenomena is of importance for many systems in nature and here we show that the symmetry-allowed qh2 coupling plays a central role. We use as case study the rubidium manganese hexacyanoferrate Prussian blue analogue, exhibiting phase transitions with hysteresis that may exceed 100 K, and based on intermetallic charge transfer (CT). During the phase transition, the intermetallic CT described through the evolution of q is coupled to cubic-tetragonal ferroelastic symmetry-breaking described through the evolution of h. In this system, the symmetry-breaking and non-symmetry breaking deformations have similar amplitudes but the large volume strain is mainly due to CT. We analyze both the ferroelastic and the CT features of the phase transition within the frame of the Landau theory, taking into account the qh2 coupling, stabilizing concomitant CT and Jahn-Teller distortion. The phase diagrams obtained with this model are in good qualitative agreement with various experimental findings and apply to diverse families of materials undergoing Mott transition, spin-crossover, neutral-ionic transition, for which isostructural electronic instability driving volume strain can couple to symmetry-breaking or not, create phase transition lines and drive cooperative phenomena.

cond-mat.mtrl-sci↗

arXiv2019

Detection of boson peak and fractal dynamics of disordered system using terahertz spectroscopy

Disordered systems exhibit universal excitation, referred to as the boson peak, in the terahertz region. Meanwhile, the so-called fracton is expected to appear in the nanoscale region owing to the self-similar structure of monomers in polymeric glasses. We demonstrate that such excitations can be detected using terahertz spectroscopy. For the interaction between terahertz light and the vibrational density of states of the fractal structure, we formulate an infrared light-vibration coupling coefficient for the fracton region. Accordingly, we show that information concerning fractal and fracton dimensions appears in the exponent of the absorption coefficient. Finally, using terahertz time-domain spectroscopy and low-frequency Raman scattering, we experimentally observe these universal excitations in a protein lysozyme system that has an intrinsically disordered and self-similar nature in a single supramolecule. These findings are applicable to disordered and polymeric glasses in general and will be key to understanding universal dynamics of disordered systems by terahertz light.

cond-mat.mtrl-sci↗

arXiv2009

Threshold Phenomena under Photo Excitation of Spin-crossover Materials with Cooperativity due to Elastic Interactions

Photo-induced switching from the low-spin state to the high-spin state is studied in a model of spin-crossover materials, in which long-range interactions are induced by elastic distortions due to different molecular sizes the two spin states. At a threshold value of the light intensity we observe nonequilibrium critical behavior corresponding to a mean-field spinodal point. Finite-size scaling of the divergence of the relaxation time is revealed by analysis of kinetic Monte Carlo simulations.

cond-mat.stat-mech↗

arXiv2007

Realization of the mean-field universality class in spin-crossover materials

In spin-crossover materials, the volume of a molecule changes depending on whether it is in the high-spin (HS) or low-spin (LS) state. This change causes distortion of the lattice. Elastic interactions among these distortions play an important role for the cooperative properties of spin-transition phenomena. We find that the critical behavior caused by this elastic interaction belongs to the mean-field universality class, in which the critical exponents for the spontaneous magnetization and the susceptibility are $β= 1/2$ and $γ= 1$, respectively. Furthermore, the spin-spin correlation function is a constant at long distances, and it does not show an exponential decay in contrast to short-range models. The value of the correlation function at long distances shows different size-dependences: $O(1/N)$, $O(1/\sqrt{N})$, and constant for temperatures above, at, and below the critical temperature, respectively. The model does not exhibit clusters, even near the critical point. We also found that cluster growth is suppressed in the present model and that there is no critical opalescence in the coexistence region. During the relaxation process from a metastable state at the end of a hysteresis loop, nucleation phenomena are not observed, and spatially uniform configurations are maintained during the change of the fraction of HS and LS. These characteristics of the mean-field model are expected to be found not only in spin-crossover materials, but also generally in systems where elastic distortion mediates the interaction among local states.

cond-mat.mtrl-sci↗

arXiv2007

Monte Carlo simulation of pressure-induced phase transitions in spin-crossover materials

Pressure-induced phase transitions of spin-crossover materials were simulated by a Monte Carlo simulation in the constant pressure ensemble for the first time. Here, as the origin of the cooperative interaction, we adopt elastic interaction among the distortions of the lattice due to the difference of the molecular sizes in different spin states, i.e., the high spin (HS) state and the low spin (LS) state. We studied how the temperature dependence of the ordering process changes with the pressure, and we obtained a standard sequence of temperature dependences that has been found in changing other parameters such as strength of the ligand field (S. Miyashita et al., Prog. Theor. Phys. \textbf{114}, 719 (2005)). Various effects of pressure on the spin-crossover ordering process are examined from a unified point of view.

cond-mat.mtrl-sci↗

arXiv2005

Structure of Metastable States in Phase Transitions with High-Spin Low-Spin Degree of Freedom

Difference of degeneracy of the low-spin (LS) and high-spin (HS) states causes interesting entropy effects on spin-crossover phase transitions and charge transfer phase transitions in materials composed of the spin-crossover atoms. Mechanisms of the spin-crossover (SC) phase transitions have been studied by using Wajnflasz model, where the degeneracy of the spin states (HS or LS) is taken into account and cooperative natures of the spin-crossover phase transitions have been well described. Recently, a charge transfer (CT) phase transition due to electron hopping between LS and HS sites has been studied by using a generalized Wajnflasz model. In the both systems of SC and CT, the systems have a high temperature structure (HT) and a low temperature structure (LT), and the change between them can be a smooth crossover or a discontinuous first order phase transition depending on the parameters of the systems. Although apparently the standard SC system and the CT system are very different, it is shown that both models are equivalent under a certain transformation of variables. In both systems, the structure of metastable state at low temperatures is a matter of interest. We study temperature dependence of fraction of HT systematically in a unified model, and find several structures of equilibrium and metastable states of the model as functions of system parameters. In particular, we find a reentrant type metastable branch of HT in a low temperature region, which would play an important role to study the photo-irradiated processes of related materials.

cond-mat.stat-mech↗