arXiv subjects

Takuma Shiga

Publications and source records attributed to Takuma Shiga.

At least 19 recordsLinked to original sources

arXiv2026

Anharmonic lattice dynamics study of phonon transport in layered and molecular-crystal indium iodides

Indium iodides, which adopt layered or molecular-crystal-like arrangements depending on composition, are expected to exhibit low lattice thermal conductivity because of their heavy constituent atoms and weak In-I bonding. In this work, we employed first-principles anharmonic lattice dynamics calculations to systematically investigate phonon transport in indium iodides from particle- and wave-like perspectives. The calculated lattice thermal conductivities of both materials remained below 1 W/m-K over a broad temperature range. Notably, the influence of wave-like phonon transport differed by composition: in InI3, the wave-like contribution became comparable to the particle-like Peierls contribution, whereas it remained negligible in InI. We also investigated the thermal transport properties of the experimentally reported high-pressure phase of InI3. Motivated by experimental indications of stacking faults and partial disorder in indium site occupancy within the rhombohedral phase, we constructed several ordered structural models with different stacking sequences. These stacking sequences exhibited no significant energetic preference and had similar lattice thermal conductivities, suggesting that in-plane thermal transport is largely governed by the vibrational properties of the In2I6 layers themselves rather than by the specific stacking sequence. These findings provide insight into phonon transport in layered and molecular-crystal systems with structural complexity and contribute to a broader understanding of thermal transport mechanisms in layered and molecular-crystal-like materials.

cond-mat.mtrl-sci↗

arXiv2025

Topological descriptor for interpretable thermal transport prediction in amorphous graphene

Understanding and predicting thermal transport in disordered materials remains a significant challenge due to the absence of periodicity and the complex nature of medium-range structural motifs. In this work, we investigate amorphous graphene and demonstrate that persistent homology, a topological data analysis technique, can serve as a physically interpretable structural descriptor for predicting thermal conductivity. We first show that ridge regression using persistent homology descriptors achieves high prediction accuracy. To gain physical insight into the prediction process, we perform inverse analysis by mapping the regression coefficients back onto the persistence diagrams. This reveals that distorted hexagonal and triangular motifs are strongly correlated with reduced thermal conductivity. A further comparison with the spatial distribution of localized vibrational modes supports the physical interpretation that these motifs suppress thermal transport. Our findings highlight that persistent homology not only enables accurate prediction of physical properties but also uncovers meaningful structure-property relationships in two-dimensional amorphous materials. This approach offers a promising framework for interpretable machine-learning models in materials science.

cond-mat.mtrl-sci↗

arXiv2025

Huge anisotropic magneto-thermal switching in high-purity polycrystalline compensated metals

Magneto-thermal transport is a promising physical property for thermal management applications. Magneto-thermal switching enables active control of heat flows, and a high switching ratio is desirable for improving performance. Here, we report on the observation of a huge magneto-thermal switching (MTS) effect in high-purity (5N) Pb polycrystalline wires, where magnetic fields perpendicular to the heat current direction are applied at low temperatures. At T = 3 K and B = 0.1 T, the measured thermal conductivity (\k{appa}) of the Pb wire is about 2500 W m-1 K-1 but is reduced to ~150 and ~5 W m-1 K-1 at B = 1 and 9 T, respectively. This strong suppression is attributed to magnetoresistance in compensated metals. Although the huge magnetoresistance has been studied in single crystals with field along the selected orbitals, our results demonstrate that a huge MTS can similarly be realized even in flexible polycrystalline wires. This finding highlights the practical potential of magneto-thermal control in low-temperature thermal management, including applications in space environments where temperatures are around 3 K.

cond-mat.mtrl-sci↗

arXiv2025

Study of magneto-thermal resistance effect in a Co50Fe50/Cu multilayer through the analysis of electron and lattice thermal conductivities

This study investigates the giant magneto-thermal resistance (GMTR) effect in a fully-bcc epitaxial Co50Fe50/Cu multilayer through both experimental and theoretical approaches. The applied magnetic field results in a giant change of the cross-plane thermal conductivity ({\Delta}\k{appa}) of 37 W m-1 K-1, which reaches 1.5 times larger than the previously reported value for a magnetic multilayer and record the highest value at room temperature among the other solid-state thermal switching materials working on different principles. We investigated the electron thermal conductivity for exploring the remarkable {\Delta}\k{appa} by the two-current-series-resistor model combined with the Wiedemann-Franz (WF) law. However, the result shows the electron contribution accounts for only 35% of the {\Delta}\k{appa}, indicating the presence of additional spin-dependent heat carriers. Further investigation of the lattice thermal conductivity, which is expected to be spin-independent, using non-equilibrium molecular dynamics (NEMD) simulations suggests a striking contrast: the additional spin-dependent heat carrier contribution is significantly enhanced in the parallel magnetization configuration but nearly negligible in the antiparallel configuration. These findings provide a fundamental insight into the origin of large GMTR effect and highlight its potential of active thermal management technologies for future electronic devices.

cond-mat.mtrl-sci↗

arXiv2022

Topological descriptor of thermal conductivity in amorphous materials

Quantifying the correlation between the complex structures of amorphous materials and their physical properties has been a long-standing problem in materials science. In amorphous Si, a representative covalent amorphous solid, the presence of a medium-range order (MRO) has been intensively discussed. However, the specific atomic arrangement corresponding to the MRO and its relationship with physical properties, such as thermal conductivity, remain elusive. Here, we solve this problem by combining topological data analysis, machine learning, and molecular dynamics simulations. By using persistent homology, we constructed a topological descriptor that can predict the thermal conductivity. Moreover, from the inverse analysis of the descriptor, we determined the typical ring features that correlated with both the thermal conductivity and MRO. The results provide an avenue for controlling the material characteristics through the topology of nanostructures.

cond-mat.mtrl-sci↗

arXiv2021

First-principles calculations of phonon transport across a vacuum gap

Phonon transport across a vacuum gap separating intrinsic silicon crystals is predicted via the atomistic Green's function method combined with first-principles calculations of all interatomic force constants. The overlap of electron wave functions in the vacuum gap generates weak covalent interaction between the silicon surfaces, thus creating a pathway for phonons. Phonon transport, dominated by acoustic modes, exceeds near-field radiation for vacuum gaps smaller than ~ 1 nm. The first-principles-based approach proposed in this work is critical to accurately quantify the contribution of phonon transport to heat transfer in the extreme near field.

cond-mat.mes-hall↗

arXiv2021

Surface phonons limit heat conduction in thin films

Understanding microscopic heat conduction in thin films is important for nano/micro heat transfer and thermal management for advanced electronics. As the thickness of thin films is comparable to or shorter than a phonon wavelength, phonon dispersion relations and transport properties are significantly modulated, which should be taken into account for heat conduction in thin films. Although phonon confinement and depletion effects have been considered, it should be emphasized that surface-localized phonons (surface phonons) arise whose influence on heat conduction may not be negligible due to the high surface-to-volume ratio. However, the role of surface phonons in heat conduction has received little attention thus far. In the present work, we performed anharmonic lattice dynamics calculations to investigate the thickness and temperature dependence of in-plane thermal conductivity of silicon thin films with sub-10-nm thickness in terms of surface phonons. Through systematic analysis of the influences of surface phonons, we found that anharmonic coupling between surface and internal phonons localized in thin films significantly suppresses overall in-plane heat conduction in thin films. We also discovered that specific low-frequency surface phonons significantly contribute to surface--internal phonon scattering and heat conduction suppression. Our findings are beneficial for the thermal management of electronics and phononic devices and may lead to surface phonon engineering for thermal conductivity control.

cond-mat.mtrl-sci↗

arXiv2021

Anisotropic Thermal Conductivity Measurement of Organic Thin Film with Bidirectional 3omega Method

Organic thin film materials with molecular ordering are gaining attention as they exhibit semiconductor characteristics. When using them for electronics, the thermal management becomes important, where heat dissipation is directional owning to the anisotropic thermal conductivity arising from the molecular ordering. However, it is difficult to evaluate the anisotropy by simultaneously measuring in-plane and cross-plane thermal conductivities of the film on a substrate, because the film is typically as thin as tens to hundreds of nanometers and its in-plane thermal conductivity is low. Here, we develop a novel bidirectional 3ω system that measures the anisotropic thermal conductivity of thin films by patterning two metal wires with different widths and preparing the films on top, and extracting the in-plane and cross-plane thermal conductivities using the difference in their sensitivities to the metal-wire width. Using the developed system, the thermal conductivity of spin-coated poly(3,4-ethylenedioxythiophene) olystyrene sulfonate (PEDOT:PSS) with thickness of 70 nm was successfully measured. The measured in-plane thermal conductivity of PEDOT:PSS film was as high as 2.9 W m-1 K-1 presumably due to the high structural ordering, giving anisotropy of 10. The calculations of measurement sensitivity to the film thickness and thermal conductivities suggest that the device can be applied to much thinner films by utilizing metal wires with smaller width.

physics.ins-det↗

arXiv2021

Extreme Near-Field Heat Transfer Between Gold Surfaces

Extreme near-field heat transfer between metallic surfaces is a subject of debate as the state-of-the-art theory and experiments are in disagreement on the energy carriers driving heat transport. In an effort to elucidate the physics of extreme near-field heat transfer between metallic surfaces, this Letter presents a comprehensive model combining radiation, acoustic phonon and electron transport across sub-10-nm vacuum gaps. The results obtained for gold surfaces show that in the absence of bias voltage, acoustic phonon transport is dominant for vacuum gaps smaller than ~2 nm. The application of a bias voltage significantly affects the dominant energy carriers as it increases the phonon contribution mediated by the long-range Coulomb force and the electron contribution due to a lower potential barrier. For a bias voltage of 0.6 V, acoustic phonon transport becomes dominant at a vacuum gap of 5 nm, whereas electron tunneling dominates at sub-1-nm vacuum gaps. The comparison of the theory against experimental data from the literature suggests that well-controlled measurements between metallic surfaces are needed to quantify the contributions of acoustic phonon and electron as a function of the bias voltage.

cond-mat.mes-hall↗

arXiv2019

One-directional thermal transport in densely aligned single-wall carbon nanotube films

Individual carbon nanotubes (CNTs) possess extremely high thermal conductivities. However, the thermal conductivities and their anisotropy of macroscopic assemblies of CNTs have so far remained small. Here, we report results of directional thermal transport measurements on a nearly-perfectly aligned CNT film fabricated via controlled vacuum filtration. We found the thermal conductivity to be 43 +- 2.2 W m^-1 K^-1 with a record-high thermal anisotropy of 500. From the temperature dependence of the thermal conductivity and its agreement with the atomistic phonon transport calculation, we conclude that the effect of intertube thermal resistance on heat conduction in the alignment direction is negligible because of the large contact area between CNTs. These observations thus represent ideal unidirectional thermal transport, i.e., the thermal conductivity of the film is determined solely by that of individual CNTs.

physics.app-ph↗

arXiv2018

Revisiting PbTe to identify how thermal conductivity is really limited

Due to the long range interaction in lead telluride (PbTe), the transverse optical (TO) phonon becomes soft around the Brillouin zone center. Previous studies have postulated that this zone-center softening causes the low thermal conductivity of PbTe through either enlarged phonon scattering phase space and/or strengthened lattice anharmonicity. In this work, we reported an extensive sensitivity analysis of the PbTe thermal conductivity to various factors: range and magnitude of harmonic and anharmonic interatomic force constants, and phonon wavevectors in the three-phonon scattering processes. The analysis reveals that the softening by long range harmonic interaction itself does not reduce thermal conductivity and it is the large magnitude of the anharmonic (cubic) force constants that realizes low thermal conductivity, however, not through the TO phonons around the zone center but dominantly through the ones with larger wavevectors in the middle of Brillion zone. The work clarifies that local band softening cannot be a direct finger print for low thermal conductivity and the entire Brillion zone needs to be characterized on exploring low thermal conductivity materials.

physics.comp-ph↗

arXiv2018

Ultimate confinement of phonon propagation in silicon nano-crystalline structure

Temperature-dependent thermal conductivity of epitaxial silicon nano-crystalline (SiNC) structures composed of nanometer-sized grains separated by ultra-thin silicon-oxide (SiO2) films is measured by the time domain thermoreflectance technique in the range from 50 to 300 K. Thermal conductivity of SiNC structures with grain size of 3 nm and 5 nm is anomalously low at the entire temperature range, significantly below the values of bulk amorphous Si and SiO2. Phonon gas kinetics model, with intrinsic transport properties obtained by first-principles-based anharmonic lattice dynamics and phonon transmittance across ultra-thin SiO2 films obtained by atomistic Green's function, reproduces the measured thermal conductivity without any fitting parameters. The analysis reveals that mean free paths of acoustic phonons in the SiNC structures are equivalent or even below half the phonon wavelength, i.e. the minimum thermal conductivity scenario. The result demonstrates that the nanostructures with extremely small length scales and controlled interface can give rise to ultimate classical confinement of thermal phonon propagation.

cond-mat.mes-hall↗

arXiv2017

Phonon-interference resonance effects in nanoparticles embedded in a matrix

We report an unambiguous phonon resonance effect originating from germanium nanoparticles embedded in silicon matrix. Our approach features the combination of phonon wave-packet method with atomistic dynamics and finite element method rooted in continuum theory. We find that multimodal phonon resonance, caused by destructive interference of coherent lattice waves propagating through and around the nanoparticle, gives rise to sharp and significant transmittance dips, blocking the lower-end frequency range of phonon transport that is hardly diminished by other nanostructures. The resonance is sensitive to the phonon coherent length, where the finiteness of the wave packet width weakens the transmittance dip even when coherent length is longer than the particle diameter. Further strengthening of transmittance dips are possible by arraying multiple nanoparticles that gives rise to the collective vibrational mode. Finally, it is demonstrated that these resonance effects can significantly reduce thermal conductance in the lower-end frequency range.

physics.comp-ph↗

arXiv2016

Effects of Defects on Thermoelectric Properties of Carbon Nanotubes

Carbon nanotubes (CNTs) have recently attracted attention as materials for flexible thermoelectric devices. To provide theoretical guideline of how defects influence the thermoelectric performance of CNTs, we theoretically studied the effects of defects (vacancies and Stone-Wales defects) on its thermoelectric properties; thermal conductance, electrical conductance, and Seebeck coefficient. The results revealed that the defects mostly strongly suppresses the electron conductance, and deteriorates the thermoelectric performance of a CNT. By plugging in the results and the intertube-junction properties into the network model, we further show that the defects with realistic concentrations can significantly degrade the thermoelectric performance of CNT-based networks. Our findings indicate the importance of the purification of CNTs for improving CNT-based thermoelectrics.

cond-mat.mes-hall↗

arXiv2016

Designing nanostructures for interfacial phonon transport via Bayesian optimization

We demonstrate optimization of thermal conductance across nanostructures by developing a method combining atomistic Green's function and Bayesian optimization. With an aim to minimize and maximize the interfacial thermal conductance (ITC) across Si-Si and Si-Ge interfaces by means of Si/Ge composite interfacial structure, the method identifies the optimal structures from calculations of only a few percent of the entire candidates (over 60,000 structures). The obtained optimal interfacial structures are non-intuitive and impacting: the minimum-ITC structure is an aperiodic superlattice that realizes 50% reduction from the best periodic superlattice. The physical mechanism of the minimum ITC can be understood in terms of crossover of the two effects on phonon transport: as the layer thickness in superlattice increases, the impact of Fabry-Pérot interference increases, and the rate of reflection at the layer-interfaces decreases. Aperiodic superlattice with spatial variation in the layer thickness has a degree of freedom to realize optimal balance between the above two competing mechanism. Furthermore, aperiodicity breaks the constructive phonon interference between the interfaces inhibiting the coherent phonon transport. The present work shows the effectiveness and advantage of material informatics in designing nanostructures to control heat conduction, which can be extended to other interfacial structures.

cond-mat.mtrl-sci↗

arXiv2016

Thermal conductivity spectrum calculation from first-principles-based harmonic phonon theory

In recent years, nanostructuring of dielectric and semiconducting crystals has enhanced controllability of their thermal conductivity. To carry out computational material search for nanostructured materials with desirable thermal conductivity, a key property is the thermal conductivity spectrum of the original single crystal, which determines the appropriate length scale of nanostructures and mutual adaptability of different kinds of nanostructures. Although the first-principles phonon transport calculations have become accessible, the anharmonic lattice dynamics calculations are still heavy to scan many materials. To this end, we have developed an empirical model that describes the thermal conductivity spectrum in terms only of harmonic phonon properties and bulk thermal conductivity. The model was tested for several crystals with different structures and thermal conductivities, and was confirmed to reproduce the overall profiles of thermal conductivity spectra and their anharmonic calculations.

cond-mat.mes-hall↗

arXiv2015

Phonon transport in perovskite SrTiO3 from first principles

We investigate phonon transport in perovskite strontium titanate (SrTiO3) which is stable above its phase transition temperature (~105 K) by using first-principles molecular dynamics and anharmonic lattice dynamics. Unlike conventional ground-state-based perturbation methods that give imaginary phonon frequencies, the current calculation reproduces stable phonon dispersion relations observed in experiments. We find the contribution of optical phonons to overall lattice thermal conductivity is larger than 60%, markedly different from the usual picture with dominant contribution from acoustic phonons. The mode- and pseudopotential-dependence analysis suggests the strong attenuation of acoustic phonons transport originated from strong anharmonic coupling with the transversely-polarized ferroelectric modes.

physics.comp-ph↗

arXiv2015

Origin of anomalous anharmonic lattice dynamics of lead telluride

The origin of the anomalous anharmonic lattice dynamics of lead telluride is investigated using molecular dynamics simulations with interatomic force constants (IFCs) up to quartic terms obtained from first principles. The calculations reproduce the peak asymmetry of the radial distribution functions and the double peaks of transverse optical phonon previously observed with neutron diffraction and scattering experiments. They are identified to be due to the extremely large nearest-neighbor cubic IFCs in the [100] direction. The outstanding strength of the nearest-neighbor cubic IFCs relative to the longer-range ones explains the reason why the distortion in the radial distribution function is local.

physics.comp-ph↗