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BaTiO3 is a well-known piezoelectric material with commercial uses. The ferroelectric state of BaTiO3 generally comprises electrically polarized domains separated by domain walls (DWs). The DW alters local polarization vectors by an angle of 90° for 90° DW or 180° for 180° DW. The DW is crucial to piezoelectric properties such as response time and fatigue. Furthermore, the DW structure and its dynamics in BaTiO3 are not well understood. Hence, for the first time, we theoretically obtained the atomistic structure of the 90° DW via molecular dynamics simulations at 300 K with the core–shell interatomic potential, using a large-scale system with a side length of 2.8 × 10 3 Å. The width of the 90° DW thereby obtained was approximately 30 Å, which was 20 Å wider than that of the 180° DW. Under the external electric field E → ext parallel to the DW, we observed an extension of a domain having a polarization vector with a positive component along the E → ext -direction. The migration velocity of the 90° DW was approximately two times that of the 180° DW at the same E ext in the range 7 – 20 MV / m. For E ext ≥ 15 MV / m , the migration velocity of the 90° DW in the direction with a positive component along the polarization vector of the extending domain was substantially higher than that in the opposite direction. The physical causes of the difference in the migration velocities of the 90° DW in the two directions were analyzed. [ABSTRACT FROM AUTHOR]

Polarization switching in ferroelectric hysteresis of BaTiO3 proceeds by localized nucleation and subsequent growth of domains of reverse polarization. While this process is driven by the applied electric field, thermal activation can play an important role in domain nucleation. As a consequence of the stochastic nature of thermal activation, coercive fields in small systems exhibit a significant scatter. It is demonstrated that the statistics of coercive fields observed in molecular dynamics simulations is consistent with the statistical distribution expected for field-assisted thermally activated nucleation of reverse polarization domains. The excellent quantitative agreement between the simulation data and the theory of thermally activated processes provides strong evidence that polarization switching occurs by nucleation-and-growth rather than loss of the local minimum of the Gibbs free energy function. In a pristine crystal, switching is controlled by the field at which thermal fluctuations can create a critical nucleus in the bulk (homogeneous nucleation). The analysis of crystals with various vacancy-type defects demonstrates that such defects may enable heterogeneous nucleation at reduced fields. In both cases, the statistical analysis gives access to the respective activation energies, their field dependence, and the sizes of the critical nuclei. [ABSTRACT FROM AUTHOR]

BaTiO3 is a well-known piezoelectric material, which is widely used in various devices. In general, the ferroelectric state of BaTiO3 is composed of polarized domains. The growth of these domains due to an applied electric field or stress is related to the piezoelectric performance. We investigated the effects of various point defects, monovacancies {VBa, VTi, VO}, and first- and second-neighbor divacancies {VBa–VO, VTi–VO} on polarized domain growth in BaTiO3 under an applied electric field by molecular dynamics simulations using the core–shell inter-atomic potential. We found that (i) the first-neighbor divacancy VBa–VO is the most effective in assisting the domain growth under an applied electric field (i.e., a smaller coercive electric field) in an asymmetrical manner with respect to the electric field direction. This is mainly due to the creation of an electric field around VBa–VO by significant Ti shifts toward VBa with the assistance of VO. (ii) Domain growth proceeds in a 1 + 2 dimensional manner. The domain growth velocity in the direction of the applied electric field is approximately two orders of magnitude higher than that in the perpendicular direction. (iii) Increasing the density of the divacancy VBa–VO further lowers the coercive electric field when the applied electric field is parallel to the divacancy dipoles. The present results will be essential for designing the type, orientation, and density of defects to modify the coercive electric field of BaTiO3 in defect engineering. [ABSTRACT FROM AUTHOR]

The moving components of combustion engines are operated under harsh conditions of high pressures and temperatures. Extreme‐pressure anti‐wear additives, such as tricresyl phosphate (TCP), are mixed with base oil to prevent wear through the formation of a lubricant film on the substrate. We studied the effect of liquid pressure on the decomposition pathway of TCP in base oil molecules (2,5‐dimethylhexane) using hybrid quantum‐classical simulations with density functional theory for electrons. At a temperature of 300 K, we found that: (i) bond‐breaking barrier energies of both the OC and PO bonds of TCP decrease monotonically as the liquid pressure increases; (ii) the bond‐breaking barrier energy of PO is lower than that of OC at pressures of 0 and 2.0 GPa, but is higher at a pressure of 5.0 GPa; and (iii) the applied pressure significantly lowers the bond‐breaking barrier energies of both OC and PO when the PO bond of TCP is directed upward from the substrate. These findings are explained by the inhomogeneous distribution of base oil molecules around TCP and the steric repulsion of the PO bond of TCP. These results indicate that the internal structures of the lubricant films are pressure‐dependent. [ABSTRACT FROM AUTHOR]

We modeled the degradation of a composite produced from an amine-cured epoxy resin and SiO2 nanoparticles with a silane coupling agent (SCA) under wet conditions using electron-level simulations. For the epoxy region, the amine group is protonated depending on its location under neutral or acidic conditions. Protonation substantially weakens the amine C–N bond. For SCA-connected HO–SiO2, terminal –OH of SiO2 is deprotonated under neutral or alkaline conditions, and the energetic barrier to break the Si–O bond is < 1 eV when 50% of the terminal –OH is deprotonated. These findings support the experimental data on pH-dependent degradation. [ABSTRACT FROM AUTHOR]

Research describing surface structure stability and space-charge distribution in free anatase and rutile nanoparticles is presented. Two titanium dioxide nanospheres subject to sintering are examined by molecular dynamic simulation.

Research was conducted to develop an interatomic potential model for molecular-dynamics simulations of TiO2 (rutile) based on the formalism of FH Streitz and JW Mintmire in which atomic charges vary dynamically based on the generalized electronegativity equalization principle. The characteristic properties of the Ti-O bonding that play an important role in reproducing the macroscopic and microscopic quantities were elucidated using detailed analyses of the calculated electric-dipole oscillations.

Developing a composite material of polymers and micrometer-sized fillers with higher heat conductance is crucial to realize modular packaging of electronic components at higher densities. Enhancement mechanisms of the heat conductance of the polymer-filler interfaces by adding the surface-coupling agent in such a polymer composite material are investigated through the non-equilibrium molecular dynamics (MD) simulation. A simulation system is composed of α-alumina as the filler, bisphenol-A epoxy molecules as the polymers, and model molecules for the surface-coupling agent. The inter-atomic potential between the α-alumina and surface-coupling molecule, which is essential in the present MD simulation, is constructed to reproduce the calculated energies with the electronic density-functional theory. Through the non-equilibrium MD simulation runs, we find that the thermal resistance at the interface decreases significantly by increasing either number or lengths of the surface-coupling molecules and that the effective thermal conductivity of the system approaches to the theoretical value corresponding to zero thermal-resistance at the interface. Detailed analyses about the atomic configurations and local temperatures around the interface are performed to identify heat-transfer routes through the interface. [ABSTRACT FROM AUTHOR]

In this paper, we present time-reversible simulation algorithms for rigid bodies in the quaternion representation. By advancing a time-reversible algorithm [Y. Kajima, M. Hiyama, S. Ogata, and T. Tamura, J. Phys. Soc. Jpn. 80, 114002 (2011)] that requires iterations in calculating the angular velocity at each time step, we propose two kinds of iteration-free fast time-reversible algorithms. They are easily implemented in codes. The codes are compared with that of existing algorithms through demonstrative simulation of a nanometer-sized water droplet to find their stability of the total energy and computation speeds. [ABSTRACT FROM AUTHOR]

This paper reports a numerical simulation study about the chemical reactions of a nanosized water droplet inserted between H-terminated Si(001) surface and a nanosized, H-terminated diamond-tip when the tip is either slid on or pushed to the surface. The hybrid quantum-classical simulation method, in which the quantum region described with the density-functional theory is embedded in the total system of classical atoms, is used to perform the simulation runs in realistic settings. A feature to select the quantum region adaptively during the run is added to trace the time evolution of the contact area of the tip and surface. When the tip pushes the water droplet, while the Si surface interacts weakly with the water molecule, the tip draws a water molecule from the droplet into a unique metastable state in close proximity to the end of the tip. When the tip is further slid on or pushed to the Si surface, the water molecule in the metastable state decomposes due to high stresses concentrated at the contact area and oxidizes the surface if the molecule is trapped in a dimple structure of the surface. On the other hand, if the water molecule finds enough space between the tip and surface, it runs away without changing the bonding characteristics of both tip and surface. [ABSTRACT FROM AUTHOR]

A hybrid quantum-mechanical/molecular-dynamics simulation is performed to study the effects of environmental molecules on fracture initiation in silicon. A (110) crack under tension (mode-I opening) is simulated with multiple H 2 O molecules around the crack front. To accurately model the long-range stress field, the quantum-mechanical description is embedded in a large classical molecular-dynamics simulation. The hybrid simulation results show that the reaction of H 2 O molecules at a silicon crack tip is sensitive to the stress intensity factor K. For K 0.4 MPa. √ m, an H 2 O molecule either decomposes and adheres to dangling-bond sites on the crack surface or oxidizes Si, resulting in the formation of a Si-O-Si structure. For a higher K value of 0.5 MPa· m, an H 2 O molecule either oxidizes or breaks a Si-Si bond. [ABSTRACT FROM AUTHOR]

For the purpose of studying effect of environment molecules on fracture initiation in silicon using hybrid quantum-mechanical/molecular-dynamics simulation is described. The different simulation results for the environmental effect on fracture in semiconductor are detailed.

Diffusion of Li-ions in graphite is an essential elementary process in the current lithium-ion battery. The C-layers of graphite deform with Li due to relatively large size of Li-ion, act to confine the Li-ions, and thereby creates correlation between them. We address theoretically the thermal diffusivity of such correlated Li-ions in graphite by the hybrid quantum–classical simulation method. In this method, the quantum-region composed of the Li-ions and surrounding C atoms is treated by the density-functional theory, while it is embedded dynamically in the total system described with an empirical inter-atomic interaction potential. We thereby take into account the long-ranged deformation field in graphite in simulating the Li-ion dynamics. Two kinds of settings of Li-ions are considered for the simulation runs at temperature 443 K : (i) seven Li-ions are inserted in the same inter-layer space of the C-layers to study their intra-plane correlation, and (ii) additional seven Li-ions are inserted in the neighboring space (i.e., fourteen Li-ions totally, 7 Li-ions in upper and 7 Li-ions in lower spaces) to study their inter-plane correlation. As for (i), the Li-ions, concentrated initially with inter-ion distances of 2.5 – 4.2 Å , scatter due to their mutual Coulomb repulsion. After about 1 ps , the Li-ions and surrounding C atoms thermalize well with deformed C-layers creating a cage of radius about 13.5 Å for 7 Li-ions. Diffusivity of Li-ions inside the cage is much higher than that of the cage itself. The long-time diffusion constant of the cage is the same order as that of an isolated Li-ion in graphite. As for (ii), the Li-ions, concentrated initially in the upper and lower inter-layer spaces of the C-layer, firstly form domains, and then the domains repel each other horizontally. The result is in accord with the experimental finding that the Li-rich and Li-poor planes stack in an alternating sequence in graphite. [ABSTRACT FROM AUTHOR]

Using first-principles calculations, we have determined key properties of Ar and Ne in bcc W that relate to the possible bubble formation of implanted Ar and Ne atoms. The most stable interstitial site of Ar/Ne in bcc W is the tetrahedral site, as in the case of H and He. An interstitial atom causes the substantial strain of surrounding W atoms and the low electron-density region. The calculated migration energy of both Ar and Ne is very small, less than 0.2 eV of H. We calculated the binding energies of nearby interstitial atoms and found a strong dependence of atomic species. The attractive interaction between Ne atoms is the largest. Owing to such a small migration energy and a significant interaction between Ar/Ne atoms, interstitial atoms can act as traps for additional atoms and tend to form clusters in the absence of previous damage such as vacancies. The results presented here can explain the possible clustering of implanted atoms in bcc W via self-trapping. [ABSTRACT FROM AUTHOR]

Spectral features of MnK-edge x-ray absorption near-edge structure (XANES) for Li2MnO3 were calculated using the first-principles full projector augmented wave method with the general gradient approximation plus U method. We demonstrated that the U parameter affects the spectral features in the pre-edge region while it does not affect those in the major absorption region. From the comparison with the experimental spectra and those of reference compounds, we showed that the spectral features of MnK-edge XANES and the differences in the valence state can be reproduced well. [ABSTRACT FROM AUTHOR]

In hybrid electronic-density-functional/molecular-dynamics schemes, a total system is partitioned in real space into the quantum-mechanical (QM) region treated by the electronic-density-functional theory and the molecular dynamics (MD) region in which atoms are interacting through the empirical inter-atomic potential. In the former hybrid scheme [Ogata et al. Comput. Phys. Commun. 149 (2002) 30], appropriate selection of QM atoms for seamless coupling between the QM and MD regions is limited in Si systems, and applications of the scheme to other materials are difficult. Novel hybrid scheme that is free from the limitation and applicable to both Si and alumina systems, is presented. [Copyright &y& Elsevier]

A suite of scalable atomistic simulation programs has been developed for materials research based on space-time multiresolution algorithms. Design and analysis of parallel algorithms are presented for molecular dynamics (MD) simulations and quantum-mechanical (QM) calculations based on the density functional theory. Performance tests have been carried out on 1,088-processor Cray T3E and 1,280-processor IBM SP3 computers. The linear-scaling algorithms have enabled 6.44-billion-atom MD and 111,000-atom QM calculations on 1,024 SP3 processors with parallel efficiency well over 90%. production-quality programs also feature wavelet-based computational-space decomposition for adaptive load balancing, spacefilling-curve-based adaptive data compression with user-defined error bound for scalable I/O, and octree-based fast visibility culling for immersive and interactive visualization of massive simulation data. [ABSTRACT FROM AUTHOR]

The stability of surface structure and space-charge distribution in free TiO[sub 2] nanoparticles are investigated for both rutile and anatase phases using a variable-charge interaction potential in which atomic charges vary dynamically depending on their environment. We find the dynamic charge transfer: (i) enhances atomic diffusion at surfaces of the spherical nanoparticles at high temperatures; and (ii) creates additional repulsive force between the two nanospheres through formation of a double-charge surface layer in each nanosphere. The surface diffusion due to the charge transfer clearly distinguishes the two nanospheres with different underlying crystalline structures; the surface diffusion constant of the anatase sphere is almost three times as great as that of the rutile sphere. Variable-charge molecular dynamics simulations are then applied to sintering of two TiO[sub 2] nanospheres. It turns out that the enhanced surface diffusion in the anatase nanosphere at high temperatures significantly promotes neck formation between the two spheres. © 2000 American Institute of Physics. [ABSTRACT FROM AUTHOR]

Barium titanate (BaTiO3) is a ferroelectric material without toxic elements, whose ferroelectric properties such as permittivity, coercive field, and spontaneous polarization are affected by the nucleation of domains of reversed polarization and the motion of domain walls. Dislocations can act as obstacles to domain‐wall migration or as active sites for domain nucleation. Thus, studies are conducted on the utilization of dislocations to improve the ferroelectric properties of BaTiO3. However, the atomistic mechanism of domain nucleation around the dislocation core is still unclear. In this article, a machine learning (ML) potential is developed to study the influence of dislocations on domain nucleation. The potential is trained using an active‐learning approach to ensure accuracy in the bulk properties of the ferroelectric and paraelectric phases, as well as in the dislocation core structures in BaTiO3. Molecular dynamics simulations using the ML potential show that the influence of dislocations on polarization reversal depends on the directional relationship between the external electric field and the dislocation. Furthermore, strong local polarizations exist surrounding the dislocation core, owing to vacancies in the core. These polarizations can act as both domain nucleation sites and obstacles for domain migration when ordered along the dislocation line. [ABSTRACT FROM AUTHOR]

BaTiO3 (BT), a lead‐free ferroelectric material, is employed in energy‐conversion devices, including actuators and capacitors. However, its ferroelectric properties, such as the piezoelectric coefficient and Curie temperature, fall short of those of harmful lead‐based ferroelectrics, such as Pb(Zrx, Ti1−x)O3. In this study, a BT crystal is examined under biaxial strain (i.e., strain in the a‐ and b‐directions of the unit cell) to investigate the alterations in its ferroelectric properties. The piezoelectric coefficient, Curie temperature, polarization magnitude, and coercive electric field are calculated under varying biaxial strains using molecular dynamics simulations. The simulations utilize a core–shell‐type interatomic potential developed from first‐principles electronic structure calculations. In the findings, it is revealed that 1) the Curie temperature, polarization magnitude, and coercive electric field increase, whereas the piezoelectric coefficient in the c‐direction decreases under biaxial compression; 2) modifications in the ferroelectric properties depend on the area of ab‐plane and not on its aspect ratio. Comprehensive analyses of the Ti‐displacement distribution offer microscopic insights into strain‐induced shifts in ferroelectric properties. [ABSTRACT FROM AUTHOR]

The increment in minimum gate trigger current in a 4H-SiC commutated gate turn-off thyristor after the current stress test is investigated. The recombination at the intersection line of the Shockley-type stacking faults and the pn junction causes a reduction in the level of carrier injection from the anode to the gate. The current gain of the top pnp bipolar junction transistor, therefore, decreases, and the minimum gate trigger current increases. The minimum gate trigger current after the current stress test does not return to that before the current stress test at 200 °C, although the on-state voltage of the degraded thyristor returns to that of the original one when the temperature is increased to more than 150 °C. The Shockley-type stacking faults, which are parallel to the current flow from the anode to the gate and cause the increment in minimum gate trigger current, exist even if the temperature increases. [ABSTRACT FROM AUTHOR]