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Despite increasing demands for the thermodynamic data of liquids in a wide range of science and engineering fields, there is a still a considerable lack of reliable data over a wide range of temperature ($T$) and pressure conditions. The most significant obstacle is that there is no practical method to calculate the entropy ($S$) of liquids. This problem can be solved using the thermodynamic definition of entropy, i.e., $S = \int C d\ln T$, where $C$ is specific heat. The specific heat is calculated by the derivative of the internal energy $U$ with respect to $T$. Both quantities, i.e., $U$ and $T$, are well defined in the molecular dynamics (MD) simulations based on density functional theory. The reliability of the present method is entirely dependent on the accuracy of the specific heat of liquid, for which there is no standard model. The problem with liquids is that there are no eigenstates, based on which the standard procedures are constructed. The relationship between $U$ and $T$ is affected by the energy relaxation processes, the effect of which appears in the $T$ dependence on the specific heat of liquids. This motivates us to conduct MD simulations by isolating the system from an external heat bath. In this paper, by applying this method to the liquid sodium, it is demonstrated that the experimental $T$ dependence of the isochoric specific heat is reproduced well without any empirical parameter. On this basis, the entropy of the liquid Na is obtained with a good agreement with experimental values.

Although the melting temperature, $T_{m}$, of a solid can be calculated based on first-principles molecular dynamics (FP-MD) simulations, systematic assessments of the accuracy of the resulting values have not yet been reported. FP-MD simulations require significant computational resources and hence an examination of the effect of cell size on convergence is difficult. In addition, calculation of the energy of a liquid is not a trivial problem because of energy dissipation effects. The present work attempts to resolve these problems, and thus allow the accuracy of $T_{m}$ values obtained from FP-MD simulations to be assessed for typical semiconductors, metals, and oxides. With the exception of Si, the $T_{m}$ value was overestimated in all cases. This overestimation can be reduced by increasing the cell size, although the convergence is slow unless the potential is very shallow. For oxides, this overestimation may not be removed by increasing the cell size. The LDA/GGA error of overbinding affects the melting enthalpy and thereby $T_{m}$. In order to fully capture the energy dissipation nature of liquids, adiabatic MD simulations are required, and such simulations have been performed in the present study.

We present a method to determine the model Hamiltonians to treat rare-earth multiplets in solids from the results of the quasiparticle self-consistent \textit{GW} (QSGW) method. We apply the method to trivalent Eu compounds EuCl$_3$, EuN, and Eu-doped GaN after examining free rare-earth ions. We solve the model Hamiltonian by the exact diagonalization. Our results justify applying the Dieke diagram to ions in solid, while its limitation is clarified. In particular, we show that the crystal fields cause sizable breaking of the Russell-Saunders coupling., Comment: 7 pages, 3 figures, 2 tables

It is well known that the temperature dependence of the effective magnetocrystalline anisotropy energy obeys the $l(l+1)/2$ power law of magnetization in the Callen-Callen theory. Therefore, according to the Callen-Callen theory, the magnetocrystalline anisotropy energy is assumed to be zero at the critical temperature where the magnetization is approximately zero. This study estimates the temperature dependence of the magnetocrystalline anisotropy energy by integrating the magnetization versus magnetic field ($M$--$H$) curves, and found that the magnetocrystalline anisotropy is still finite even above the Curie temperature in the uniaxial anisotropy, whereas this does not appear in the cubic anisotropy case. The origin is the fast reduction of the anisotropy field, which is the magnetic field required to saturate the magnetization along the hard axis, in the case of cubic anisotropy. Therefore, the magnetization anisotropy and anisotropic magnetic susceptibility, those are the key factors of magnetic anisotropy, could not be established in the case of cubic anisotropy. In addition, the effect of magnetocrystalline anisotropy on magnetocaloric properties, as the difference between the entropy change curves of AlFe$_{2}$B$_{2}$ appears above the Curie temperature, which is in good agreement with a previous experimental study. This is proof of magnetic anisotropy at slightly above Curie temperature.

The mobility and disorder in the lattice of Cu atoms as liquid-like behavior is an important characteristic affecting the thermoelectric properties of Cu$_{2}$S. In this study, using a theoretical model called acanthite-like structure for Cu$_{2}$S at a low-temperature range, we systematically investigate the electronic structure, intrinsic defect formation, and transport properties by first-principles calculations. Thereby, previous experimental reports on the indirect bandgap nature of Cu$_{2}$S were confirmed in this work with an energy gap of about 0.9-0.95 eV. As a result, the optical absorption coefficient estimated from this model also gives a potential value of $\alpha > 10^{4}$ cm$^{-1}$ in the visible spectrum range. According to the bonding analysis and formation energy aspect, Cu vacancy is the most preferred defect to form in Cu$_{2}$S, which primarily affects the conductive behavior as a $p$-type, as experimentally observed. Finally, the transport properties of Cu$_{2}$S system were successfully reproduced using an electron-phonon scattering method, highlighting the important role of relaxation time prediction in conductivity estimation instead of regarding it as a constant., Comment: 10 pages

We introduce a new extended Heisenberg model. The model contains the orbital-dependent spins together with the retarded effects of spin torque. The model is directly derived from the dynamical linear response functions on the transversal spin fluctuation. Our model allows us to address effects which are not accessible via the usual Heisenberg model. With the model, we can describe not only the relaxation effects due to the Landau damping caused by the Stoner excitations, but also the nesting effects of the Fermi surface. We discuss possibilities of the extended Heisenberg model based on the high-resolution plots of the spin susceptibility for Fe.

High $ZT$ value and large Seebeck coefficient have been reported in the nanostructured Fe-doped Si-Ge alloys. In this work, the large Seebeck coefficient in Fe-doped Si-Ge systems is qualitatively reproduced from the computed electronic density of states, where a hybrid functional, HSE06, is used for an exchange-correlation functional, as well as a special quasi-random structure (SQS) for a disordered atomic configuration. Furthermore, by replacing Fe with other transition metals, such as Mn, Co, Ni, Cu, Zn, and Au, a better dopant that produces a larger Seebeck coefficient in Si-Ge alloy systems is explored., Comment: 6 pages

We calculate transverse spin susceptibility in the linear response method based on the ground states determined in the quasi-particle self-consistent $GW$ (QSGW) method. Then we extract spin wave (SW) dispersions from the susceptibility. We treat bcc Fe, hcp Co, fcc Ni, and B2-type FeCo. Because of the better description of the independent-particle picture in QSGW, calculated spin stiffness constants for Fe, Co, and Ni give much better agreement with experiments in QSGW than that in the local density approximation (LDA), where the stiffness for Ni in LDA is two times bigger than the experiment. For Co, both acoustic and optical branches of SWs agree with the experiment. As for FeCo, we have some discrrepancy between the spin stiffness in QSGW and that in the experiment. We may need further theoretical and experimental investigations on the discrepancy., Comment: 10 pages, 9 figures

We have recently implemented a new version of the quasiparticle self-consistent GW (QSGW) method in the ecalj package released at http://github.com/tkotani/ecalj. Since the new version of the ecalj is numerically stable and accurate compared to the previous versions, we can perform calculations easily without being bothered with setting input parameters. Here we examine its ability to describe energy band properties, e.g., band-gap energy, eigenvalues at special points and effective mass, for variety of semiconductors and insulators. We treat C, Si, Ge, Sn, SiC (in 2H, 3C, and 4H structures), (Al, Ga, N)x(N, P, As, Pb), (Zn, Cd, Mg)x(O, S, Se, Te), SiO2, HfO2, ZrO2, SrTiO3, PbS, PbTe, MnO, NiO, and HgO. We propose that a hybrid QSGW method, where we mix 80 percent of QSGW and 20 percent of LDA, gives universally good agreement with experiments for these materials., Comment: 8 pages, 3 figures, 4 tables

The prospects of half-metallic ferromagnetism being induced by the incorporation of C atoms into alkaline-earth-metal-oxides are investigated by the first principle calculation. The origin of the ferromagnetism is discussed through the calculation of the electronic structure and exchange coupling constant by using the pseudo-potential-like self-interaction-corrected local spin density method. The Curie temperature ($T_c$) is also predicted by employing the Monte Carlo simulation. It is shown that by taking the electron self-interaction into account, the half-metallic ferromagnetism induced by C in the host materials is more stabilized in comparison with the standard LDA case, and the C's $2p$ electron states in the bandgap become more localized resulting in the predominance of the short-ranged exchange interaction. While the ferromagnetism in MgO$_{1-x}$C$_x$ is stabilized due to the exchange interaction of the $1st$-nearest neighbor pairs and might be suppressed by the anti-ferromagnetic super-exchange interaction at higher $x$, the ferromagnetism in CaO$_{1-x}$C$_x$, SrO$_{1-x}$C$_x$, and BaO$_{1-x}$C$_x$ is stabilized by both the $1st$- and $2nd$-nearest neighbor pairs, and $T_c$ monotonously increases with the C concentration., Comment: 5 pages, 5 figures

We present a first principle study of new class of high-$T_c$ half-heusler ferromagnets NiCrZ (Z = Si, P, Ge, As, Te). The structure and magnetic properties are investigated through the calculation of the electronic structure, equilibrium lattice constant, magnetic exchange interaction $J_{ij}$ and Curie temperature $T_c$. The role of $sp$-elements and the influence of lattice expansion/compression are also studied. In alloys having 20 valence electrons, a pseudo-gap of the majority band can be formed at Fermi level. Otherwise, the half-metallicity and ferromagnetism at temperatures much higher than room temperature are found to be stable in a wide range of lattice expansion. Based on these results, NiCrZ can be expected to be promising materials for spintronics., Comment: 10 pages, 3 figures

Based on the first principle calculation, we propose a new class of high-$T_c$ half-heusler ferromagnets NiMnZ (Z = Si, P, Ge, As). The structural and magnetic properties are investigated through the calculation of the electronic structure, phase stability, equilibrium lattice constant, magnetic exchange interaction $J_{ij}$ and Curie temperature $T_c$. It is found that all alloys show half-metallicity and ferromagnetism at temperatures much higher than room temperature in a wide range of lattice expansion (compression). At the equilibrium lattice constant, $T_c$ of 715K, 840K, 875K and 1050K are predicted by Monte Carlo simulation for NiMnP, NiMnAs, NiMnGe and NiMnSi, respectively. Following these results, these alloys are strongly expected to be promising candidates for spintronic applications., Comment: 6 pages, 6 figures