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The enthalpy of mixing in the liquid phase is a thermodynamic property reflecting interactions between elements that is key to predict phase transformations. Widely used models exist to predict it, but they have never been systematically evaluated. To address this, we collect a large amount of enthalpy of mixing data in binary liquids from a review of about 1000 thermodynamic evaluations. This allows us to clarify the prediction accuracy of Miedema's model which is state-of-the-art. We show that more accurate predictions can be obtained from a machine learning model based on LightGBM, and we provide them in 2415 binary systems. The data we collect also allows us to evaluate another empirical model to predict the excess heat capacity that we apply to 2211 binary liquids. We then extend the data collection to ternary metallic liquids and find that, when mixing is exothermic, extrapolations from the binary systems by Muggianu's model systematically lead to slight overestimations of roughly 10% close to the equimolar composition. Therefore, our LightGBM model can provide reasonable estimates for ternary alloys and, by extension, for multicomponent alloys. Our findings extracted from rich datasets can be used to feed thermodynamic, empirical and machine learning models for material development., Comment: Manuscript: 27 pages, 5 figures ; Supplementary notes: 3 pages, 5 figures

Sublattices A and B are opposite in the decay direction of the edge state of the zigzag graphene ribbon (ZGR). Detecting exponential growth from the zigzag edges to the ZGR center remains challenging. The tight-binding model calculations in this letter reveal that interlayer conductance manifests this growth in parallel contact with the armchair nanotube. The transfer integrals of oblique interlayer bonds are comparable to those of vertical interlayer bonds. However, the phase of the ZGR wave function strongly suppresses the contribution of oblique bonds, allowing the selective detection of the growing component., Comment: 13 pages, 5 Figures

The tunnel current (TC) and valley current (VC) are crucial in realizing high-speed and energy-saving in next-generation devices. This paper presents the TC and VC link in the partially overlapped graphene. Under the vertical electric field, the two graphene layers have the opposite AB sublattice symmetry, followed by a block on the intravalley transmission. In the allowed intervalley transmission, the difference in the phase of the decay factor prefers only one of the valleys in the output according to the overlapped length. These results suggest that the band gap with no edge state is a new platform of valleytronics., Comment: 14 pages, 4 figures

Despite the attempts to apply a quantum annealer to Boltzmann sampling, it is still impossible to perform accurate sampling at arbitrary temperatures. Conventional distribution correction methods such as importance sampling and resampling cannot be applied, because the analytical expression of sampling distribution is unknown for a quantum annealer. Stein correction (Liu and Lee, 2017) can correct the samples by weighting without the knowledge of the sampling distribution, but the naive implementation requires the solution of a large-scale quadratic program, hampering usage in practical problems. In this letter, a fast and approximate method based on random feature map and exponentiated gradient updates is developed to compute the sample weights, and used to correct the samples generated by D-Wave quantum annealers. In benchmarking problems, it is observed that the residual error of thermal average calculations is reduced significantly. If combined with our method, quantum annealers may emerge as a viable alternative to long-established Markov chain Monte Carlo methods., Comment: 5 pages, 2 figures

NIMS-OS (NIMS Orchestration System) is a Python library created to realize a closed loop of robotic experiments and artificial intelligence (AI) without human intervention for automated materials exploration. It uses various combinations of modules to operate autonomously. Each module acts as an AI for materials exploration or a controller for a robotic experiments. As AI techniques, Bayesian optimization (PHYSBO), boundless objective-free exploration (BLOX), phase diagram construction (PDC), and random exploration (RE) methods can be used. Moreover, a system called NIMS automated robotic electrochemical experiments (NAREE) is available as a set of robotic experimental equipment. Visualization tools for the results are also included, which allows users to check the optimization results in real time. Newly created modules for AI and robotic experiments can be added easily to extend the functionality of the system. In addition, we developed a GUI application to control NIMS-OS.To demonstrate the operation of NIMS-OS, we consider an automated exploration for new electrolytes. NIMS-OS is available at https://github.com/nimsos-dev/nimsos., Comment: 29 pages, 5 figures, 2 tables

Using the tight-binding model, we investigate the valley current of the `low-bi-up' and `low-bi-low' graphene junction, where `low' and `up' are respectively the lower and upper graphene layers extended from the central AB stacking bilayer graphene layer, `bi'. Source and drain electrodes connect with the left and right monolayer regions, respectively, and thus the total current is forced to flow through the interlayer path in the low-bi-up junction. We measure valley current reversal (VCR) using the average of $\frac{1}{2} \sum_{\nu =\pm}(T_{\nu,-\nu}-T_{\nu,\nu})$ per lateral wave number, where $T_{\nu,\nu'}$ denotes the electron transmission rate from the left $K_{\nu'}$ valley to the right $K_{\nu}$ valley. Without the vertical electric field, the VCR is less than half in both junctions. This VCR is attributed to monolayer--bilayer matching. As the vertical field intensifies, the VCR declines in the low-bi-low junction, but increases to about 0.8 in the low-bi-up junction. This VCR enhancement originates from interlayer matching. Analytic scattering matrixes elucidate these matching effects. Experiments of VCR detection are also proposed., Comment: 39 pages, 17 figures

Black-box optimization has potential in numerous applications such as hyperparameter optimization in machine learning and optimization in design of experiments. Ising machines are useful for binary optimization problems because variables can be represented by a single binary variable of Ising machines. However, conventional approaches using an Ising machine cannot handle black-box optimization problems with non-binary values. To overcome this limitation, we propose an approach for integer-variable black-box optimization problems by using Ising/annealing machines and factorization machines in cooperation with three different integer-encoding methods. The performance of our approach is numerically evaluated with different encoding methods using a simple problem of calculating the energy of the hydrogen molecule in the most stable state. The proposed approach can calculate the energy using any of the integer-encoding methods. However, one-hot encoding is useful for problems with a small size., Comment: 12 pages, 5 figures

Knowledge of phase diagrams is essential for material design as it helps in understanding microstructure evolution during processing. The determination of phase diagrams is thus one of the central tasks in materials science. When exploring new materials for which the phase diagram is unknown, experimentalists often try to determine the key experiments that should be performed by referencing known phase diagrams of similar systems. To enhance this practical strategy, we attempted to estimate unknown phase diagrams based on known phase diagrams using a machine learning-based classification approach. As a proof of concept, we focused on predicting the number of coexisting phases across the 800 K isothermal section of each of the 10 ternaries of the Al-Cu-Mg-Si-Zn system from the other 9 sections. To increase the prediction accuracy, we introduced new descriptors generated from the thermodynamic properties of the elements and CALPHAD extrapolations from lower-order systems. Using the random forest method, the presence of single-, two-, and three-phase domains was predicted with an average accuracy of 84% across all 10 considered sections with a standard deviation of 11%. The proposed approach represents a promising tool for assisting the investigator in developing new materials and determining phase equilibria efficiently., Comment: Manuscript: 29 pages (double-spaced), 6 figures. Supplementary notes: 19 pages, 13 figures

PHYSBO (optimization tools for PHYSics based on Bayesian Optimization) is a Python library for fast and scalable Bayesian optimization. It has been developed mainly for application in the basic sciences such as physics and materials science. Bayesian optimization is used to select an appropriate input for experiments/simulations from candidate inputs listed in advance in order to obtain better output values with the help of machine learning prediction. PHYSBO can be used to find better solutions for both single and multi-objective optimization problems. At each cycle in the Bayesian optimization, a single proposal or multiple proposals can be obtained for the next experiments/simulations. These proposals can be obtained interactively for use in experiments. PHYSBO is available at https://github.com/issp-center-dev/PHYSBO., Comment: 12 pages, 6 figures

Owing to the advances in computational techniques and the increase in computational power, atomistic simulations of materials can simulate large systems with higher accuracy. Complex phenomena can be observed in such state-of-the-art atomistic simulations. However, it has become increasingly difficult to understand what is actually happening and mechanisms, for example, in molecular dynamics (MD) simulations. We propose an unsupervised machine learning method to analyze the local structure around a target atom. The proposed method, which uses the two-step locality preserving projections (TS-LPP), can find a low-dimensional space wherein the distributions of datapoints for each atom or groups of atoms can be properly captured. We demonstrate that the method is effective for analyzing the MD simulations of crystalline, liquid, and amorphous states and the melt-quench process from the perspective of local structures. The proposed method is demonstrated on a silicon single-component system, a silicon-germanium binary system, and a copper single-component system., Comment: 16 pages, 13 figures

A black-box optimization algorithm such as Bayesian optimization finds extremum of an unknown function by alternating inference of the underlying function and optimization of an acquisition function. In a high-dimensional space, such algorithms perform poorly due to the difficulty of acquisition function optimization. Herein, we apply quantum annealing (QA) to overcome the difficulty in the continuous black-box optimization. As QA specializes in optimization of binary problems, a continuous vector has to be encoded to binary, and the solution of QA has to be translated back. Our method has the following three parts: 1) Random subspace coding based on axis-parallel hyperrectangles from continuous vector to binary vector. 2) A quadratic unconstrained binary optimization (QUBO) defined by acquisition function based on nonnegative-weighted linear regression model which is solved by QA. 3) A penalization scheme to ensure that the QA solution can be translated back. It is shown in benchmark tests that its performance using D-Wave Advantage$^{\rm TM}$ quantum annealer is competitive with a state-of-the-art method based on the Gaussian process in high-dimensional problems. Our method may open up a new possibility of quantum annealing and other QUBO solvers including quantum approximate optimization algorithm (QAOA) using a gated-quantum computers, and expand its range of application to continuous-valued problems., Comment: 8 pages, 5 figures

We propose a data-driven technique to estimate the spin Hamiltonian, including uncertainty, from multiple physical quantities. Using our technique, an effective model of KCu$_4$P$_3$O$_{12}$ is determined from the experimentally observed magnetic susceptibility and magnetization curves with various temperatures under high magnetic fields. An effective model, which is the quantum Heisenberg model on a zigzag chain with eight spins having $J_1= -8.54 \pm 0.51 \{\rm meV}$, $J_2 = -2.67 \pm 1.13 \{\rm meV}$, $J_3 = -3.90 \pm 0.15 \{\rm meV}$, and $J_4 = 6.24 \pm 0.95 \{\rm meV}$, describes these measured results well. These uncertainties are successfully determined by the noise estimation. The relations among the estimated magnetic interactions or physical quantities are also discussed. The obtained effective model is useful to predict hard-to-measure properties such as spin gap, spin configuration at the ground state, magnetic specific heat, and magnetic entropy., Comment: 10 pages, 8 figures

The intertube conductance $G$ of the parallel side contacted armchair nanotubes is calculated by Landauer's formula as a function of the Fermi level $E$. When the intertube difference in the dope strength is large enough, a resonant peak dominant over the others appears in the $E$-$G$ curve. The overlap length and the interlayer configuration do not influence the resonant energy. The intervalley transmission at the resonant peak works as a reverser and a filter of the valley current., Comment: version 4. In part just above Table V in version 3, there is a typo, where $|q_{\rm r}|$ is replaced by $E'/E$ by mistake. (correct) The small nonzero $I_{-\sigma,\sigma}$ being inversely proportional to $\widetilde{E}^2$ originates from the slight difference of $|q_{\rm r}|$ from 1 as is explained by Appendix D

Mixing heterogeneous Li-ion conductive materials is one of potential ways to enhance the Li-ion conductivity more than that of the parent materials. However, the development of the mixtures had not exhibited significant progress because it is a formidable task to cover the vast possible composition of the parent materials using traditional ways. Here, we introduce a fashion based on machine learning to optimize the composition ratio of ternary Li3PO4-Li3BO3-Li2SO4 mixture for its Li-ion conductivity. According to our results, the optimum composition of the ternary mixture system is 25:14:61 (Li3PO4: Li3BO3: Li2SO4 in mol%), whose Li-ion conductivity is measured as 4.9 x 10E-4 S/cm at 300 {\deg}C. Our X-ray structure analysis indicates that Li-ion conductivity in the mixing systems is enhanced by virtue of the coexistence of two or more phases. Although the mechanism enhancing Li-ion conductivity is not simple, our results demonstrate the effectiveness of machine learning for the development of materials., Comment: 12 pages, 7 Figures, 3 Tables

Machine learning applications in materials science are often hampered by shortage of experimental data. Integration with legacy data from past experiments is a viable way to solve the problem, but complex calibration is often necessary to use the data obtained under different conditions. In this paper, we present a novel calibration-free strategy to enhance the performance of Bayesian optimization with preference learning. The entire learning process is solely based on pairwise comparison of quantities (i.e., higher or lower) in the same dataset, and experimental design can be done without comparing quantities in different datasets. We demonstrate that Bayesian optimization is significantly enhanced via addition of legacy data for organic molecules and inorganic solid-state materials., Comment: 10 pages, 4 figures

Complexity of materials designed by machine learning is currently limited by the inefficiency of classical computers. We show how quantum annealing can be incorporated into automated materials discovery and conduct a proof-of-principle study on designing complex thermofunctional metamaterials consisting of SiO2, SiC, and Poly(methyl methacrylate). Empirical computing time of our quantum-classical hybrid algorithm involving a factorization machine, a rigorous coupled wave analysis, and a D-Wave 2000Q quantum annealer was insensitive to the problem size, while a classical counterpart experienced rapid increase. Our method was used to design complex structures of wavelength selective radiators showing much better concordance with the thermal atmospheric transparency window in comparison to existing human-designed alternatives. Our result shows that quantum annealing provides scientists gigantic computational power that may change how materials are designed., Comment: 26pages, 5 figures

Partially overlapping two parallel armchair nanotubes are investigated theoretically with the $\pi$ orbital tight bonding model. Considering the interlayer Hamiltonian as perturbation, we obtain approximate analytical formulas of the interlayer transmission rates $T_{\sigma',\sigma}$ from channel $\sigma$ to $\sigma'$ for all the four combinations $(\sigma',\sigma)=(\pm,\pm)$ and $(\pm,\mp)$, where suffixes $+$ and $-$ represent symmetric and anti-symmetric channels, respectively, with respect to the mirror plane of each tube. Landauer's formula conductance is equal to the sum of them in units of $2e^2/h$. According to the perturbation calculation, the interlayer Hamiltonian is transformed into the parameter $w_{\sigma',\sigma}$ that determines the analytical formula of $T_{\sigma',\sigma}$. By comparison with the exact numerical results, the effective range of the analytical formulas is discussed. In the telescoped coaxial contact, the off-diagonal part $T_{-,+}+T_{+,-}$ is very small compared to the diagonal part $T_{+,+}+T_{-,-}$. In the side contact, on the other hand, the off-diagonal part is more significant than the diagonal part in the zero energy peak of the conductance., Comment: 14 figures

We develop a method to efficiently construct phase diagrams using machine learning. Uncertainty sampling (US) in active learning is utilized to intensively sample around phase boundaries. Here, we demonstrate constructions of three known experimental phase diagrams by the US approach. Compared with random sampling, the US approach decreases the number of sampling points to about 20%. In particular, the reduction rate is pronounced in more complicated phase diagrams. Furthermore, we show that using the US approach, undetected new phase can be rapidly found, and smaller number of initial sampling points are sufficient. Thus, we conclude that the US approach is useful to construct complicated phase diagrams from scratch and will be an essential tool in materials science., Comment: 8 pages, 4 figures

We study a generalization performance of the machine learning (ML) model to predict the atomic forces within the density functional theory (DFT). The targets are the Si and Ge single component systems in the liquid state. To train the machine learning model, Gaussian process regression is performed with the atomic fingerprints which express the local structure around the target atom. The training and test data are generated by the molecular dynamics (MD) based on DFT. We first report the accuracy of ML forces when both test and training data are generated from the DFT-MD simulations at a same temperature. By comparing the accuracy of ML forces at various temperatures, it is found that the accuracy becomes the lowest around the phase boundary between the solid and the liquid states. Furthermore, we investigate the transferability of ML models trained in the liquid state to temperature and pressure. We demonstrate that, if the training is performed at a high temperature and if the volume change is not so large, the transferability of ML forces in the liquid state is high enough, while its transferability to the solid state is very low., Comment: 21 pages, 8 figures

An efficient method for finding a better maximizer of computationally extensive probability distributions is proposed on the basis of a Bayesian optimization technique. A key idea of the proposed method is to use extreme values of acquisition functions by Gaussian processes for the next training phase, which should be located near a local maximum or a global maximum of the probability distribution. Our Bayesian optimization technique is applied to the posterior distribution in the effective physical model estimation, which is a computationally extensive probability distribution. Even when the number of sampling points on the posterior distributions is fixed to be small, the Bayesian optimization provides a better maximizer of the posterior distributions in comparison to those by the random search method, the steepest descent method, or the Monte Carlo method. Furthermore, the Bayesian optimization improves the results efficiently by combining the steepest descent method and thus it is a powerful tool to search for a better maximizer of computationally extensive probability distributions., Comment: 13 pages, 5 figures

We develop a method to estimate the spin-spin interactions in the Hamiltonian from the observed magnetization curve by machine learning based on Bayesian inference. In our method, plausible spin-spin interactions are determined by maximizing the posterior distribution, which is the conditional probability of the spin-spin interactions in the Hamiltonian for a given magnetization curve with observation noise. The conditional probability is obtained by the Markov-chain Monte Carlo simulations combined with an exchange Monte Carlo method. The efficiency of our method is tested using synthetic magnetization curve data, and the results show that spin-spin interactions are estimated with a high accuracy. In particular, the relevant terms of the spin-spin interactions are successfully selected from the redundant interaction candidates by the $l_1$ regularization in the prior distribution., Comment: 9 pages, 7 figures

In recent years, universal scaling has gained renewed attention in the study of magnetocaloric materials. It has been applied to a wide variety of pure elements and compounds, ranging from rare earth-based materials to transition metal alloys, from bulk crystalline samples to nanoparticles. It is therefore necessary to quantify the limits within which the scaling laws would remain applicable for magnetocaloric research. For this purpose, a threefold approach has been followed: a) the magnetocaloric responses of a set of materials with Curie temperatures ranging from 46 to 336 K have been modeled with a mean-field Brillouin model, b) experimental data for Gd has been analyzed, and c) a 3D-Ising model ---which is beyond the mean-field approximation--- has been studied. In this way we can demonstrate that the conclusions extracted in this work are model-independent. It is found that universal scaling remains applicable up to applied fields which provide a magnetic energy to the system up to 8\% of the thermal energy at the Curie temperature. In this range, the predicted deviations from scaling laws remain below the experimental error margin of carefully performed experiments. Therefore, for materials whose Curie temperature is close to room temperature, scaling laws at the Curie temperature would be applicable for the magnetic field range available at conventional magnetism laboratories ($\sim 10$ T), well above the fields which are usually available for magnetocaloric devices., Comment: 14 pages, 11 figures

Recently, machine learning has emerged as an alternative, powerful approach for predicting quantum-mechanical properties of molecules and solids. Here, using kernel ridge regression and atomic fingerprints representing local environments of atoms, we trained a machine-learning model on a crystalline silicon system in order to directly predict the atomic forces at a wide range of temperatures. Our idea is to construct a machine-learning model using a quantum-mechanical data set taken from canonical-ensemble simulations at a higher temperature, or an upper bound of the temperature range. With our model, the force prediction errors were about 2% or smaller with respect to the corresponding force ranges, in the temperature region between 300 and 1650 K. We also verified the applicability to a larger system, ensuring the transferability with respect to system size., Comment: 20pages, 5 figures