Based on irreducible representations (or symmetry eigenvalues) and compatibility relations, a material can be predicted to be a topological/trivial insulator [satisfying compatibility relations] or a topological semimetal [violating compatibility relations]. However, Weyl semimetals usually go beyond this symmetry-based strategy. In other words, Weyl nodes could emerge in a material, no matter if its occupied bands satisfy compatibility relations, or if the symmetry indicators are zero. In this work, we propose a new topological invariant $χ$ for the systems with S$_4$ symmetry [i.e., the improper rotation S$_4$ ($\equiv$ IC$_{4z}$) is a proper four-fold rotation (C$_{4z}$) followed by inversion (I)], which can be used to diagnose the Weyl semimetal phase. Moreover, $χ$ can be easily computed through the one-dimensional Wilson-loop technique. By applying this method to the high-throughput screening in first-principles calculations, we predict a lot of Weyl semimetals in both nonmagnetic and magnetic compounds. Various interesting properties (e.g. magnetic frustration effects, superconductivity and spin-glass order, etc.) are found in predicted Weyl semimetals, which provide realistic platforms for future experimental study of the interplay between Weyl fermions and other exotic states.
Although topological invariants have been introduced to classify the appearance of protected electronic states at surfaces of insulators, there are no corresponding indexes for Weyl semimetals whose nodal points may appear randomly in the bulk Brillouin Zone (BZ). Here we use a well-known result that every Weyl point acts as a Dirac monopole and generates integer Berry flux to search for the monopoles on rectangular BZ grids that are commonly employed in self-consistent electronic structure calculations. The method resembles data mining technology of computer science and is demonstrated on loc…
We compute the polarization function in a doped three-dimensional anisotropic-Weyl semimetal, in which the fermion energy dispersion is linear in two components of the momenta and quadratic in the third. Through detailed calculations, we find that the long wavelength plasmon mode depends on the fermion density $n_e$ in the form $Ω_{p}^{\bot}\propto n_{e}^{3/10}$ within the basal plane and behaves as $Ω_{p}^{z}\propto n_{e}^{1/2}$ along the third direction. This unique characteristic of the plasmon mode can be probed by various experimental techniques, such as electron energy-loss spectroscopy.…
Topological materials in crystal solids, including topological insulators (TIs), topological crystalline insulators (TCIs), topological Dirac semimetals (DSMs), topological Weyl semimetals (WSMs), topological Dirac or Weyl nodal line semimetals (NLSMs) and beyond, are mainly featured with topological, protected non-trivial surface states, and their bulk phases are insulators or semimetals with the proper presence of Dirac cones, Weyl nodes or Dirac nodal lines around the Fermi level. The author suggests a two-step computational screening strategy of 3D topological materials by mixing chemistry…
High-Throughput Discovery of Semimetallic Borophenes with Diverse Dirac States Via Transferable Tight-Binding Approach
School of Physics and Optoelectronics, Xiangtan University（湘潭大学物理与光电工程学院）；Hunan Provincial Key Laboratory of Computational Condensed Matter Physics and Quantum Materials Engineering（湖南省计算凝聚态物理与量子材料工程重点实验室）
A theory is developed for the density and temperature dependent carrier conductivity in doped three-dimensional (3D) Dirac materials focusing on resistive scattering from screened Coulomb disorder due to random charged impurities (e.g., dopant ions and unintentional background impurities). The theory applies both in the undoped intrinsic ("high-temperature", $T \gg T_F$) and the doped extrinsic ("low-temperature", $T \ll T_F$) limit with analytical scaling properties for the carrier conductivity obtained in both regimes, where $T_F$ is the Fermi temperature corresponding to the doped free carr…
Due to their chemical and structural diversity, nanoporous materials can be used in a wide variety of applications, including fluid separation, gas storage, heterogeneous catalysis, drug delivery, etc. Given the large and rapidly increasing number of known nanoporous materials, and the even bigger number of hypothetical structures, computational screening is an efficient method to find the current best-performing materials and to guide the design of future materials. This review highlights the potential of high-throughput computational screenings in various applications. The achievements and t…
We screen a large chemical space of perovskite alloys for systems with the right properties to accommodate a morphotropic phase boundary (MPB) in their composition-temperature phase diagram, a crucial feature for high piezoelectric performance. We start from alloy end-points previously identified in a high-throughput computational search. An interpolation scheme is used to estimate the relative energies between different perovskite distortions for alloy compositions with a minimum of computational effort. Suggested alloys are further screened for thermodynamic stability. The screening identifi…
A Materials Project based open-source Python tool, MPInterfaces, has been developed to automate the high-throughput computational screening and study of interfacial systems. The framework encompasses creation and manipulation of interface structures for solid/solid hetero-structures, solid/implicit solvents systems, nanoparticle/ligands systems; and the creation of simple system-agnostic workflows for in depth computational analysis using density-functional theory or empirical energy models. The package leverages existing open-source high-throughput tools and extends their capabilities towards…
Luttinger semimetals are three-dimensional electron systems with a parabolic band touching and an effective total spin $J=3/2$. In this paper, we present an analytical theory of dielectric screening of inversion-symmetric Luttinger semimetals with an arbitrary carrier density and conduction-valence effective mass asymmetry. Assuming a spherical approximation for the single-particle Luttinger Hamiltonian, we determine analytically the dielectric screening function in the random phase approximation for arbitrary values of the wave vector and frequency, the latter in the complex plane. We use thi…
The development of new high dielectric materials is essential for advancement in modern electronics. Oxides are generally regarded as the most promising class of high dielectric materials for industrial applications as they possess both high dielectric constants and large band gaps. Most previous researches on high dielectrics were limited to already known materials. In this study, we conducted an extensive search for high dielectrics over a set of ternary oxides by combining crystal structure prediction and density functional perturbation theory calculations. From this search, we adopted mult…
Herein, we performed ab initio screening to identify the best doping of LiNiO2 to achieve improved cycle performance in lithium ion batteries. The interlayer interaction that dominates the c-axis contraction and overall performance was captured well by density functional theory using van der Waals exchange-correlation functionals. The screening indicated that Nb-doping is promising for improving cycle performance. To extract qualitative reasonings, we performed data analysis in a materials informatics manner to obtain a reasonable regression to reproduce the obtained results. LASSO analysis im…
The quasi-harmonic Debye approximation has been implemented within the AFLOW and Materials Project frameworks for high-throughput computational science (Automatic Gibbs Library, AGL), in order to calculate thermal properties such as the Debye temperature and the thermal conductivity of materials. We demonstrate that the AGL method, which is significantly cheaper computationally compared to the fully ab initio approach, can reliably predict the ordinal ranking of the thermal conductivity for several different classes of semiconductor materials. We also find that for the set of 182 materials inv…
Nano-materials, such as metal-organic frameworks, have been considered to capture CO$_2$. However, their application has been limited largely because they exhibit poor selectivity for flue gases and low capture capacity under low pressures. We perform a high-throughput screening for selective CO$_2$ capture from flue gases by using first principles thermodynamics. We find that elements with empty d orbitals selectively attract CO$_2$ from gaseous mixtures under low CO$_2$ pressures at 300 K and release it at ~450 K. CO$_2$ binding to elements involves hybridization of the metal d orbitals with…
We perform a high-throughput screening on phonon-mediated superconductivity in ternary metal diboride structure with alkali, alkaline earth, and transition metals. We find 17 ground states and 78 low-energy metastable phases. From fast calculations of zone-center electron-phonon coupling, 43 compounds are revealed to show electron-phonon coupling strength higher than that of MgB2. An anti-correlation between energetic stability and electron-phonon coupling strength is identified. We suggest two phases, i.e., Li3ZrB8 and Ca3YB8, to be synthesized, which show reasonable energetic stability and s…
Searching ferromagnetic semiconductor materials with electrically controllable spin polarization is a long-term challenge for spintronics. Bipolar magnetic semiconductors (BMS), with valence and conduction band edges fully spin-polarized in different spin directions, show great promise in this aspect because the carrier's spin polarization direction can be easily tuned by voltage gate. Here, we propose a standard high-throughput computational screening scheme for searching BMS materials. The application of this scheme to the Materials Project database gives 11 intrinsic BMS materials (1 experi…
Hierarchical high-throughput screening of alkaline-stable lithium-ion conductors combining machine learning and first-principles calculations
Materials Sciences Division, Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室材料科学部）；Department of Materials Science and Engineering, University of California, Berkeley（加州大学伯克利分校材料科学与工程系）
Based on high throughput density functional theory calculations, we performed systematic screening for spin-gapless semiconductors (SGSs) in quaternary Heusler alloys XX 0 YZ (X, X 0 , and Y are transition metal elements without Tc, and Z is one of B, Al, Ga, In, Si, Ge, Sn, Pb, P, As, Sb, and Bi). Following the empirical rule, we focused on compounds with 21, 26, or 28 valence electrons, resulting in 12, 000 possible chemical compositions. After systematically evaluating the thermodynamic, mechanical, and dynamical stabilities, we successfully identified 70 stable SGSs, confirmed by explicit …
Finding cost-effective and efficient photocatalytic materials able to catalyse the water splitting reaction under visible light is one of the greatest challenges in current environmental material science. Despite that many photocatalysts are already known in the context of green hydrogen production, strategies to systematically and rationally modify their optoelectronic properties to achieve desired photocatalytic performance are yet to be established. Piezoelectric materials react to mechanical stimuli by adjusting their band gaps and band alignments, thus offering a possible route to precise…
Intrinsic polar metals are rare, especially in oxides, because free electrons screen electric fields in a metal and eliminate the internal dipoles that are needed to break inversion symmetry. Here we use first-principles high-throughput structure screening to predict a new polar metal in bulk and thin film forms. After screening more than 1000 different crystal structures, we find that ordered BiPbTi2O6 can crystallize in three polar and metallic structures, which can be transformed between via pressure or strain. In a heterostructure of layered BiPbTi2O6 and PbTiO3, multiple states with diffe…
First-principles-based materials screening is systematically performed to discover new combinations of chemical elements possibly making shape-memory alloys (SMAs). The B2, D03, and L21 crystal structures are considered as the parent phases, and the 2H and 6M structures are considered as the martensitic phases. 3,384 binary and 3,243 ternary alloys (6,627 in total) with stoichiometric composition ratios are investigated by the materials screening in terms of energetic and dynamical stabilities of the martensitic phases as well as structural compatibility between the parent and the martensitic …
Recent advances in two-dimensional (2D) magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low-dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, we conducted firstprinciples based high-throughput search to screen potentially stable mixed metal phosphorous trichalcogenides (MM'P2X6, where M and M' are transition metals and X is a chalcogenide) that have a wide …
Nontrivial band topologies in semimetals lead to robust surface states that can contribute dominantly to the total conduction. This may result in reduced resistivity with decreasing feature size contrary to conventional metals, which may highly impact the semiconductor industry. Here we study the resistivity scaling of a representative topological semimetal CoSi using realistic band structures and Green's function methods. We show that there exists a critical thickness d_c dividing different scaling trends. Above d_c, when the defect density is low such that surface conduction dominates, resis…
Important phenomena such as magnetostriction, magnetocaloric, and magnetoelectric effects arise from, or could be enhanced by, the coupling of magnetic and structural degrees of freedom. The coupling of spin and lattice also influence transport and structural properties in magnetic materials in particular around phase transitions. In this paper we propose a method for screening materials for a strong magneto-structural coupling by assessing the effect of the local magnetic configuration on the atomic forces using density functional theory (DFT). We have employed the disordered local moment app…
High throughput screening, crystal structure prediction, and carrier mobility calculations of organic molecular semiconductors as hole transport layer materials in perovskite solar cells
We perform a computational screening for two-dimensional magnetic materials based on experimental bulk compounds present in the Inorganic Crystal Structure Database and Crystallography Open Database. A recently proposed geometric descriptor is used to extract materials that are exfoliable into two-dimensional derivatives and we find 85 ferromagnetic and 61 anti-ferromagnetic materials for which we obtain magnetic exchange and anisotropy parameters using density functional theory. For the easy-axis ferromagnetic insulators we calculate the Curie temperature based on classical Monte Carlo simula…
Despite their extraordinary properties, electrides are still a relatively unexplored class of materials with only a few compounds grown experimentally. Especially for layered electrides, the current researches mainly focus on several isostructures of Ca2N with similar interlayer two-dimensional (2D) anionic electrons. An extensive screening for different layered electrides is still missing. Here, by screening materials with anionic electrons for the structures in Materials Project, we uncover 12 existing materials as new layered electrides. Remarkably, these layered electrides demonstrate comp…
High-Throughput Discovery of Chiral Carbon-Boron Semimetals with Weyl Topology and Phonon-Mediated Superconductivity
University of Science and Technology of China（中国科学技术大学）；Wuhan Institute of Technology（武汉工程大学）；Hefei University of Technology（合肥工业大学）；Hanhai Lingchao Intelligent Computing (Shanghai) Technology Services Co., Ltd.（瀚海凌潮智能计算（上海）科技有限公司）
Owing to the natural compatibility with current semiconductor industry, silicon allotropes with diverse structural and electronic properties provide promising platforms for the next-generation Si-based devices. After screening 230 all-silicon crystals in the zeolite frameworks by first-principles calculations, we disclose two structurally stable Si allotropes (AHT-Si24 and VFI-Si36) containing open channels as topological node-line semimetals with Dirac nodal points forming a nodal loop in the kz=0 plane of Brillouin zone. Interestingly, their nodal loops protected by inversion and time-revers…
Auger recombination (AR) being electron-hole annihilation with energy-momentum transfer to another carrier is believed to speed up in materials with small band gap. We theoretically show that this rule is violated in gapless three-dimensional materials with ultra-relativistic electron-hole dispersion, Weyl semimetals (WSM). Namely, AR is prohibited by energy-momentum conservation laws in prototypical WSM with a single Weyl node, even in the presence of anisotropy and tilt. In real multi-node WSM, the geometric dissimilarity of nodal dispersions enables weak inter-node AR, which is further supp…
Half-antiperovskites (HAPs) are a class of materials consisting of stacked kagome lattices and thus host exotic magnetic and electronic states. We perform high-throughput calculations based on density functional theory (DFT) and atomistic spin dynamics (ASD) simulations to predict stable magnetic HAPs M$_3$X$_2$Z$_2$ (M = Cr, Mn, Fe, Co, and Ni; X is one of the elements from Li to Bi except noble gases and 4$f$ rare-earth metals; Z = S, Se, and Te), with both thermodynamical and mechanical stabilities evaluated. Additionally, the magnetic ground states are obtained by utilizing DFT calculation…
We present a computational screening of experimental structural repositories for fast Li-ion conductors, with the goal of finding new candidate materials for application as solid-state electrolytes in next-generation batteries. We start from ~1400 unique Li-containing materials, of which ~900 are insulators at the level of density-functional theory. For those, we calculate the diffusion coefficient in a highly automated fashion, using extensive molecular dynamics simulations on a potential energy surface (the recently published pinball model) fitted on first-principles forces. The ~130 most pr…
The discovery of metals as catalytic centers for nitrogen reduction reactions has stimulated great enthusiasm for single-atom catalysts. However, the poor activity and low selectivity of available SACs are far away from the industrial requirement. Through the high throughout first principles calculations, the doping engineering can effectively regulate the NRR performance of b-Sb monolayer. Especially, the origin of activated N2 is revealed from the perspective of the electronic structure of the active center. Among the 24 transition metal dopants, Re@Sb and Tc@Sb showed the best NRR catalytic…
Electrides are a unique class of electron-rich materials where excess electrons are localized in interstitial lattice sites as anions, leading to a range of unique properties and applications. While hundreds of electrides have been discovered in recent years, magnetic electrides have received limited attention, with few investigations into their fundamental physics and practical applications. In this work, 51 magnetic electrides (12 antiferromagnetic, 13 ferromagnetic, and 26 interstitial-magnetic) were identified using high-throughput computational screening methods and the latest Material Pr…
The design of corrosion-resistant high entropy alloys (CR-HEAs) is challenging due to the alloys' virtually astrological composition space. To facilitate this, efficient and reliable high-throughput exploratory approaches are needed. Toward this end, the current work reports a first-principles-based approach exploiting the correlations between work function, surface energy, and corrosion resistance (i.e., work function and surface energy are, by definitions, proportional and inversely proportional to an alloy's inherent corrosion resistance, respectively). Two Bayesian CALPHAD models (or datab…
Finding the true magnetic structure at given external conditions is crucial for describing magnetic materials and predicting their properties. This is especially important for high-throughput screening of potentially good magnets that without adequate description of the magnetic structure may result in an enormous waste of computational resources. I introduce a method, which accurately and efficiently treats magnetic ordering in the course of standard first-principles calculations. The method is suitable for all temperatures and is based on Monte Carlo (MC) technique. At high temperatures MC i…
High-Throughput Photovoltaic Screening and Spacer-Dependent Shift Current in Two-Dimensional Hybrid Perovskites
Humboldt-Universität zu Berlin（柏林洪堡大学）；Institute of Materials Science, Technische Universität Darmstadt（达姆施塔特工业大学材料科学研究所）；North University of China（中北大学）；State Key Laboratory of Extreme Environment Optoelectronic Dynamic Measurement Technology and Instrument（极端环境光电动态测量技术与仪器国家重点实验室）；Materials Genome Institute, Shanghai University（上海大学材料基因组研究院）；Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China（福建省光电信息科技创新实验室）
High-through computational thermodynamic approaches are becoming an increasingly popular tool to uncover novel compounds. However, traditional methods tend to be limited to stability predictions of stoichiometric phases at absolute zero. Such methods thus carry the risk of identifying an excess of possible phases that do not survive to temperatures of practical relevance. We demonstrate how the Calphad formalism, informed by simple first-principles input can be simply used to overcome this problem at a low computational cost and deliver quantitatively useful phase diagram predictions at all te…
The close approach of the Fermi energy EF of a Dirac semimetal to the Dirac point ED uncovers new physics such as velocity renormalization,1,2,3 and the Dirac plasma 4,5 at |EF -ED| < kBT, where kBT is the thermal energy. In graphene, substrate disorder drives fluctuations in EF. Three-dimensional topological Dirac semimetals (TDS)6,7 obviate the substrate, and should show reduced EF fluctuations due to better metallic screening and higher dielectric constants. Here we map the potential fluctuations in TDS Na3Bi using a scanning tunneling microscope. The rms potential fluctuations are signific…
Great enthusiasm in single atom catalysts (SACs) for the N2 reduction reaction (NRR) has been aroused by the discovery of Metal (M)-Nx as a promising catalytic center. However,the performance of available SACs,including poor activity and selectivity,is far away from the industrial requirement because of the inappropriate adsorption behaviors of the catalytic centers. Through the first principles high throughput screening, we find that the rational construction of Fe-Fe dual atom centered site distributed on graphite carbon nitride (Fe2/gCN) compromises the ability to adsorb N2H and NH2, achiev…
Decoding Oxygen K-edge Fingerprints of NCM-811 Degradation via Ab Initio Many-Body Theory and High-Throughput Screening of Crystal Proxies
Carl von Ossietzky Universit\"at Oldenburg, Institute of Physics, 26129 Oldenburg, Germany；Department Interface Design, Helmholtz-Zentrum Berlin f\"ur Materialien und Energie GmbH, Berlin, Germany；Friedrich-Schiller-Universit\"at Jena, Institute of Condensed Matter Theory
First-principles high-throughput screening of ruthenium compounds for advanced interconnects
Department of Electronics Engineering, Incheon National University（仁川国立大学电子工程系）；Research Institute for Engineering and Technology, Incheon National University（仁川国立大学工程技术研究院）
Using high-throughput screening coupled with state-of-the-art van der Waals density functional theory, we investigate the adsorption properties of four important molecules, H_2, CO_2, CH_4, and H_2O in MOF-74-M with M = Be, Mg, Al, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Sr, Zr, Nb, Ru, Rh, Pd, La, W, Os, Ir, and Pt. We show that high-throughput techniques can aid in speeding up the development and refinement of effective materials for hydrogen storage, carbon capture, and gas separation. The exploration of the configurational adsorption space allows us to extract crucial information concer…
The high-throughput (HT) computational method is a useful tool to screen high performance functional materials. In this work, using the deformation potential method under the single band model, we evaluate the carrier relaxation time and establish an electrical descriptor (\c{hi}) characterized by the carrier effective masses based on the simple rigid band approximation. The descriptor (\c{hi}) can be used to reasonably represent the maximum power factor without solving the electron Boltzmann transport equation. Additionally, the Grüneisen parameter (γ), a descriptor of the lattice anharmonici…
We have developed a machine learning-based interatomic potential (MLIP) for the quaternary MoNbTaW (R4) and quinary MoNbTaTiW (R5) high entropy alloys (HEAs). MLIPs enabled accurate high throughput calculations of elastic and mechanical properties of various non-equimolar R4 and R5 alloys, which are otherwise very time consuming calculations when performed using density functional theory (DFT). We demonstrate that the MLIP predicted properties compare well with the DFT results on various test cases and are consistent with the available experimental data. The MLIPs are also utilized for high th…
Ultra-high temperature ceramics, UHTCs, are a group of materials with high technological interest because their use in extreme environments. However, their characterization at high temperatures represents the main obstacle for their fast development. Obstacles are found from a experimental point of view, where only few laboratories around the world have the resources to test these materials under extreme conditions, and also from a theoretical point of view, where actual methods are extremely expensive. Here, a new theoretical high-throughput framework for the prediction of the thermoelastic p…
