We model amorphous Zirconia-doped Tantala with machine learning interactomc potentials based on explicit multielement spectral neighbor analysis (EME-SNAP). These atomic structure models can reproduce partial radial distribution functions obtained from first-principles calculations and elastic moduli found from experimental measurements. The two-body pair forces calculated from EME-SNAP further affirm that the potentials capture the atomic interactions well. Molecular dynamics simulations of simulated annealing with EME-SNAP show that the final density of the amorphous models depends on the thermal history even when the annealing rate is kept constant, which captures experimental observations of history-dependent densities. Mechanical spectroscopy is also simulated using both Morse-Beest-Kramer-Santen pair potentials and EME-SNAP. The success in applying the EME-SNAP to amorphous Zirconia-doped Tantala pushes the boundaries of simulation accuracy and system size and enables better and more realistic atomistic modeling for amorphous systems. There are still some limitations in applying the potentials generated in this paper. They are only optimized for trained amorphous phases; high-temperature stability and transferability need to be further investigated.

This study shows a method of enhancing the thermoelectric properties of GeTe-based materials through Ti and Bi codoping on cation sites along with self-doping of Ge via simultaneous optimization of electronic (via crystal field engineering and precise Fermi level optimization) and thermal (via point-defect scattering) transport properties. Pristine GeTe has high carrier concentration $n$ due to intrinsic Ge vacancies, a low Seebeck coefficient $\alpha$, and high thermal conductivity $\kappa$. The Ge vacancy optimization and crystal field engineering result in an enhanced $\alpha$ via excess Ge and Ti doping, which is further improved by band structure engineering through Bi doping. As a result of improved $\alpha$ and the optimized Fermi level (carrier concentration), an enhanced power factor ${\alpha }^2\sigma$ is obtained for Ti-Bi codoped ${\mathrm{Ge}}_{1.01}\mathrm{Te}$. These experimental results are also evidenced by theoretical calculations of band structure and thermoelectric parameters using density functional theory and boltztrap calculations. A significant reduction in the phonon thermal conductivity ${\kappa }_{\mathrm{ph}}$ from $\sim$3.5 to $\sim$1.06 W m${}^{-1}$ K${}^{-1}$ at 300 K for Ti-Bi codoping in GeTe is attributed to point-defect scattering due to mass and strain field fluctuations. This decrease in ${\kappa }_{\mathrm{ph}}$ is in line with the Debye-Callaway model. Also, the phonon dispersion calculations show a decreasing group velocity in Ti-Bi co-doped GeTe, supporting the obtained reduced ${\kappa }_{\mathrm{ph}}$. The strategies used in the present study significantly increase the effective mass, optimize the carrier concentration, and decrease phonon thermal conductivity while achieving an impressive maximum $zT$ value of 1.75 at 773 K and an average $zT$ of 1.03 for ${\mathrm{Ge}}_{0.91}{\mathrm{Ti}}_{0.02}{\mathrm{Bi}}_{0.08}\mathrm{Te}$ over a temperature range of 300–773 K.

The ${\mathrm{YNiO}}_3$ nickelate is a paradigm $d$-electron oxide that manifests the intriguing temperature-mediated sequence of three phases transitions from (i) magnetically ordered insulator to (ii) paramagnetic (PM) insulator and then to (iii) PM metal. Such phenomena raised the question of the nature of the association of magnetism and structural symmetry breaking with the appearance in (i) and (ii) and disappearance in (iii) of insulating band gaps. It is demonstrated here that first-principles mean-field–like density-functional theory (DFT), driven by molecular dynamics temperature evolution, can describe not only the origin of the magnetically long-range ordered insulating phase (i), but also the creation of an insulating paramagnet (ii) that lacks spin- long-range order, and of a metallic paramagnet (iii) as temperature rises. This approach provides the patterns of structural and magnetic symmetry breaking at different temperatures, in parallel with band gaps obtained when the evolving geometries are used as input to DFT electronic band-structure calculations. This disentangles the complex interplay among spin, charge, and orbital degrees of freedom. Analysis shows that the success in describing the rise and fall of the insulating band gaps along the phase transition sequence is enabled by allowing sufficient flexibility in describing diverse local structural and magnetic motifs as input to DFT. This entails the use of sufficiently large supercells that allow expressing structural disproportionation of octahedra, as well as a description of PM phases as a distribution of local magnetic moments (rather than using a single averaged moment). It appears that the historic dismissal of mean-field–like DFT as being unable to describe such Mott-like transitions was premature, as it was based on consideration of averaged crystallographic unit cells, a description that washes out local symmetry-breaking motifs. The magnetically ordered insulating ${\mathrm{YNiO}}_3$ phase (i) and the PM insulating phase (ii) result in DFT from allowing symmetry breaking, evident already by considering the athermal internal energy. In contrast, the PM metallic phase (iii) is formed thermally by smearing out thus weakening symmetry breaking. Analysis of snapshots of the different forms of structural vs magnetic symmetry breaking shows that only the loss of the polymorphous distribution of magnetic moments existing in (ii) causes the fall of the band gap, resulting in the metallic state in (iii). The interesting conclusion is that such a description of the rise [in phases (i) and (ii)] and fall [in phase (iii)] of the insulating gap does not rely on the traditional Mott-like strong correlation understanding, but on breaking and remaking of magnetic and structural symmetries reflected in energy lowering.

A plethora of fundamentally different electronic states can coexist in orbital-selective systems, including Mott-localized, pseudogapped, Fermi, and non-Fermi-liquid phases. Understanding their emergence as a result of electronic correlations remains a fundamental challenge in condensed matter theory. Superconductivity in infinite-layer nickelates is driven by a subtle balance between valence charge and crystal structures, two aspects that are strongly affected by synthetic protocols. Here, using density functional plus dynamical mean-field theory, we explore correlation and hole-doping-induced electronic reconstruction in the ${\mathrm{NdNiO}}_2$ superconductor. Based on a direct comparison with extant RIXS data, we show that the electronic spectra of ${\mathrm{NdNiO}}_2$ films can be understood as mixed valence due to static modulation of $3d^9/3d^8$ Mott/metal states. The coexistence of Mott-localized $3d^9$ and partially restored Fermi-liquid $3d^8$ low-energy excitations results in a two-fluid system exhibiting different coupling parameters, a novel scenario in infinite-layer nickelate superconductors. We expect that our present results are also applicable to access novel phases of matter in other quantum systems, in which structural domains can host different doping levels.

Mechanophores (MPs), stimuli-responsive molecules that respond chromatically to mechanochemical reactions, are important for understanding the coupling between mechanics and chemistry as well as in engineering applications. However, the atomic-level understanding of their activation originates from gas phase studies or under simple linear elongation forces directly on molecules or polymer chains containing MPs. The effect of many-body distortions, pervasive in condensed-phase applications, is not understood. Therefore, we performed large-scale molecular dynamics (MD) simulations of a poly(methyl methacrylate)-spiropyran copolymer under dynamic mechanical loading and studied the activation of the MP under various conditions from dynamical compression to tension during unloading. Detailed analysis of the all-atom MD trajectories shows that the MP blocks experience significant many-body intramolecular distortion that can significantly decrease the activation barrier as compared with when deformation rates are slow relative to molecular relaxation time scales. We find that the reactivity of MPs under material compression states is governed by many-body effects of intramolecular torsions, whereas under tension, the reactions are governed by tensile stresses.

We present a study of the optical properties of quasi-freestanding epitaxial monolayer graphene grown on the Si face of 6H-SiC (0001) in a broad spectral range from midinfrared to ultraviolet. After growth, the sample was intercalated by hydrogen in order to ensure that no dangling bonds between the substrate and graphene layer remain. Spectral dependence of the dielectric function of graphene was parametrized based on spectroscopic ellipsometry fits. We show that, from the viewpoint of optical properties, the investigated sample is very close to exfoliated graphene. We provide information about the spectral dependence of the complex dielectric function of quasi-freestanding graphene in a broad spectral range.

We systematically perform density-functional theory (DFT) calculations for all possible ${\mathrm{M}}_{n+1}{\mathrm{AX}}_n$ (MAX) phases with transition metal M=Sc to Au (excluding Tc), A in group IIIA-IVA, X=C, N, and $n=1,2,3$, a total of about 1200 systems. The thermodynamic stability is determined by comparing the formation enthalpy (at 0 K) against all possible combinations of unary, binary, and ternary boundary phases (available from online DFT databases). Thereby, we identify 124 so far unknown phases (in terms of both experimental synthesis and other theoretical predictions), of which 54 are carbides and 70 are nitrides. Among all stable MAX phases, we identify nine with magnetic properties. In addition to already known and synthesized magnetic phases $({\mathrm{Cr}}_2\mathrm{AlC},$ ${\mathrm{Cr}}_2\mathrm{GeC},$ ${\mathrm{Cr}}_2\mathrm{GaN},$ and ${\mathrm{Mn}}_2\mathrm{GaC})$, we predict five more MAX phases with magnetic ordering $\left[{\mathrm{Mn}}_2\mathrm{A}\right(=\mathrm{Ge}, \mathrm{Sn})\mathrm{C}, {\mathrm{Cr}}_3\mathrm{A}(=\mathrm{Ga}, \mathrm{Ge}){\mathrm{N}}_2, \mathrm{and} {\mathrm{Cr}}_4\mathrm{A}(=\mathrm{Ge}){\mathrm{N}}_3]$. Evaluating previously suggested descriptors for the stability of MAX phases [valence electron concentrations (VECs), differences in atomic radius difference $\mathrm{\Delta }{R}_{\mathrm{at}}$, and differences in electronegativities $\mathrm{\Delta }\chi$], we find that $\mathrm{\Delta }{R}_{\mathrm{at}}$ does not correlate with stability and stable phases are characterized by $\text{VEC}<5.5$, $\mathrm{\Delta }\chi >1.5$. The reverse is, however, not true; for example, a MAX phase with $\text{VEC}<5.5$ and $\mathrm{\Delta }\chi >1.5$ is not necessarily stable.

We have synthesized single-crystal samples of $\beta \text{−}{\mathrm{VOSO}}_4$ and fully characterized their magnetic properties. Our magnetic susceptibility, high field magnetization, and powder inelastic neutron scattering results are in excellent agreement with theoretical expressions for a one-dimensional spin-1/2 Heisenberg chain with an exchange parameter of $3.83\left(2\right)$ meV. Ab initio calculations identify the superexchange pathway, revealing that the spin-chain does not run along the expected crystallographic chain $a$ direction but instead between ${\mathrm{V}}^{4+}{\mathrm{O}}_6$ octahedra that are linked via ${\mathrm{SO}}_4$ tetrahedra along the $b$ axis. We do not detect any phase transition to a long-range magnetic order within our experimental conditions, indicating $\beta \text{−}{\mathrm{VOSO}}_4$ is very close to an ideal one-dimensional magnetic system.

Using microfocused angle-resolved photoemission spectroscopy we investigated microstructures containing regions of single-layer (SL) and bilayer (BL) ${\mathrm{WSe}}_2$ on graphite substrates at different twist angles between SL ${\mathrm{WSe}}_2$ and graphite and within the BL ${\mathrm{WSe}}_2$. Fermi level electrons emitted from the graphite are sharply focused near their $K{}_{gr}$ points in the Brillouin zone, and, when passing through the ${\mathrm{WSe}}_2$, get diffracted to form band replicas readily observed in experimental Fermi surface maps from twisted SL ${\mathrm{WSe}}_2$/graphite. We investigated two twisted BL ${\mathrm{WSe}}_2$ at twist angles $\sim {28}^{\circ }$ and $\sim {10}^{\circ }$ and found no evidence of hybridization gaps at the interlayer band-crossing points, that could be precursors of the flat bands at smaller twist angles. Similarly, no such gaps were found for SL ${\mathrm{WSe}}_2$/graphite. Experimental results are complemented by theoretical density functional theory calculations, which suggest that a formation of hybridization gaps in the ${\mathrm{WSe}}_2$/graphene (which approximates the experimental ${\mathrm{WSe}}_2$/graphite system) sensitively depends on the ${\mathrm{WSe}}_2$ band character at the crossing point with the graphene Dirac band.

Magnetic materials are crucial components of many technologies that could drive the ecological transition, including electric motors, wind turbine generators, and magnetic refrigeration systems. Discovering materials with large magnetic moments is therefore an increasing priority. Here, using state-of-the-art machine learning methods, we scan the Inorganic Crystal Structure Database (ICSD) of hundreds of thousands of existing materials to find those that are ferromagnetic and have large magnetic moments. Crystal graph convolutional neural networks (CGCNNs), materials graph network (MEGNet), and random forests are trained on the Materials Project database that contains the results of high-throughput density functional theory (DFT) predictions. For random forests, we use a stochastic method to select nearly 100 relevant descriptors based on chemical composition and crystal structure. This gives results that are comparable to those of neural networks. Our findings suggests that magnetic properties are intrinsically more difficult to predict than other DFT-calculated properties. The comparison between the different machine learning approaches gives an estimate of the errors for our predictions on the ICSD database. Validating our final predictions by comparisons with available experimental data, we found 15 materials that are likely to have large magnetic moments and have not yet been studied experimentally.

The manipulation of the Rashba spin-splitting is crucial for the development of nanospintronic technology. Here, it is proposed that the Rashba spin-splitting can be turned on and off by reversing electric-field direction. By the first-principles calculations, our proposal is illustrated by a concrete example of Janus monolayer RbKNaBi. The designed RbKNaBi possesses dynamical, thermal, and mechanical stabilities, and is a large-gap quantum spin Hall insulator (QSHI) with Rashba spin-splitting near the Fermi level. A small built-in electric field is predicted due to very small electronegativity difference between the bottom and top atoms, which is very key to switch Rashba spin-splitting through the experimentally available electric field intensity. Due to out-of-plane structural asymmetry, the Janus monolayer has distinctive behaviors by applying external electric field $E$ with the same magnitude but different directions ($z$ or $-z$). Our results reveal that the Rashba energy ($E_R$) and Rashba constant (${\alpha }_R$) are increased by the positive $E$, while a negative $E$ suppresses the Rashba splitting to disappear, and then appears again. In a certain $E$ region (0.15 $\mathrm{V}/\AA$ to 0.25 $\mathrm{V}/\AA$), switching Rashba spin-splitting can be achieved by only reversing electric-field direction. Besides, the piezoelectric strain coefficients $d_{11}$ and $d_{31}$ (5.52 pm/V and –0.41 pm/V) are predicted, which are higher than or compared with those of many 2D materials. By piezoelectric effect, the strain can also be used to tune Rashba spin-splitting of RbKNaBi. In Janus RbKNaBi monolayer, the combination of piezoelectricity and Rashba spin-splitting with topological insulating phase can promote the integration of various physical phenomena. Moreover, a possible spintronic device is proposed to realize the function of spintronic switch. Our proposed manipulation of the Rashba spin-splitting may make a special contribution to semiconductor spintronics.

A family of magnetic halide double perovskites (HDPs) have recently attracted attention due to their potential to broaden application areas of halide double perovskites into, e.g., spintronics. Up to date the theoretical modeling of these systems have relied on primitive approximations to the density functional theory (DFT). In this paper, we study structural, electronic and magnetic properties of the ${\mathrm{Fe}}^{3+}$-containing HDPs ${\mathrm{Cs}}_2{\mathrm{AgFeCl}}_6$ and ${\mathrm{Cs}}_2{\mathrm{NaFeCl}}_6$ using a combination of more advanced DFT-based methods, including $\mathrm{DFT}+U$, hybrid-DFT, and treatments of various magnetic states. We examine the effect of varying the effective Hubbard parameter, $U_{\mathrm{eff}}$, in $\mathrm{DFT}+U$ and the mixing-parameter, $\alpha$, in hybrid DFT on the electronic structure and structural properties. Our results reveal a set of localized $\mathrm{Fe}\left(d\right)$ states that are highly sensitive to these parameters. ${\mathrm{Cs}}_2{\mathrm{AgFeCl}}_6$ and ${\mathrm{Cs}}_2{\mathrm{NaFeCl}}_6$ are both antiferromagnets with Neél temperatures well below room temperature and are thus in their paramagnetic (PM) state at the external conditions relevant to most applications. Therefore, we have examined the effect of disordered magnetism on the electronic structure of these systems and find that while ${\mathrm{Cs}}_2{\mathrm{NaFeCl}}_6$ is largely unaffected, ${\mathrm{Cs}}_2{\mathrm{AgFeCl}}_6$ shows significant renormalization of its electronic band structure.

Intrinsic point defects play a vital role in regulating the electronic structure and electron carrier concentration ($n_0$) of ${\mathrm{Bi}}_2\mathrm{Mo}{\mathrm{O}}_6$, which has been demonstrated as a promising photocatalyst. Unfortunately, the source of $n$-type conductivity for its intrinsic defects has proved challenging. Using first-principles hybrid density functional calculations, we investigate the formation energies and electronic structure of intrinsic point defects in ${\mathrm{Bi}}_2\mathrm{Mo}{\mathrm{O}}_6$. The self-consistent Fermi energies and equilibrium carrier and defect concentrations are calculated using the sc-fermi code based on thermodynamic simulation. It is found that the easy formation of the +2 charged O vacancy ($V_{\mathrm{O}}^{2+}$) is responsible for its intrinsic $n$-type conductivity under Bi-rich/O-poor conditions, and thus, it can have a very high density (reaching up to ${10}^{19} \mathrm{c}{\mathrm{m}}^{-3}$), making it the dominant defect in ${\mathrm{Bi}}_2\mathrm{Mo}{\mathrm{O}}_6$. Under O-rich conditions, only adopting both ${\mathrm{D}}^{+}$ doping and quenching methods in ${\mathrm{Bi}}_2\mathrm{Mo}{\mathrm{O}}_6$ can reach a higher carrier density $\left(>{10}^{17}\mathrm{c}{\mathrm{m}}^{-3}\right)$. Moreover, under the broad range of chemical potentials of $-2.50\mathrm{eV}<\mathrm{\Delta }{\mu }_{\mathrm{Bi}}<0, -6.32\mathrm{eV}<\mathrm{\Delta }{\mu }_{\mathrm{Mo}}<-1.48\mathrm{eV}$, and $-2.19\mathrm{eV}<\mathrm{\Delta }{\mu }_{\mathrm{O}}<-0.65\mathrm{eV}$, after quenching from 700 to 300 K, ${\mathrm{Bi}}_2\mathrm{Mo}{\mathrm{O}}_6$ can be effectively donor doped without significant compensation, and $n_0$ increases as $\mathrm{\Delta }{\mu }_{\mathrm{O}}$ decreases or temperature increases. Our results can give a guide in selecting optimum growth and quenching conditions to achieve high $n$-type doping and suppress compensation.

The atomic cluster expansion (ACE) was proposed recently as a new class of data-driven interatomic potentials with a formally complete basis set. Since the development of any interatomic potential requires a careful selection of training data and thorough validation, an automation of the construction of the training dataset as well as an indication of a model's uncertainty are highly desirable. In this work, we compare the performance of two approaches for uncertainty indication of ACE models based on the D-optimality criterion and ensemble learning. While both approaches show comparable predictions, the extrapolation grade based on the D-optimality (MaxVol algorithm) is more computationally efficient. In addition, the extrapolation grade indicator enables an active exploration of new structures, opening the way to the automated discovery of rare-event configurations. We demonstrate that active learning is also applicable to explore local atomic environments from large-scale molecular-dynamics simulations.

Brillouin laser light scattering spectra of hexagonal boron nitride were measured in its pure form as well as with zero-valent copper, gold, and silver intercalants including one sample co-intercalated with copper and silver. Up to four of the five independent elastic stiffness constants were determined along with the associated sound velocities for the five distinct materials. Intercalation radically changes the optical color of the boron nitride. Brillouin scattering measurements show almost no change in the $c_{33}$ out-of-plane elastic stiffness and the $c_{66}$ in-plane shear modulus, while the $c_{11}$ in-plane stiffness increases by roughly 100 GPa with copper-silver co-intercalation and decreases by roughly 30 GPa with silver intercalation. The results lie within the broad range of literature values for $c_{11},$ $c_{33},$ and $c_{44}$ but differ substantially for $c_{66}$.

Single crystals of a new layered compound, ${\mathrm{Cr}}_{1.21}{\mathrm{Te}}_2$, were synthesized via a vapor transport method. The crystal structure and physical properties were characterized by single crystal and powder x-ray diffraction, temperature- and field-dependent magnetization, zero-field heat capacity, and angle-resolved photoemission spectroscopy. ${\mathrm{Cr}}_{1.21}{\mathrm{Te}}_2$, containing two Cr sites, crystalizes in a trigonal structure with a space group P-3 (No. 147). The Cr site in the interstitial layer is partially occupied. Physical property characterizations indicate that ${\mathrm{Cr}}_{1.21}{\mathrm{Te}}_2$ is metallic with hole pockets at the Fermi energy and undergoes a ferromagnetic phase transition at $\sim 173\mathrm{K}$. The magnetic moments align along the $c$ axis in the ferromagnetic state. Based on low-temperature magnetization, the spin stiffness constant, D, and spin excitation gap, $\mathrm{\Delta }$, were estimated according to Bloch's law to be $D=94\pm 17\mathrm{meV}{\AA }^2$ and $\mathrm{\Delta }=0.45\pm 0.33$ meV, suggesting its possible application as a low dimensional ferromagnet.

Two-dimensional MXenes, with ${\mathrm{Ti}}_3{\mathrm{C}}_2{\mathrm{T}}_x$ being the most prominent member, show properties that make them promising for a manifold of applications, including electrodes in light-emitting diodes, solar cells, and field-effect transistors based on organic semiconductors. In these cases, the work function of MXenes plays an important role in the energy level alignment to the subsequently deposited organic layer, as it determines the electron and hole injection barriers. Therefore, methods for controlling the ${\mathrm{Ti}}_3{\mathrm{C}}_2{\mathrm{T}}_x$ work function should be developed. We demonstrate that, by using thin layers of (metal-)organic donor/acceptor molecules, the work function of ${\mathrm{Ti}}_3{\mathrm{C}}_2{\mathrm{T}}_x$ can be tuned over a range of $>3$ eV. This enables tuning the energy level alignment to a subsequently deposited organic semiconductor, all the way from intrinsic Fermi level pinning at the highest occupied molecular energy level (minimal hole injection barrier) to pinning at the lowest unoccupied level (minimal electron injection barrier). Furthermore, it is shown that a predominantly oxygen-terminated surface does not lead to an extraordinary high work function, in contrast to theoretical predictions. The proposed strategy may greatly expand the use of MXenes in conjunction with organic hole and electron transport layers in optoelectronic devices.

Excellent high-temperature mechanical properties of Ni-based single-crystal superalloys (NSCSs) are attributed to the yield strength anomaly of ${\mathrm{Ni}}_3\mathrm{Al}$ that is intimately related to generalized stacking fault energies (GSFEs). Therefore, clarifying the effects of alloying elements on the GSFEs is of great significance for alloys design. Here, by means of ab initio density functional theory calculations, we systematically calculated the GSFEs of different slip systems of Ni and ${\mathrm{Ni}}_3\mathrm{Al}$ without and with alloying elements using the alias shear method. We obtained that for Ni, except for magnetic elements Mn, Fe, and Co, most of the alloying elements decrease the unstable stacking fault energy (${\gamma }_{\text{USF}}$) of the $\left[01\overline{1}\right]\left(111\right)$ and $\left[11\overline{2}\right]\left(111\right)$ slip systems and also decrease the stable stacking fault energy (${\gamma }_{\text{SF}}$) of the $\left[11\overline{2}\right]\left(111\right)$ slip system. Interestingly, the reduction effects exhibit a strong correlation with the inverse of atom radii. For ${\mathrm{Ni}}_3\mathrm{Al}$, most of the alloying elements in groups IIIB–VIIB show a strong Al site preference. Except for Mn and Fe, the elements in groups VB–VIIB and the first column of group VIII increase the values of ${\gamma }_{\text{USF}}$ of different slip systems of ${\mathrm{Ni}}_3\mathrm{Al}$, which makes the slip deformation and dislocation emits difficult. On the other hand, the elements in groups IIIB–VIIB also increase the value of ${\gamma }_{\text{SF}}$, and thus reduce the stability of the antiphase boundary, complex stacking fault, and superlattice intrinsic stacking fault of ${\mathrm{Ni}}_3\mathrm{Al}$. We found that Re is an excellent strengthening alloying element that significantly increases the slip barrier of the tailing slip process for Ni, and also enhances the slip barrier of the leading slip process of three slip systems for ${\mathrm{Ni}}_3\mathrm{Al}$. W and Mo exhibit similar effects as Re. We predicted that Os, Ru, and Ir are good strengthening alloying elements as well, since they show the strengthening effects on both the leading and the tailing slip process for Ni and ${\mathrm{Ni}}_3\mathrm{Al}$. This work established an exhaustive dictionary of the effects of various alloying elements on the GSFEs of both Ni and ${\mathrm{Ni}}_3\mathrm{Al}$ phases, which would help to guide the design of next-generation high-performance NSCSs.