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When searching for novel inorganic materials, limiting the combination of constituent elements can greatly improve the search efficiency. In this study, we used machine learning to predict elemental combinations with high reactivity for materials discovery. The essential issue for such prediction is the uncertainty of whether the unreported combinations are non-reactive or not just investigated, though the reactive combinations can be easily collected as positive datasets from the materials databases. To construct the negative datasets, we developed a process to select reliable non-reactive combinations by evaluating the similarity between unreported and reactive combinations. The machine learning models were trained by both datasets and the prediction results were visualized by two-dimensional heatmaps: elemental reactivity maps to identify elemental combinations with high reactivity but no reported stable compounds. The maps predicted high reactivity (i.e., synthesizability) for the Co_Al_Ge ternary system, and two novel ternary compounds were synthesized: Co4Ge3.19Al0.81 and Co2Al1.24Ge1.76., Comment: 14 pages, 5 figures

The nodal-line semimetals NaAlSi and NaAlGe have significantly different ground states despite having similar electronic structures: NaAlSi exhibits superconductivity below 7 K, while NaAlGe exhibits semiconductive electrical conductivity at low temperatures, indicating the formation of a pseudogap at approximately 100 K. The origin of the pseudogap in NaAlGe is unknown but may be associated with excitonic instability. We investigated hole-doping effects on the ground state in the solid solution Na(Al1-xZnx)Ge and discovered that the pseudogap is suppressed continuously with increasing Zn content, followed by the appearance of a superconducting dome with the highest transition temperature of 2.8 K. This superconductivity most likely results from excitonic fluctuations., Comment: 7 pages, 9 figures

NaAlSi and NaAlGe are isostructural and isoelectronic semimetals with topological nodal lines close to the Fermi level. Despite having virtually identical electronic structures, NaAlSi exhibits superconductivity below Tc = 6.8 K, whereas NaAlGe does not. We investigate NaAlGe by measuring its electrical resistivity, Hall effect, magnetic susceptibility, and heat capacity using single crystals. It is revealed that NaAlGe is not a simple semimetal but rather has an unusual ground state with a small pseudogap of approximately 100 K close to the Fermi level. We argue that the formation of the pseudogap in NaAlGe is due to an unexpected Fermi surface instability, such as an excitonic instability, as opposed to the electron-phonon instability that leads to the formation of the superconducting gap in NaAlSi., Comment: 6 pages, 5 figures

NaAlSi is a quasi-two-dimensional semimetal with superconductivity below Tc = 6.8 K and a band structure characterized by nodal lines near the Fermi level and potential topological surface states. Electrical resistivity measurements on its superconducting transitions in magnetic fields were made using plate-like single crystals. In the magnetic field-temperature phase diagram, we observed a substantial reduction in resistivity in a pre-transitional zone above the bulk superconducting regime only when the magnetic fields were perpendicular to the plane, rather than parallel to it. Significant sample (thickness) dependence, reentrant behavior, and sensitivity to electrode configurations all indicate that a portion of the crystal has an upper critical field greater than the bulk superconductivity in the pre-transitional region. This fractional superconductivity may occur on the side surface of the crystal.

NaAlSi is an sp electron superconductor crystallizing in a layered structure of the anti-PbFCl type with a relatively high transition temperature Tc of ~7 K. Recent electronic state calculations revealed the presence of topological nodal lines in the semimetallic band structure, which attracted much attention owing to the superconductivity. However, experimental investigation remained limited because of the lack of single crystals. Here, we successfully prepared single crystals of NaAlSi by a Na-Ga flux method and characterized their superconducting and normal-state properties through electrical resistivity, magnetization, and heat capacity measurements. A sharp superconducting transition with a Tc of 6.8 K is clearly observed, and heat capacity data suggest an anisotropic superconducting gap. Surprisingly, despite the sp electron system, the normal state is governed by the electron correlations, which is indicated by a T2 resistivity and a Wilson ratio of 2.0. The origin of the electron correlation may be related to the orthogonal saddle-shaped Fermi surfaces derived from the Si px and py states, which intersect with the light Al s bands to form the nodal lines near the Fermi level. These results strongly suggest that the superconductivity of NaAlSi is not caused by a simple phonon mechanism but involves a certain unconventional aspect, although its relevance to the nodal lines is unclear.