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Abstract The highest ambient‐pressure Tc among binary compounds is 40 K (MgB2). Higher Tc is achieved in high‐pressure hydrides or multielement cuprates. Alternatively, are explored superconducting properties of binary, metastable sub‐oxides, that may emerge under extremely low oxygen partial pressure. The emphasis is on the rock‐salt structure, which is known to promote superconductivity, and exploring AlO, ScO, TiO, and NbO. Dynamic lattice stability is achieved by introducing metal and oxygen vacancies in the fashion of Nb_1−xO_1−x‐type structure (x = ¼). The electron‐phonon (e‐ph) coupling is remarkably large in Al_1−xO_1−xand Ti_1−xO_1−x(λ ≈ 2 at x = ¼), with Tc ≈ 35 K according to the Allen–Dynes equation. Significantly, the coupling strength is comparable to that in high‐pressure hydrides, yet, in contrast to hydrides and MgB2, the coupling is largely driven by low frequency phonons. Sc_1−xO_1−xand Nb_1−xO_1−xshow significantly smaller λ and Tc. Further, hydrogen intercalation to boost λ and Tc is investigated. Only Ti_1−x(O_1−xHx) and Nb_1−x(O_1−xHx) are dynamically stable upon intercalation, where H, respectively, decreases and increases Tc. The effect of H doping on electronic structure and Tc is discussed. Altogether, the study suggests that metal sub‐oxides are promising compounds to achieve strong e‐ph coupling at ambient pressure. 

The precise controllability of the Fermi level is a critical aspect of quantum materials. For topological Weyl semimetals, there is a pressing need to fine-tune the Fermi level to the Weyl nodes and unlock exotic electronic and optoelectronic effects associated with the divergent Berry curvature. However, in contrast to two-dimensional materials, where the Fermi level can be controlled through various techniques, the situation for bulk crystals beyond laborious chemical doping poses significant challenges. Here, we report the milli-electron-volt (meV) level ultra-fine-tuning of the Fermi level of bulk topological Weyl semimetal tantalum phosphide using accelerator-based high-energy hydrogen implantation and theory-driven planning. By calculating the desired carrier density and controlling the accelerator profiles, the Fermi level can be experimentally fine-tuned from 5 meV below, to 3.8 meV below, to 3.2 meV above the Weyl nodes. High-resolution transmission electron microscopy reveals the crystalline structure is largely maintained under irradiation, while electrical transport indicates that Weyl nodes are preserved and carrier mobility is also largely retained. Our work demonstrates the viability of this generic approach to tune the Fermi level in semimetal systems and could serve to achieve property fine-tuning for other bulk quantum materials with ultrahigh precision.