Here, we report on a new kind of compound, X delta Ir4X12-delta(X = P, As), thefirst hole-doped skutterudites superconductor. We provide atomic-resolution images ofthe caging As atoms using scanning transmission electron microscopy (STEM). Byinserting As atoms into the caged structure under a high pressure, superconductivityemerges with a maximum transition temperature (Tc) of 4.4 K (4.8 K) in IrAs3(IrP3).In contrast to all of the electron-doped skutterudites, the electronic states around theFermi level in X delta Ir4X12-delta are dominated by the caged X atom, which can be described bya simple body-centered tight-binding model, implying a distinct pairing mechanism. Ourdensity functional theory (DFT) calculations reveal an intimate relationship betweenthe pressure-dependent local-phonon mode and the enhancement ofTc. The discoveryof X delta Ir4X12-delta provides an arena to investigate the uncharted territory of hole-doped skutterudites, and the method proposed hererepresents a new strategy of carrier doping in caged structures, without introducing extra elements
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