The dataset for the article "Vacancy-mediated covalent bridge formation governs facet-dependent bonding and band-edge alignment at CsPbBr₃/ZnO interfaces"

Dataset for the article "Vacancy-mediated covalent bridge formation governs facet-dependent bonding and band-edge alignment at CsPbBr₃/ZnO interfaces" Krzysztof Pyrchla, Ghulam Abbas, Egor Ukraintsev, Bohuslav Rezek Faculty of Electrical Engineering, Czech Technical University in Prague, Technická 2, 16627 Prague, Czechia Simulation scripts for Quantum ATK for 5 different ZnO surface terminations and 2 different orientations of CPB.Folders with simulation scripts for different ZnO surfaces and CPB orientations:1 000-1+CPB_Cs2 000-1+CPB_Pb3 000-1+OH05+CPB_Cs4 000-1+OH05+CPB_Pb5 0001+CPB_Cs6 0001+CPB_Pb7 10-10+CPB_Cs8 10-10+CPB_Pb9 11-20+CPB_Cs10 11-20+CPB_Pb11 CPB_PESDIRECT12 Slab_optimisation_PESDIRECT Abstract:Interfaces between halide perovskites and oxide electron-transport contacts govern carrier injection, band alignment, and device stability, yet the atomistic rules connecting oxide surface polarity to interfacial bond formation and band-edge reconstruction remain unresolved. Here, we employ machine-learning force-field optimisation and dielectric-dependent hybrid DFT with spin–orbit coupling to resolve bonding and electronic structure at CsPbBr₃/ZnO across four low-index ZnO orientations and two perovskite terminations. We reveal that PbBr₂-terminated CsPbBr₃ binds to Zn-terminated ZnO at −11.5 eV – more than twice the −4.5 eV of CsBr-terminated surfaces – owing to cooperative Pb substitution at Zn vacancies and Zn–Br bridge formation governed by surface polarity and defect exposure. Polar ZnO facets induce the strongest band-edge hybridisation and introduce facet-dependent electronic states near the conduction-band minimum, offering a handle for tuning carrier injection. These findings provide a predictive atomistic framework for the surface engineering of oxide electron-transport contacts in CsPbBr₃-based photodetectors and radiation sensors. Keywords: CsPbBr₃ perovskite, Perovskite–oxide interface, Hybrid heterostructures, DFT modelling