In designing material functionalities for transition metal oxides, lattice structure and d-orbital occupancy are key determinants. However, the modulation of these two factors is inherently limited by the need to balance thermodynamic stability, growth kinetics, and stoichiometry precision, particularly for metastable phases. We introduce a methodology, namely the gigantic-oxidative atomic-layer-by-layer epitaxy (GOALL-Epitaxy), enhancing oxidation power 3-4 orders of magnitude beyond conventional pulsed laser deposition (PLD) and oxide molecular beam epitaxy (OMBE), while ensuring atomic-layer-by-layer growth of designed complex structures. Thermodynamic stability is markedly augmented with stronger oxidation at elevated temperatures, whereas growth kinetics is sustained by laser ablation at lower temperatures. We demonstrate the accurate growth of complex nickelates and cuprates, especially an artificially designed structure with alternating single and double NiO2 layers possessing distinct nominal d-orbital occupancy, as a parent of high-temperature superconductor. The GOALL-Epitaxy enables material discovery within the vastly broadened growth parameter space.
@article{arxiv.2406.16520,
title = {Gigantic-oxidative atomic-layer-by-layer epitaxy for artificially designed complex oxides},
author = {Guangdi Zhou and Haoliang Huang and Fengzhe Wang and Heng Wang and Qishuo Yang and Zihao Nie and Wei Lv and Cui Ding and Yueying Li and Jiayi Lin and Changming Yue and Danfeng Li and Yujie Sun and Junhao Lin and Guang-Ming Zhang and Qi-Kun Xue and Zhuoyu Chen},
journal= {arXiv preprint arXiv:2406.16520},
year = {2025}
}