Intermediate-States Mediated 2D MoO3-x Plasmon Enabling Pure-Phased CsPbX3 Photovoltaics with 27.33% Bifacial Efficiency

All-inorganic CsPbX 3 (X = I, Br, Cl) perovskites emerged as a crucial material for addressing the stability bottleneck due to their exceptional resistance to both light-thermal stress. However, their performance is limited by adverse optoelectronic dissipation arising from inadequate photon conversion and chaotic carrier energetics. Herein, the mechanism of the unique nonlinear plasmonic effect in van der Waals 2D MoO 3-x is elucidated, which is mediated by electronic intermediate states. It demonstrates that the 2D MoO 3-x serves as a light-capture-antenna in heterodimensional CsPbX 3 -MoO 3-x optically coupled system, contributing to the accumulation the optical field energy on the nanoscale and resulting in a remarkable 59% increase in photon convergence. Additionally, facet-oriented carrier channels can be established through heteroepitaxy along matched Mo-O octahedron. This optoelectrical-bimodal-coupling engineering combined with a bifacial light-harvesting configuration yields a bifacial equivalent efficiency of 27.33%, which stands as the supreme performance in all-inorganic perovskite photovoltaics. Graphical This remarkable work combines supercritical CO 2 chemical engineering, two-dimension plasmon photophysical science, and perovskite photovoltaic technology. It introduces novel concepts like broad - spectrum coupled photon absorption, the intermediate - localized - states model, and optoelectrical - bimodal - coupling engineering. It aims to combat optoelectronic dissipation and enhance energy harvesting via a heterodimensional van der Waals optically coupled system.