Dye-sensitized halide perovskite systems have recently been demonstrated as promising candidates for photoelectrochemical devices. In this manuscript, we focus on the calcein dye-sensitized halide perovskite systems for aqueous-based photoelectrochemical system. This is achieved via the deposition of the commercially available self-assembled dye layer at the CH₃NH₃PbI₃/TiO₂ interface. Enhanced optoelectronic properties are obtained when the calcein dye is incorporated in the perovskite-based material. The photoelectrode consisting of the calcein/CH₃NH₃PbI₃ hybrid film produces a photocurrent value that is orders of magnitude higher than that from a bare CH₃NH₃PbI₃ photoelectrode under the same condition. In addition, the calcein dye improves the light-emitting properties of the CH₃NH₃PbI₃-based photoelectrode in water. The first-principles calculations suggest that multiple Lewis-acid-base coordination sites are available between the calcein dye and the halide perovskite substrate, such that the calcein dye could simultaneously enhance the light harvesting properties and passivates the perovskite electrode. This manuscript highlights the potentials of the multifunctional dye-sensitized halide perovskite materials, and facilitates the convergent understanding of halide perovskite materials for integrated optoelectronic devices.

染料敏化的卤化物钙钛矿体系最近被证明是光电化学装置的有希望的候选者。在本手稿中，我们重点研究用于水基光电化学系统的钙黄绿素染料敏化卤化物钙钛矿体系。这是通过在CH ₃ NH ₃ PbI ₃ / TiO ₂界面上沉积可商购的自组装染料层来实现的。当钙黄绿素染料掺入钙钛矿基材料中时，可获得增强的光电性能。由钙黄绿素/ CH ₃ NH ₃ PbI ₃杂化膜组成的光电极产生的光电流值比裸CH产生的光电流值高几个数量级。在相同条件下的₃ NH ₃ PbI ₃光电电极。另外，钙黄绿素染料改善了基于CH ₃ NH ₃ PbI ₃的光电极在水中的发光性能。第一性原理计算表明，钙黄绿素染料与卤化物钙钛矿基质之间存在多个路易斯酸-碱配位点，因此钙黄绿素染料可同时增强光收集性能并钝化钙钛矿电极。该手稿突出了多功能染料敏化卤化钙钛矿材料的潜力，并促进了对集成光电器件卤化钙钛矿材料的一致理解。