Band engineering of two-dimensional Ruddlesden–Popper perovskites for solar utilization: the relationship between chemical components and electronic properties

Abstract

Perovskite materials have been attracting much attention in recent years, especially in the field of energy conversion. However, the inherent disadvantages constrict the development of perovskites. Though many modification strategies have been proposed, the fundamental connection between those modifications and electronic properties is not clear. In this work, we investigated a series of Ruddlesden–Popper (RP) perovskites to explore the relationship between chemical components and their electronic properties. We revealed the influence of the components at A and B sites on band gaps and band edge positions by first-principles computations. After summarizing the design rules for RP perovskites, we proposed three new ones, MgSrMnO₄, Mg₂SrMn₂O₇ and MgSr₂Mn₂O₇. Computed electronic properties demonstrate that Mg₂SrMn₂O₇ has the suitable band gap and optimal light absorption, while MgSrMnO₄ also has the optimal band edge position at the same time. These two new perovskites have desirable potential for application in the field of luminous energy conversion. Therefore, the rules of band engineering can provide guidance for further development of RP perovskites for photovoltaic or photocatalytic applications.