Abnormal spatial heterogeneity governing the charge-carrier mechanism in efficient Ruddlesden？Popper perovskite solar cells
- Abnormal spatial heterogeneity governing the charge-carrier mechanism in efficient Ruddlesden？Popper perovskite solar cells
- 김지영; Jun Xi; 변준섭; 김운수; 방기준; 한기림; 윤정진; Hua Dong; Zhaoxin Wu; Giorgio Divitini; Kai Xi; 박진우; 이태우; 최만수; 이종우; Seong Keun Kim
- Issue Date
- Energy & environmental science
- VOL 온라인게재, 온라인게재
- Layered Ruddlesden？Popper perovskite (RPP) photovoltaics have gained substantial attention owing to their excellent air stability. However, their photovoltaic performance is still limited by the unclear real-time charge-carrier mechanism of operating devices. Herein, we report the correlation between the charge-carrier mechanism and the spatially heterogeneous RPP bulks induced by distinct sublattice cations in the state-of-the-art antisolvent-driven RPP devices. In particular, abnormal heterogeneities ranging from the lateral long-range to local sub-grain scale and corresponding charge-carrier behaviours are visualized for triple-cation RPPs. We discovered that such heterogeneities with a unitary 2D/3D hybrid suppress lattice vibrations and reduce Fr？hlich interactions by about 2 times, significantly promoting charge-carrier dynamics. Consequently, optimized triple-cation RPP solar cells greatly outperform their mono-cation counterparts. Furthermore, this principle can be applicable irrespective of 2D layer thickness (n > 2) and substrate type. This work provides a rationale for leveraging a disordered structure to stimulate charge-carrier motion and suggests the design principle of low-dimensional perovskites.
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