Impact of functional groups in spacer cations on the properties of PEA-based 2D monolayer halide perovskites  

作　　者：Chenchen Li Xian Chen Tan Jin Tianmin Wu Jun Chen Wei Zhuang 

机构地区：[1]Key Laboratory of Opto-Electronic Science and Technology for Medicine of Ministry of Education,College of Physics and Energy&College of Photonic and Electronic Engineering,Fujian Normal University,Fuzhou,350117,PR China [2]State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,350002,PR China [3]College of Artificial Intelligence,Yango University,Fuzhou,350015,PR China [4]Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry,Xiamen,361005,PR China [5]Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China,Fuzhou,Fujian,350108,PR China

出　　处：《Nano Materials Science》2025年第1期74-82,共9页纳米材料科学(英文版)

基　　金：supported by the National Natural Science Foundation of China(Grant Nos.22103012,22173104);Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(FJOEL,Grant No.2021ZR109);the Future-prospective and Stride-across Programs of Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences(Grant No.CXZX-2022-GH02)。

摘　　要：Incorporating low-dimensionalization technologies effectively tackle the challenge of inadequate long-term stability in hybrid halide perovskites,however their wide bandgap and strong quantum well confinement remain substantial obstacle for various optoelectronic applications.Addressing these issues without compromising longterm stability has emerged as a pivotal focus in materials science,in particular exploring the effects of the functional groups within spacer cations.Our simulations reveal that the robustπ-πstacking interactions involving PEA^(+)and the strong hydrogen bonding interactions between PEA^(+)and MX^(4-)_(6)contribute to narrowing the electronic bandgap in 2D monolayer PEA_(2)MX_(4)(e.g.2D monolayer PEA_(2)SnI_(4):1.34 eV)for reasonable visible-light absorption while simultaneously ensuring their favorable long-term stability.Moreover,the delocalized orbitals and relatively high dielectric constants in PEA^(+),attributed to the conjugated benzene ring,has been observed to weaken the potential barrier,exciton binding effect and quantum well confinement in 2D monolayer PEA2MX4,thus facilitating photogenerated electron-hole separations and out-of-plane carrier transport.The impact of spacer cations on the optoelectronic and transport properties of 2D monolayer perovskites highlights the critical role of meticulously chosen and well-designed spacer cations,especially functional groups,in shaping their photophysical properties and ensuring long-term stability even under extremely operating conditions.

关 键 词：Long-term stability Exciton binding effect Quantum transport First-principles calculations Quantum well confinement 

分 类 号：O469[理学—凝聚态物理]