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First‐Principles Optimization of Out‐of‐Plane Charge Transport in Dion–Jacobson CsPbI 3 Perovskites with π‐Conjugated Aromatic Spacers
Author(s) -
Fang Zhi,
Hou Xinmei,
Zheng Yapeng,
Yang Zuobao,
Chou KuoChih,
Shao Gang,
Shang Minghui,
Yang Weiyou,
Wu Tom
Publication year - 2021
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.202102330
Subject(s) - materials science , conjugated system , perovskite (structure) , intercalation (chemistry) , chemical physics , charge (physics) , charge carrier , optoelectronics , nanotechnology , crystallography , inorganic chemistry , polymer , chemistry , physics , quantum mechanics , composite material
Quasi‐2D CsPbI 3 perovskites have emerged as excellent candidates for advanced photovoltaic technologies due to their fundamentally enhanced stability than conventional 3D counterparts. However, the applications of quasi‐2D perovskites are plagued with their poor out‐of‐plane carrier mobility induced by the intercalated insulating organic layers. In this work, a new strategy is explored to significantly enhance the out‐of‐plane charge transport in quasi‐2D Dion–Jacobson (DJ) CsPbI 3 perovskites via leveraging the intercalation of aromatic diamine cations ( p ‐phenylenediamine, PPDA) with unique π‐conjugated bond based on the first‐principles calculations. The strong interactions between PPDA 2+ cations and inorganic Pb‐I framework (i.e., I–I interaction, p ‐π coupling, and H‐bonds) provide three carrier pathways to facilitate the out‐of‐plane charge transport. Furthermore, the restricted in‐plane and out‐of‐plane structural distortion induced by the π‐conjugated bond could improve the electronic coupling and charge mobility along the out‐of‐plane direction with reduced bandgaps. As a proof of concept, the calculated average photovoltaic conversion efficiency of such engineered DJ CsPbI 3 perovskite solar cells is ≈17%, which is very close to the certificated champion efficiency of 3D α‐CsPbI 3 , underscoring their potential for solar cell applications.