Bottom-up holistic carrier management strategy induced synergistically by multiple chemical bonds to minimize energy losses for efficient and stable perovskite solar cells

The defects from electron transport layer,perovskite layer and their interface would result in carrier nonradiative recombination losses.Poor buried interfacial contact is detrimental to charge extraction and device stability.Here,we report a bottom-up holistic carrier management strategy induced synergistically by multiple chemical bonds to minimize bulk and interfacial energy losses for high-performance perovskite photovoltaics.4-trifluoromethyl-benzamidine hydrochloride(TBHCl)containing–CF_(3),amidine cation and Cl^(-)is in advance incorporated into SnO_(2)colloid solution to realize bottom-up modification.The synergistic effect of multiple functional groups and multiple-bond-induced chemical interaction are revealed theoretically and experimentally.F and Cl^(-)can passivate oxygen vacancy and/or undercoordinated Sn^(4+)defects by coordinating with Sn^(4+).The F can suppress cation migration and modulate crystallization via hydrogen bond with FA^(+),and can passivate lead defects by coordinating with Pb^(2+).The–NH_(2)–C=NH^(+)_(2)and Cl^(-)can passivate cation and anion vacancy defects through ionic bonds with perovskites,respectively.Through TBHCl modification,the suppression of agglomeration of SnO_(2)nanoparticles,bulk and interfacial defect passivation,and release of tensile strains of perovskite films are demonstrated,which resulted in a PCE enhancement from 21.28%to 23.40%and improved stability.With post-treatment,the efficiency is further improved to 23.63%.

Unraveling abnormal buried interface anion defect passivation mechanisms depending on cation-induced steric hindrance for efficient and stable perovskite solar cells

Although ionic liquids(ILs)have been widely employed to heal the defects in perovskite solar cells(PSCs),the corresponding defect passivation mechanisms are not thoroughly understood up to now.Herein,we first reveal an abnormal buried interface anion defect passivation mechanism depending on cationinduced steric hindrance.The IL molecules containing the same anion([BF4]^(-))and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface.It was revealed what passivated interfacial defects is mainly anions instead of cations.Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations,and facilitate the interaction between anions and SnO2as well as perovskites,which is conducive to interfacial defect passivation and ameliorating interfacial contact.It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations.The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite.Compared with the control device(21.54%),the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate(BAIMBF4)with maximum size cations achieves a significantly enhanced efficiency of 23.61%along with much increased moisture,thermal and light stabilities.