TY - JOUR
T1 - Nucleation Regulation and Mesoscopic Dielectric Screening in α-FAPbI3
AU - Tian, Ruijia
AU - Liu, Chang
AU - Meng, Yuanyuan
AU - Wang, Yaohua
AU - Cao, Ruikun
AU - Tang, Bencan
AU - Walsh, Darren
AU - Do, Hainam
AU - Wu, Haodong
AU - Wang, Kai
AU - Sun, Kexuan
AU - Yang, Shuncheng
AU - Zhu, Jintao
AU - Li, Xin
AU - Ge, Ziyi
N1 - Publisher Copyright:
© 2023 Wiley-VCH GmbH.
PY - 2024/3/28
Y1 - 2024/3/28
N2 - While significant advancements in power conversion efficiencies (PCEs) of α-FAPbI3perovskite solar cells (PSCs) have been made, attaining controllable perovskite crystallization is still a considerable hurdle. This challenge stems from the initial formation of δ-FAPbI3, a more energetically stable phase than the desired black α-phase, during film deposition. This disrupts the heterogeneous nucleation of α-FAPbI3, causing the formation of mixed phases and defects. To this end, polarity engineering using molecular additives, specifically ((methyl-sulfonyl)phenyl)ethylamines (MSPEs) are introduced. The findings reveal that the interaction of PbI2-MSPEs-FAI intermediates is enhanced with the increased polarity of MSPEs, which in turn expedites the nucleation of α-FAPbI3. This leads to the development of high-quality α-FAPbI3 films, characterized by vertical crystal orientation and reduced residual stresses. Additionally, the increased dipole moment of MSPE at perovskite grain boundaries attenuates Coulomb attractions among charged defects and screens carrier capture process, thereby diminishing non-radiative recombination. Utilizing these mechanisms, PSCs treated with highly polar 2-(4-MSPE) achieve an impressive PCE of 25.2% in small-area devices and 20.5% in large-area perovskite solar modules (PSMs) with an active area of 70 cm2. These results demonstrate the effectiveness of this strategy in achieving controllable crystallization of α-FAPbI3, paving the way for scalable-production of high-efficiency PSMs.
AB - While significant advancements in power conversion efficiencies (PCEs) of α-FAPbI3perovskite solar cells (PSCs) have been made, attaining controllable perovskite crystallization is still a considerable hurdle. This challenge stems from the initial formation of δ-FAPbI3, a more energetically stable phase than the desired black α-phase, during film deposition. This disrupts the heterogeneous nucleation of α-FAPbI3, causing the formation of mixed phases and defects. To this end, polarity engineering using molecular additives, specifically ((methyl-sulfonyl)phenyl)ethylamines (MSPEs) are introduced. The findings reveal that the interaction of PbI2-MSPEs-FAI intermediates is enhanced with the increased polarity of MSPEs, which in turn expedites the nucleation of α-FAPbI3. This leads to the development of high-quality α-FAPbI3 films, characterized by vertical crystal orientation and reduced residual stresses. Additionally, the increased dipole moment of MSPE at perovskite grain boundaries attenuates Coulomb attractions among charged defects and screens carrier capture process, thereby diminishing non-radiative recombination. Utilizing these mechanisms, PSCs treated with highly polar 2-(4-MSPE) achieve an impressive PCE of 25.2% in small-area devices and 20.5% in large-area perovskite solar modules (PSMs) with an active area of 70 cm2. These results demonstrate the effectiveness of this strategy in achieving controllable crystallization of α-FAPbI3, paving the way for scalable-production of high-efficiency PSMs.
KW - Dielectric screening
KW - Nonradiative decay
KW - Nucleation regulation
KW - Perovskite solar modules
KW - Polarity engineering
UR - http://www.scopus.com/inward/record.url?scp=85180695501&partnerID=8YFLogxK
U2 - 10.1002/adma.202309998
DO - 10.1002/adma.202309998
M3 - Article
C2 - 38108580
AN - SCOPUS:85180695501
SN - 0935-9648
VL - 36
JO - Advanced Materials
JF - Advanced Materials
IS - 13
M1 - 2309998
ER -