Tailoring anchoring functionalities of self-assembled materials for efficient wide-bandgap perovskite solar cells
Journal
Chemical Engineering Journal
Journal Volume
526
Start Page
171321
ISSN
13858947
Date Issued
2025-12-15
Author(s)
Shi, Zhong-En
Fu, Yu-Fan
Peng, Bo-Shun
Hung, Ting-Chun
Ganesan, Deebakkrishnan
Balasaravanan, Rajendiran
Hong, Shao-Huan
Su, Chun-Jen
Chen, Ming-Chou
Chen, Chih-Ping
Abstract
The strategic passivation of interfacial defects and modulation of perovskite crystallization via the hole-selective layer (HSL) have emerged as pivotal approaches to advancing perovskite solar cell (PSC) performance. Here, we report the rational design of dithienobenzothiadiazole (DTPBT)-based self-assembled monolayers (SAMs) featuring diverse anchoring groups—carboxylic acid (CA), dicyanovinyl (MN), diethyl phosphonate (PE), and phosphonic acid (PA)—as HSLs for PSCs. Through systematic investigation, we elucidate how these SAMs influence NiOx surface chemistry, energy level alignment, carrier extraction dynamics at the HSL/perovskite interface, and the resulting optoelectronic properties of PSCs. Among the SAM variants, DTPBT-CA demonstrates the most significant performance enhancements. Notably, incorporating a co-SAM strategy with 4PADBC yields a denser, more uniform monolayer, mitigates molecular aggregation, and further optimizes interfacial energetics and charge extraction, culminating in improved perovskite crystallinity. Devices utilizing the optimized co-SAM approach achieve a power conversion efficiency (PCE) of 21.35 ± 0.71 % for the methylammonium-free wide-bandgap PSCs under AM 1.5G illumination, and an indoor PCE of 42.44 ± 1.02 % (WLED, 1000 lx). Our findings underscore the synergistic potential of molecular design and co-assembly in interfacial engineering to unlock high-performance PSCs across varied operational environments.
Subjects
Dithienobenzothiadiazole
Hole selective layer
Indoor photovoltaics
Interfacial engineering
Perovskite
Solar cell
Publisher
Elsevier B.V.
Type
journal article