Two
structural isomers of carbazole decorated with triarylamine
have been designed and synthesized with a facile synthetic procedure.
The impact of triarylamine substitution on the isomeric structural
linkage of carbazole on the optical, thermal, electrochemical, and
photovoltaic properties has been extensively studied by combining
experimental and simulation methods. Car[2,3] showed
a red shift in the absorption maximum compared to that of Car[1,3], indicating the linear conjugation along the 2,7-position of carbazole
in the former. The high thermal decomposition temperature (>420
°C)
of these compounds could be attributed to the rigid structure of the
carbazole core. Perovskite solar cells fabricated with Car[2,3] as the hole transporting material (HTM) displayed the highest power
conversion efficiency (PCE) of 19.23%. It can be attributed to the
suitable energy alignment of the highest occupied molecular orbital
(HOMO) of HTM with the adjacent perovskite valence band energy level,
which results in efficient hole transport. Furthermore, the molecular
dynamic simulation demonstrates that the triphenylamine substitution
on the 2,3,6,7 positions of Car[2,3] results in a more
planar molecular alignment on top of the perovskite surface, promoting
an efficient hole extraction. Essentially, when Car[1,3] and Car[2,3] were applied in perovskite solar cells,
they showed enhanced long-term stability by retaining >80% of their
initial PCEs after 1000 h of continuous illumination.