To drive the development of perovskite
solar cells (PSCs), hole-transporting
materials are imperative. In this context, pyridine derivatives are
being probed as small molecules-based hole-transporting materials
due to their Lewis base and electron-deficient unit. Herein, we focused
our investigation on pyridine isomer molecules 4,4′-(10-(pyridin-
x
-yl)-10H-phenothiazine-3,7-diyl)bis(N,N-bis(4-methoxyphenyl)aniline) (
x
= 2, 3, or 4), in which the pyridine nitrogen heteroatom is located at
the 2, 3, and 4 positions, named as 2PyPTPDAn, 3PyPTPDAn, and 4PyPTPDAn, respectively. We decipher
the structure–properties–device performance relationship
impacted by the different N-atom positions in pyridine.
In the case of 3PyPTPDAn, the partial orbital overlap
between highest occupied molecular orbital (HOMO) and the lowest unoccupied
molecular orbital (LUMO) favors the generation of neutral excitons
and hole transport, as well as improves the film-formation ability,
and this induces efficient hole extraction as compared to their 2,4
analogues. The solar cells fabricated with 3PyPTPDAn gave
on-par photovoltaic performance as that of typical Spiro-OMeTAD, and
higher performance than those of 2PyPTPDAn and 4PyPTPDAn. The hydrophobicity and homogeneous film properties
of 3PyPTPDAn add merits to the stability. This work emphasizes
the guidelines to develop small molecules for organic solar cells,
organic light-emitting diodes, and thermally activated delayed fluorescence.