The
innovative choice of core and periphery groups for organic
hole-transporting materials (HTMs) has gained more attention for modern
development in hybrid organic–inorganic perovskite solar cells
(PSCs). For large-scale application of PSCs, the replacement of 2,2′,7,7′-tetrakis(N,N-di-4-methoxyphenylamino)-9,9′-spirobifluorene
(spiro-OMeTAD) has its demands such as low stability, high cost, and
multistep synthesis. This has necessitated the introduction of novel
cost-effective HTMs. Hence, at first, we obtained a theoretical design
of tetraphenylethene (TPE)-based HTMs through the Gaussian method,
which exhibits a substantial highest occupied molecular orbital energy
level as compared with the perovskite. Further, the photophysical,
electrochemical, and thermal properties were meticulously investigated
with the aid of both experimental and computational methods. In order
to enhance the solubility of HTMs in chlorobenzene, the methoxy-substituted
phenyl group was replaced with the hexyloxy-substituted phenyl group,
and also, the higher extent of solubility is recognized after the
functional group exchanges. The power conversion efficiencies of TOHE
and TOME are η = 13.96%, J
sc = 21.00
mA/cm2, and V
oc = 0.93 (V)
and η = 6.83%, J
sc = 13.45 mA/cm2, and V
oc = 0.97 (V), respectively
(under full sunlight AM 1.5G, 100 mW cm–2 irradiation).
Moreover, the synthesis of highly stable TOHE involves a simple and
cost-effective synthetic procedure, proving to be the most promising
lead for designing efficient organic–inorganic hybrid solar
cells.