Pyrrole/thiophene π‐bridged two triphenylamine electron donor and substituted thiobarbituric electron acceptor for D‐π‐A‐D‐featured DSSC applications.

We designed a series of organic dyes based on two triphenylamine units (electron donors), pyrrole/thiophene (π‐bridge) and N‐substituted alkyl thiobarbituric acid (electron acceptors) to construct the D‐π‐A‐D photosensitizer systems. The electronic structures and photophysical properties of the sensitizers were investigated by density functional theory (DFT) and time‐dependent DFT (TD‐DFT). The potential use of the dyes as photosensitizers in DSSCs was explored by calculating the light harvesting efficiency (LHE), electrons driving force injection (ΔGinject), the open‐circuit photovoltage (VOC), and surface interaction with semiconductor (TiO2). From alkyl‐substituted sensitizers, N‐ethyl derivatives TPAA3 and TPAB3 performance for ΔGinject (−1.69 and −1.65 eV) and VOC (1.43, and 1.11 eV) was superior to the other dyes. In addition, the anchoring ability of the N‐substituted alkyl derivatives was higher than the cyanoacrylic dyes. [ABSTRACT FROM AUTHOR]