Effect of heterocyclic and non-heterocyclic units on FDT-based hole transport materials for efficient perovskite solar cells: a DFT study

The development of a new structure is one of the important approaches for the advancement of efficient hole-transporting materials (HTMs). In this work, novel and efficient HTMs are designed based on the experimentally reported fluorene-dithiophene (FDT) system which shows the effect of four different units phenyl, pyridine, thiane, and oxane in the FDT unit. The structural, optoelectronic, and charge transport properties of the newly developed HTMs are probed using density functional theory (DFT) and time-dependent DFT (TD-DFT) methodologies. The calculated highest occupied molecular orbital (HOMO) energies for all HTMs are higher compared to the valence band energy level of the perovskite which exhibits outstanding hole extraction ability of all HTMs at the charge buffer interface. In addition, the designed HTMs have red-shifted absorption spectra compared to FDT. The computed hole mobilities of newly designed HTMs are faster compared to that of FDT. Moreover, newly tailored HTMs demonstrate improved solubility. The results indicate that a one thiane and one phenyl unit-based system among all materials is the most suitable for HTM design.