Fine structural tuning of diphenylaniline-based dyes for designing semiconductors relevant to dye-sensitized solar cells

Motivated by recent study on synthesized N, N-diphenylaniline (DPA)-based dyes [DOI: https://doi.org/10.1016/j.solener.2022.01.062 ] for use in dye-sensitized solar cells (DSSCs), we theoretically design several dyes and explore their potential for enhancing the efficiency of DSSCs. Our designed dyes are based on the molecular structure of synthesized DPA-azo-A and DPA-azo-N dyes with a donor-π-bridge-acceptor (D-π-A) framework. In this research, we aim to develop the power conversion efficiency (PCE) of DSSCs by fine-tuning the molecular structure of the synthesized dyes. To this end, we focus on designing dyes by replacing the units of DPA-azo-A and DPA-azo-N with a variety of donor, π-bridge, and acceptor. Hence the density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations are done to explore their structure, electronic, optical, charge transport, and photovoltaic properties. Among all newly designed and reference dyes, the D3-azo-N and DPA-π3-N dyes which are designed by substituting the donor (DPA) and π-bridge (azo) units of DPA-azo-N with D3 and π3, respectively exhibit the highest PCE of 45.46% (for D3-azo-N) and 43.20% (for DPA-π3-N) and can be favorable dyes for improving the efficiency of DSSCs. Therefore, the dyes that are designed by substituting the donor and π-bridge units of synthesized dyes have more impact on improving the efficiency of DSSCs than those that involve replacing the acceptor units. Consequently, our theoretical findings will provide valuable insights for the experimentalists to employ these novel effective dyes and boost the performance of DSSCs.