Physical-chemical Approach for the Impact of Modifying Molecular Bridges of TPA-Based Systems to Improve the Photovoltaic Properties of Organic Solar Cells

Abstract

The theoretical design of donor chromophores based on triphenylamine and 2-(1,1-dicyanomethylene)rhodanine (\textbf{DCRD-DCRD-2}) is proposed through structural adaptation with several molecular bridges derived from thiophene that can be used as new organic materials for organic solar cells (OSC). The optoelectronics properties and geometries of the \textbf{DCRD-DCRD-2} organic molecules are characterized using the B3LYP and CAM-B3LYP functional, with the basis set 6-31G(d,p). Consequently, the UV-Visible results revealed that a good relationship was found between the experimental values and the calculated using the DFT and TD-DFT level of theory. The study involved the prediction of photo-physical descriptors such as frontier molecular orbitals, ionization potential, electron affinity, molecular electrostatic potential, reorganization energy, open circuit voltage ($V_{oc}$), fill factor (FF), and short-circuit current ($J_{sc}$) in the ground state geometry, using the B3LYP/6-31G(d,p) basis set. Structural tailoring with various molecular bridges resulted in a narrowing of the energy gap (2.130--1.96eV) with broader absorption spectra (525.55--417.69 nm). An effective charge transfer toward the lowest unoccupied molecular orbitals (LUMO) from the highest occupied molecular orbitals (HOMO) was studied, which played a crucial role in conducting materials. \textbf{DCRD-2} exhibited $λ_{max}$ at $417.69$~nm in EtOH (ethanol) solvent with the lowest band gap (1.96 eV) and the lowest excitation energy of 2.968 eV. The highest mobility of holes and electrons is determined in all the designed molecules due to their low reorganization energy values that validated preferable photovoltaic properties in the \textbf{DCRD-1} molecular system.