Shortcomings associated with metal-free dye-sensitized solar cells can be overcome with dye modification. Using Density Functional Theory (DFT) and Time Dependent (TD-DFT), acridine orange dyes (main Donors) are modified with molecular moieties (2-Hydroxy-4-propoxyphen)(phenyl)methanone (UV absorber), 4,4'-Dimethoxydiphenylamine (Donor 1), 2-(Thiophen-2-yl)-1,3,4-oxadiazole (π-bridge), anisole (Donor 2), cyanoacetic-acid and carboxylic-acid functional groups (Acceptors 1 and 2), to form new UV Absorber-D-(A)₂ and D’- π -D-(A)₂ dyes with least computational costs, where acridine derivatives act as main donors. Absorption spectra, highest-occupied molecular orbitals, and lowest-unoccupied molecular orbitals are predicted by DFT and TD-DFT calculations. Ionization potential, electron affinity, electronegativity and light-harvesting efficiency are predicted with frontier-molecular orbital energies by Koopmans' theorem, using TiO₂ conduction-band edge (E_CB -4.0 eV) and [I^-/I₃^-] redox-potential (-4.80 eV). Absorption redshifts with expanded range of 700 nm, and improved energy-alignment with TiO₂, charge-transfer processes, redox-couple compatibility, cell stability and higher performance are all achieved by molecular level tuning of dyes.

Title

Computational and Theoretical Chemistry

Publisher

Elsevier

Publisher Country

Netherlands

Indexing

Thomson Reuters

Impact Factor

2.8

Publication Type

Both (Printed and Online)

Volume

1234

Year

2024

Pages

114550