Keremane, K.S.Planchat, A.Pellegrin, Y.Jacquemin, D.Odobel, F.Vasudeva Adhikari, A.2026-02-042022ChemSusChem, 2022, 15, 16, pp. -18645631https://doi.org/10.1002/cssc.202200520https://idr.nitk.ac.in/handle/123456789/22449Finding new efficient p-type sensitizers for NiO photocathodes is a great challenge for the development of promising low-cost tandem dye-sensitized solar cells (DSSCs). Now, the focus of researchers investigating these cells has been to create high-performance p-type systems. With this intention, herein, the design and synthesis of six new phenoxazine-based donor–acceptor (D–A)-configured organic dyes PO<inf>1–6</inf> was reported, comprising different acceptor moieties specially designed for the sensitization of mesoporous p-type semiconductor NiO for the construction of p-type DSSCs (p-DSSCs). This work includes structural, photophysical, thermal, electrochemical, theoretical, and photoelectrochemical studies of these dyes, including evaluation of their structure-property relationships. The optical studies revealed that PO<inf>1–6</inf> displayed adequate absorption and emission features in the range of 480–550 and 560–650 nm, respectively, with a bandgap in the order of 2.05–2.40 eV, and their thermodynamic parameters favored an efficient interfacial charge transfer involving NiO. Among the six new dyes, the device based on sensitizer PO<inf>2</inf> carrying electron-withdrawing 1,3-diethyl-2-thiobarbituric acid achieved the highest power conversion efficiency of 0.031 % (short-circuit current density=0.89 mA cm−2, open-circuit voltage=101 mV, and fill factor=35 %). Conclusively, the study furnishes an understanding of the intricacies involved in the structural modification of phenoxazine-based sensitizers to further ameliorate the performance of the p-type DSSCs. © 2022 Wiley-VCH GmbH.Charge transferDensity functional theoryField emission cathodesMagnetic semiconductorsNickel oxideOpen circuit voltagePhotovoltaic effectsSolar power generationCell effectsDensity-functional-theoryDye- sensitized solar cellsP-typePerformancePhenoxazinesPhotovoltaic performancePhotovoltaicsPush pullSensitiserDye-sensitized solar cells