We study the impact of organic surface ligands on the electronic structure and electronic band edge energies of quasi-two-dimensional (2D) colloidal cadmium selenide nanoplatelets (NPLs) using density functional theory. We show how control of the ligand and ligand-NPL interface dipoles results in large band edge energy shifts, over a range of 5 eV for common organic ligands with a minor effect on the NPL band gaps. Using a model self-energy to account for the dielectric contrast and an effective mass model of the excitons, we show that the band edge tunability of NPLs together with the strong dependence of the optical band gap on NPL thickness can lead to favorable photochemical and optoelectronic properties.
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