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The design of novel functional materials in silico is severely hampered bythe lack of robust and computationally efficient methods for describing bothmolecular absorbance and screening on substrates. Here we employ our hybrid$G_0[W_0+\Delta W]$-BSE implementation, which incorporates the substrate viaits screening $\Delta W$ at both the quasiparticle $G_0W_0$ level and whensolving the Bethe-Salpeter equation (BSE). We show this method can be used toboth efficiently and accurately describe the absorption spectra of physisorbedmolecules on metal substrates and thereby tailor the molecule's absorbance byaltering the surface plasmon's energy. Specifically, we investigate how theoptical absorption spectra of three prototypical $\pi$-conjugated molecules:benzene (C$_6$H$_6$), terrylene (C$_{30}$H$_{16}$) and fullerene (C$_{60}$),depends on the Wigner-Seitz radius $r_s$ of the metallic substrate. To gainfurther understanding of the light--molecule/substrate interaction, we alsostudy the bright exciton's electron and hole densities and their interactionswith infrared active vibrational modes. Our results show that (1) benzene'sbright $E_{1u}^1$ exciton at 7.0 eV, whose energy is insensitive to changes in$r_s$, could be relevant for photocatalytic dehydrogenation and polymerizationreactions, (2) terrylene's bright $B_{3u}$ exciton at 2.3 eV hybridizes withthe surface plasmon, allowing the tailoring of the excitonic energy and opticalactivation of a surface plasmon-like exciton, and (3) fullerene's $\pi-\pi^*$bright and dark excitons at 6.4 and 6.8 eV hybridize with the surface plasmon,resulting in the tailoring of their excitonic energy and the activation of botha surface plasmon-like exciton and a dark quadrupolar mode via symmetrybreaking by the substrate.

Tailoring a Molecule's Optical Absorbance Using Surface Plasmonics