Hot luminescence from single-molecule chromophores electrically and mechanically self-decoupled by tripodal scaffolds

Nat Commun. 2023 Dec 12;14(1):8253. doi: 10.1038/s41467-023-43948-y.

Abstract

Control over the electrical contact to an individual molecule is one of the biggest challenges in molecular optoelectronics. The mounting of individual chromophores on extended tripodal scaffolds enables both efficient electrical and mechanical decoupling of individual chromophores from metallic leads. Core-substituted naphthalene diimides fixed perpendicular to a gold substrate by a covalently attached extended tripod display high stability with well-defined and efficient electroluminescence down to the single-molecule level. The molecularly controlled spatial arrangement balances the electric conduction for electroluminescence and the insulation to avoid non-radiative carrier recombination, enabling the spectrally and spatially resolved electroluminescence of individual self-decoupled chromophores in a scanning tunneling microscope. Hot luminescence bands are even visible in single self-decoupled chromophores, documenting the mechanical decoupling between the vibrons of the chromophore and the substrate.