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Disentangling the contributions of radiative and non-radiative localizedplasmonic modes from the photonic density of states of metallic nanocavitiesbetween atomically-sharp tips and flat substrates remains an experimentalchallenge nowadays. Electroluminescence due to tunnelling through thetip-substrate gap allows discerning solely the excitation of radiative modes,but this information is inherently convolved with that of the electronicstructure of the system. In this work we present a fully experimental procedureto eliminate the electronic-structure factors from the scanning tunnellingmicroscope luminescence spectra by confronting them with spectroscopicinformation extracted from elastic current measurements. Comparison againstelectromagnetic calculations demonstrates that this procedure allowscharacterizing the meV shifts experienced by the dipolar and quadrupolarplasmonic modes supported by the nanocavity under atomic-scale gap sizechanges. Our method, thus, gives us access to the frequency-dependent radiativePurcell enhancement that a microscopic light emitter would undergo when placedat the nanocavity.

Unveiling the Radiative Local Density of Optical States of a Plasmonic Nanocavity by STM Luminescence and Spectroscopy