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Following the lifespan of optical excitations from their creation to decayinto photons is crucial in understanding materials optical properties.Macroscopically, techniques such as the photoluminescence excitationspectroscopy provide unique information on the photophysics of materials withapplications as diverse as quantum optics or photovoltaics. Materialsexcitation and emission pathways are affected by nanometer scale variationsdirectly impacting devices performances. However, they cannot be directlyaccessed, despite techniques, such as optical spectroscopies with freeelectrons, having the relevant spatial, spectral or time resolution. Here, weexplore optical excitation creation and decay in two representative opticaldevices: plasmonic nanoparticles and luminescent 2D layers. The analysis of theenergy lost by an exciting electron that is coincident in time with avisible-UV photon unveils the decay pathways from excitation towards lightemission. This is demonstrated for phase-locked interactions, such as inlocalized surface plasmons, and non-phase-locked ones, such as the lightemission by individual point defects. This newly developed cathodoluminescenceexcitation spectroscopy images energy transfer pathways at the nanometer scale.It widens the toolset available to explore nanoscale materials.

Cathodoluminescence excitation spectroscopy: nanoscale imaging of excitation pathways