Revealing time characteristics of optical excitations in dielectric and plasmonic structures through cathodoluminescence interferometry

Abstract

Cathodoluminescence (CL) spectroscopy provides access to optical excitations with nanometer spatial resolution, but direct time-resolved measurements of optical resonances remain challenging. Here, we demonstrate that CL interferometry provides access to the temporal response, phase behavior, and modal spectral structure of resonant nanoscale scatterers without requiring ultrafast pump-probe schemes. We develop an analytical framework in which Fourier transformation angle- and frequency-resolved CL interferograms yields the decay time of optical resonances governed by the linear optical response. Multimode resonators exhibit characteristic temporal CL beating signatures associated with spectral mode splitting. By exploiting transition radiation emitted from a nearby metallic surface as a broadband reference, we further demonstrate phase retrieval and cross-correlation measurements between instantaneous and resonant emission processes. Experimental measurements on Au nanoparticles, broadband plasmonic emitters, Au nanostars, and Si nanospheres supporting multipolar Mie resonances confirm the theoretical predictions, and decay times in the range 1-10 fs are derived for each system. Our results establish CL interferometry as a powerful approach for accessing spectral, spatial, and phase information within a single nanoscale measurement with fs resolution.