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The paper proposes a new approach to studying cathodoluminescence spectra ofsubstrate-free rare-gas clusters produced in supersonic jets exhausting into avacuum. The approach, which takes into account the fraction of the clusteredsubstance in the jet, is applied to quantitatively analyze integratedintensities of the luminescence bands of the neutral and charged excimercomplexes (Rg2)* and (Rg4+)* measured for nanoclusters of three rare gases (Rg= Ar, Kr, and Xe) with average sizes ranging from 100 to 18000 atoms perclusters (diameters varying from 2 to 13 nm). The amount of the clusteredsubstance, which affects the absolute values of integrated intensity of thebands, is shown to be proportional to the logarithm of the average size ofclusters in the jet. Analysis of normalized intensities allowed us tospectroscopically find two ranges of average sizes of Ar, Kr, and Xenanoclusters which, in accordance with the electron diffraction studies, can beassigned to quasicrystalline icosahedral and crystalline fcc structures inclusters, as well as to find the cluster size range in which both structurescoexist. We show that in fcc clusters the luminescence of the neutral molecules(Rg2)* comes from within the volume of the cluster, while the charged excimercomplexes (Rg4+)* emit mostly from subsurface layers.

Quasicrystalline and crystalline rare-gas clusters produced in supersonic jets: Impact of the jet clustering level on cathodoluminescence spectra