The relative abundances of C 60 Cs͑N͒, N # 500, determined from mass spectra measurements, are presented and explained in terms of the successive filling of the electronic shells by the cesium valence electrons. The motion of the Cs valence electrons, confined to a metal layer surrounding the C 60 molecule, is described within the jellium model, with Cs spread into a uniform positive background. The electronic shell structure is calculated with the local approximation to density-functional theory and is shown to correspond to measured abundances. Strong Friedel oscillations in the electronic density are found and closed forms for them are given for jellium spheres both with and without the void. [S0031-9007(96) Recently alkali clusters have been shown to exhibit an electronic shell structure, which can be described in a jellium model where the alkali valence electrons move in the uniform positive background of the ions [1][2][3][4][5]. The stability of these clusters as a function of size (i.e., as a function of the number of jellium electrons) is described in terms of occurrence of closed electronic shells.In this paper we describe a new system, C 60 Cs͑N͒ (a buckyball coated with N Cs atoms), for which relative abundances are also shown to be described reasonably well in terms of the electronic shell structure within the jellium model. These metal-coated buckyballs were produced by coevaporation of fullerenes and cesium metal in a gas aggregation cell [6]. They were subsequently ionized with monochromatic photons and analyzed with a time-offlight mass spectrometer. The ionization energy of the cluster oscillates with the size of the cluster, which is caused by the successive filling of the electronic shells of the C 60 Cs͑N͒ system. For certain values of the total number of electrons, all electronic shells are either completely filled or completely empty. Addition of just one more electron causes a new shell to open up leading to a drop in the ionization energy. It is tedious and virtually impossible to ionize each individual cluster and measure its ionization energy. Fortunately, the shell oscillations can be observed in a much simpler experiment where the clusters are ionized with photons followed by a measurement of a single mass spectrum. The photon energy is chosen in such a way that it is large enough to ionize the openshell clusters, but is too small to ionize the closed-shell clusters. Clusters with closed-shell structures are therefore not ionized and do not appear in the mass spectra.Thus dips in the mass spectra correspond to closed-shell clusters.Figure 1(a) shows the measured mass spectra of C 60 Cs͑N͒ clusters ionized at different photon energies. The dips in the mass spectra are indicated by the corresponding number N of cesium atoms.The C 60 Cs͑N͒ system is a very complicated system for exact electronic-structure studies and it is therefore desirable to develop approximate models that can describe its main features and which, furthermore, provide general insight into its properties. We shall he...