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Versatile quantum modes emerge for plasmon describing the collectiveoscillations of free electrons in metallic nanoparticles when the particlesizes are greatly reduced. Rather than traditional nanoscale study, theunderstanding of quantum plasmon desires extremal atomic control of thenanoparticles, calling for size dependent plasmon measurement over a series ofnanoparticles with atomically adjustable atom number over several orders ofmagnitude. Here we report the N dependent plasmonic evolution of atomicallysize selected gold particles with N= 100 70000 using electron energy loss (EEL)spectroscopy in a scanning transmission electron microscope. The EEL mappingassigns a feature at 2.7 eV as the bulk plasmon and another at 2.4 eV assurface plasmon, which evolution reveals three regimes. When N decreases from70000 to 887, the bulk plasmon stays unchanged while the surface plasmonexhibits a slight red shift from 2.4 to 2.3 eV. It can be understood by thedominance of classical plasmon physics and electron boundary scattering inducedretardation. When N further decreases from 887 to 300, the bulk plasmondisappears totally and the surface plasmon shows a steady blueshift, whichindicates that the quantum confinement emerges and modifies the intrabandtransition. When N 100 300, the plasmon is split to three fine features, whichis attributed to superimposed single electron transitions between the quantizedmolecular like energy level by the time dependent density functional theorycalculations. The surface plasmon's excitation ratio has a scaling law with anexponential dependence on N ( N^0.669), essentially the square of the radius. Aunified evolution picture from the classical to quantum, molecular plasmon isthus demonstrated.

Investigation of plasmonic evolution of atomically size-selected Au clusters by electron energy loss spectrum--from solid state to molecular scale