Abstract
For the first time, systematic investigations of the damping parameter A of gold nanoparticles as a function of photon energy are presented. A is an essential parameter that quantifies the size-dependent optical properties of metal nanoparticles in the dielectric function. To determine the damping parameter, the dephasing time T 2 of gold nanoparticles has been systematically determined under ultrahigh vacuum conditions as a function of photon energy. Dephasing times ranging from \(T_2 = 5\) fs to \(T_2 = 17\) fs were measured, and subsequently, the damping parameter has been extracted. We found a strong resonance-like damping of the plasmon resonance in the vicinity of the onset of the interband transition. While the damping parameter scatters statistically around a value of \(A = 0.19\) nm/fs for photon energies below \(h\nu = 1.70\) eV, it increases rapidly to 0.32 nm/fs for \(h\nu = 1.85\) eV. For higher photon energies, A decreases steadily to \(A = 0.24\) nm/fs at \(h\nu = 2.15\) eV. A comparison to former measurements as well as to theoretical predictions reveals surface scattering and a discretizing and broadening of the band structure that influences the interband transition as the most dominant size-dependent damping mechanisms. The latter, i.e., a damping via increased interband transitions, assumes a coherent damping process of the oscillating electrons and, as a consequence, the plasmon is treated as a two-level system. Thus, the results deliver new physical insight to the fundamental understanding of surface plasmons.
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Financial support by the Deutsche Forschungsgemeinschaft, SPP 1093 is gratefully acknowledged.
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Hubenthal, F. Increased Damping of Plasmon Resonances in Gold Nanoparticles Due to Broadening of the Band Structure. Plasmonics 8, 1341–1349 (2013). https://doi.org/10.1007/s11468-013-9536-8
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DOI: https://doi.org/10.1007/s11468-013-9536-8