Electron spill-out effect on third-order optical nonlinearity of metallic nanostructure

Abstract

Over the last three decades, plasmonics using metallic nanostructures has become central to nanophotonics research. Recently, its targets have been extended to nonlinear optical phenomena. In a nonlinear regime, quantum mechanical effects, as exemplified by electron spill-out on the surface of nanostructures, significantly influence the optical response. Quantum hydrodynamic theory (QHT) is a promising basis for the analysis of nonlinear optical responses involving such quantum mechanical effects. Herein, QHT was applied to calculate the third-order optical nonlinearity of a spherical metallic nanostructure. The results demonstrate how electron spill-out strongly affects plasmon resonance and third-order optical nonlinearity.

29 pages, 6 figures

References in corpus (3)

• Nonlocal optical response in metallic nanostructures
• Resonance shifts and spill-out effects in self-consistent hydrodynamic nanoplasmonics
• Time-dependent Orbital-free Density Functional Theory: Background and Pauli kernel approximations