title: Simulation of resonance hyper-Rayleigh scattering of molecules and metal clusters using a time-dependent density functional theory approach.
abstract: Resonance hyper-Rayleigh scattering (HRS) of molecules and metal clusters have been simulated based on a time-dependent density functional theory approach. The resonance first-order hyperpolarizability (β) is obtained by implementing damped quadratic response theory using the (2n + 1) rule. To test this implementation, the prototypical dipolar molecule para-nitroaniline (p-NA) and the octupolar molecule crystal violet are used as benchmark systems. Moreover, small silver clusters Ag 8 and Ag 20 are tested with a focus on determining the two-photon resonant enhancement arising from the strong metal transition. Our results show that, on a per atom basis, the small silver clusters possess two-photon enhanced HRS comparable to that of larger nanoparticles. This finding indicates the potential interest of using small metal clusters for designing new nonlinear optical materials.
authors.affiliation: Department of Chemistry, The Pennsylvania State University, 104 Chemistry Building, University Park, Pennsylvania 16802-4615, USA.
authors.forename: Zhongwei
authors.initials: Z
authors.lastname: Hu
authors.affiliation: Department of Chemistry, University at Buffalo, State University of New York, Buffalo, New York 14260-3000, USA.
authors.forename: Jochen
authors.initials: J
authors.lastname: Autschbach
authors.affiliation: Department of Chemistry, The Pennsylvania State University, 104 Chemistry Building, University Park, Pennsylvania 16802-4615, USA.
authors.forename: Lasse
authors.initials: L
authors.lastname: Jensen
mesh_terms: D000465:Algorithms; D000814:Aniline Compounds / Q000737:chemistry*; D003198:Computer Simulation; D005740:Gases / Q000737:chemistry; D005840:Gentian Violet / Q000737:chemistry*; D053768:Metal Nanoparticles / Q000737:chemistry*; D008956:Models, Chemical; D017711:Nonlinear Dynamics; D012542:Scattering, Radiation; D012834:Silver / Q000737:chemistry*; D013057:Spectrum Analysis
chemical_list: D000814:Aniline Compounds; D005740:Gases; C019498:4-nitroaniline; D012834:Silver; D005840:Gentian Violet