Simulations of resonance hyper-Rayleigh scattering (HRS) for molecules and metal clusters in both resonance and off-resonance regions have been studied using TDDFT, with a new implementation by the ADF development groups of Lasse Jensen and Jochen Autschbach. An efficient algorithm based on damped quadratic response theory using the (2n+1) rule allows for studying the nonlinear optical properties (NLO, first-order hyperpolarizability β) of materials near one- and two-photon resonances.
Small silver clusters are shown to display strong two-photon enhanced HRS, making them interesting candidates for desiging new NLO materials.
NLO properties, TDDFT, (off-)resonance hyper-Raleigh scattering, nanoparticles
Z. Hu, J. Autschbach, and L. Jensen, Simulation of resonance hyper-Rayleigh scattering of molecules and metal clusters using a time-dependent density functional theory approach J. Chem. Phys., 141, 124305 (2014).Key conceptsnanoscience NLO TDDFT