Simulation of resonance hyper-Rayleigh scattering of molecules and metal clusters using a time-dependent density functional theory approach

Zhongwei Hu, Jochen Autschbach, Lasse Jensen

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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 \documentclass[12pt]{minimal}\begin{document}$\rm {Ag-8}$\end{document} Ag 8 and \documentclass[12pt]{minimal}\begin{document}$\rm {Ag-{20}}$\end{document} 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.

Original languageEnglish (US)
Article number124305
JournalJournal of Chemical Physics
Issue number12
StatePublished - Jan 1 2014


All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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