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 \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 language | English (US) |
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Article number | 124305 |
Journal | Journal of Chemical Physics |
Volume | 141 |
Issue number | 12 |
DOIs | |
State | Published - Sep 28 2014 |
All Science Journal Classification (ASJC) codes
- Physics and Astronomy(all)
- Physical and Theoretical Chemistry