Abstract
The surface-enhanced hyper-Raman (SEHRS) spectra of Rhodamine 6G (R6G) are measured for two different excitation energies: ∼25 000 cm–1 (∼810 nm) and ∼19 000 cm–1 (1030 nm). The collected spectra are compared to time-dependent density functional theory simulations of the resonance hyper-Raman spectra for the same excitation energies. The analysis of molecular orbital changes in these nonlinear transitions elucidates the mechanism of vibronic enhancement. This analysis is used to elucidate features in the two-photon absorption spectra of R6G.
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