Probing two-photon properties of molecules: large non-Condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G |
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Authors: | Milojevich Chris B Silverstein Daniel W Jensen Lasse Camden Jon P |
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Institution: | Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996-1600, USA. |
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Abstract: | Experimentally measured resonance hyper-Raman (RHR) spectra spanning the S(1) ← S(0), S(2) ← S(0), and S(3) ← S(0) transitions in rhodamine 6G (R6G) have been recorded. These spectra are compared to the results of first-principles calculations of the RHR intensity that include both Franck-Condon (A-term) and non-Condon (B-term) scattering effects. Good agreement between the experimental and theoretical results is observed, demonstrating that first-principles calculations of hyper-Raman intensities are now possible for large molecules such as R6G. Such agreement indicates that RHR spectroscopy will now be a routine aid for probing multiphoton processes. This work further shows that optimization of molecular properties to enhance either A- or B-term scattering might yield molecules with significantly enhanced two-photon properties. |
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