Probing two-photon properties of molecules: Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G

Chris B. Milojevich, Daniel W. Silverstein, Lasse Jensen, Jon P. Camden

Research output: Contribution to journalArticle

28 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)14590-14592
Number of pages3
JournalJournal of the American Chemical Society
Volume133
Issue number37
DOIs
StatePublished - Sep 21 2011

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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