TY - JOUR
T1 - Probing two-photon properties of molecules
T2 - Large non-condon effects dominate the resonance hyper-Raman scattering of rhodamine 6G
AU - Milojevich, Chris B.
AU - Silverstein, Daniel W.
AU - Jensen, Lasse
AU - Camden, Jon P.
PY - 2011/9/21
Y1 - 2011/9/21
N2 - 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.
AB - 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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U2 - 10.1021/ja2054622
DO - 10.1021/ja2054622
M3 - Article
C2 - 21851085
AN - SCOPUS:80052789506
SN - 0002-7863
VL - 133
SP - 14590
EP - 14592
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 37
ER -