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Coherent Raman scattering in liquid benzene from symmetric ring vibrations in the /sup 1/B/sub 2u/ electronic state excited by two-photon absorption

Journal Article · · J. Chem. Phys.; (United States)
OSTI ID:6695605
In the presence of two-photon absorption in benzene at 5268 A, we observe coherent anti-Stokes Raman scattering at 993 and 935 cm/sup -1/. These energies correspond to symmetric ring breathing vibrations (a/sub 1g/ symmetry) in the /sup 1/A/sub 1g/ ground, and /sup 1/B/sub 2u/ excited state of benzene, respectively. Raman activity in the latter state is demonstrated for the first time. Its observation is made possible by strong two-photon absorption to the /sup 1/B/sub 2u/ level via vibronically assisted transitions, and resonance enhancement of the Raman process by /sup 1/B/sub 2u/--/sup 1/E/sub 1u/ one-photon transitions. Simultaneously, we observe a resonance enhanced electronic background at the anti-Stokes frequency over a broad, featureless spectrum arising from two-photon transitions to /sup 1/B/sub 2u/. At wavelengths well below the two-photon absoprtion band of benezene, neither electronic contributions nor the 925 cm/sup -1/ peak are observed and only the ground state vibrations at 993 cm/sup -1/ remain.
Research Organization:
Department of Physics, Brown University, Providence, Rhode Island 02912
OSTI ID:
6695605
Journal Information:
J. Chem. Phys.; (United States), Journal Name: J. Chem. Phys.; (United States) Vol. 77:9; ISSN JCPSA
Country of Publication:
United States
Language:
English