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Letter

Nature 280, 304-306 (26 July 1979) | doi:10.1038/280304a0; Accepted 14 June 1979

Two-photon absorption spectra and cross-section measurements in liquids

A. C. TAM & C. K. N. PATEL

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THE recently developed high-sensitivity opto–acoustic (OA) absorption measurement technique1 has proved ideal for the measurement of a variety of weak absorption phenomena in liquids2–4. We report here the results of an investigation of two-photon absorption in liquid benzene using the OA technique. Weak two-photon spectra (cross-section less than or similar to10-51 cm4 molecule-1 photon-1 s) in nonfluorescing liquids have been difficult to measure. The only previous published study for such a measurement used thermal blooming5, which is difficult to interpret theoretically and apparently produces a poor signal-to-noise ratio. We demonstrate here that far superior spectra can be obtained by the simple and sensitive two-photon OA spectroscopy (TPOAS) technique. Polarisation dependence, vibrational intervals and electronic origin are obtained, and two-photon absorption cross-sections are derived for the first time in this study for the case of a weak two-photon absorption band in liquid benzene. Note that Bonch-Bruevich et al.6 have recently attempted similar two-photon OA measurements, but they can only measure strong absorption (cross-section greater than or similar to10-48 cm4 molecule-1 s) with a poor signal-to-noise ratio.