Abstract
For the crystal and solution of 1-(3-thienyl)-3-(4-chlorophenyl)propene-1-one (TCPP), which is transparent over the whole visible region, the nonresonant third-order nonlinear dynamics is investigated by time-resolved degenerate four-wave mixing spectroscopy. The temporal nonlinear behaviors of both crystal and solution exhibit the instantaneous responses during 80 fs excitation at around 625 nm. The third-order nonlinear susceptibilities are determined to be |χ(3)bbbb| = 7.1 ×10-13 esu for crystal and |χ (3)TC1111| = 7.1 ×10-14 esu at 1 mol/l for solution. This suggests that the TCPP crystal has a large value of χ(3)/ατ= 2.4 ×103 esu·cm·s-1 under the assumption of the nonlinear response time τ= 30 fs (absorption coefficient α= 0.01 cm-1), which is a parameter important for ultrafast optical control materials. The obtained |χ(3)bbbb| value satisfies an already known relationship between the second- and third-order susceptibilities.
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