Abstract
The two‐photon absorption properties of trans‐1,3‐butadiene have been calculated at an ab initio level employing RPA vertical excitation energies and transition moments and taking the random molecular orientation into account. For single‐beam two‐photon absorption with every possible combination of photon polarization the transition probability coefficients and polarization ratios for the low‐lying 1Ag and 1Bg final states are reported. The strongest two‐photon absorptivity is predicted under excitation from linearly polarized photons for 1Ag states and from circularly polarized photons for 1Bg states. The polarization ratios take sizably different values for the various 1Ag states. The case of concerted absorption of two photons with various polarizations from two laser beams has also been investigated exhaustively as a function of the photon frequencies.
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