Abstract
Abstract Polarized two-photon excitation spectra associated with the lowest absorption system of the phenanthrene crystal at T ∼ 4.2 K are reported. Intensity analyses for different principal faces reveal that the dominant intermediate states for the two-photon mechanism derive from molecular states of B 2(L) symmetry. This finding is consistent with theoretical calculations. The spectra principally associated with intermediate states of A 1(M) symmetry exhibit dramatic manifestations of intramolecular vibronic coupling which are in qualitative accord with coupling calculations. The origin region associated with the lower and upper Davydov components exhibits a marked dependence on photon propagation direction k and polarization. Included here are the center of gravity and profile of the so-called upper Davydov component. These results are discussed in terms of the exciton-phonon interactions.
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