Abstract
Abstract We found unique burning power dependence in the hole formation of linear Frenkel exciton system, J-aggregates of pseudo-isocyanine bromide, in water-ethylene glycol glasses at 4.7 K. With DC-laser light for burning, clear zero-phonon hole was formed with the width of 0.36 cm−1. Once switching the laser for burning to the pulse mode operation, on the other hand, nano-second pulses e.g. can give rise to novel feature of dispersive lineshape of spectral change from the initial stage of burning: a broad and red-shifted (∼3 cm−1 from the laser frequency ωB) non-resonant hole accompanied by antihole with similar size at shorter wavelength side. We consider the appearance of red-shifted nonresonant hole is essential in the present situation and is due to the two-exciton excitation through one-exciton transition by two-photon absorption. Based on this model, the shift of the hole is equal to half of the difference of k = 2 and k = 1 exciton energy, from which we can estimate the coherence length of N = 5...
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