Dispersive Line Shape of Persistent Spectral Hole-Burning Observed in Pseudo-Isocyanine Bromide J-Aggregates and Its Exciton-Phonon Interaction

Abstract

Abstract Hole formation profiles of the exciton band of J-aggregates of pseudo-isocyanine bromide / water-ethyleneglycol system were carefully examined and significant difference of the burning sources, DC-light laser or nanosecond pulsed laser was observed. The results on the upper J-band are described mainly though the essential features are commonly observed also in the lower band. In the former case clear zero-phonon hole was formed with the width of 0.4 cm−1. Assuming negligible contribution of the dephasing by phonons the homogeneous width of the one-exciton state is lifetime-limited in nature and T 1 ∼ 28 psec. In the pulsed mode burning, peculiar feature of dispersive lineshape of the hole was observed from the initial stage of irradiation. It is described at the moment as a result of the excitation of the two-exciton band which is inherent to the excitonic state with large coherence length.