Solute migration caused by excited state absorptions.

Using the Z-scan technique, we find that migration of chloroaluminum phthalocyanine in liquid ethanol can be induced by the absorption of a 19 ps laser pulse with energy exceeding a threshold but not by that of a 2.8 ns pulse depositing more energy at the solute molecules. Considering each solute molecule as an oscillator confined within a potential well, we explain, in accordance with the five-energy-band model, that solute molecules excited by a 19 ps pulse retain more translational excess energy to overcome the potential well barrier compared with those excited by a 2.8 ns pulse of equal energy. Therefore, they are more likely to migrate out of the laser beam center, weakening the solution's absorption that we detect in the Z-scan measurements. Furthermore, we theoretically infer that the 19 ps pulse-induced solute migration tends to be nonquasistatic and experimentally verify that it cannot be attributed to the Soret effect, a quasistatic process.

Mass transport following impulsive optical excitation.

Transition from reverse-saturable absorption to saturable absorption of the chloroaluminum phthalocyanine solution excited by a giant laser pulse is ascribed not just to the saturation of excited state absorption, but also to the outward migration of the solute molecules at the laser beam center. While the saturation of excited state absorption occurs within a single picosecond laser pulse, the beam center population decrease is sustained much longer than the pulse duration. We distinguish these two mechanisms with the Z-scan technique, utilizing picosecond pulses with pulse-to-pulse separations ranging from 0.1 to 5.0 s.