Mechanism of stimulated Mie scattering: Light-induced redistribution of self-assembled nanospheres of two-photon absorbing chromophore

We report the observation of backward stimulated Mie scattering (SMS) due to light-field induced spatial redistribution of self-assembled nanospheres of a two-photon resonant organic chromophore in water, pumped by ∼10-ns laser pulses of ∼816-nm wavelength. The pump-energy threshold for generating backward stimulated scattering in such a system is remarkably lower than that in pure water. The gain of backscattering originates from an induced Bragg grating that reflects partial energy from the pump beam into the backward Mie scattering beam. Based on the experimental fact that the time-delay of the SMS pulse onset depends on both the pump level and the viscosity of the solvent, a physical model of SMS generation is proposed. Our experimental results have shown that the major contribution to the formation of an induced Bragg grating is spatial redistribution of nanoparticles suspended in the liquid. These nanoparticles are driven by a force that is proportional to the intensity gradient of the standing-wave field resulting from interference between the forward pump beam and the backward Mie scattering beam. When the nanoparticle motion is frozen in a gel-like medium, no SMS is observed, which experimentally supports the validity of the proposed physical model.