Nonlinear bleaching, absorption, and scattering of 532-nm-irradiated plasmonic nanoparticles

Abstract

Single-pulse irradiation of Au and Ag suspensions of nanospheres and nanodisks with 532-nm 4-ns pulses has identified complex optical nonlinearities while minimizing material damage. For all materials tested, we observe competition between saturable absorption (SA) and reverse SA (RSA), with RSA behavior dominating for intensities above ∼50 MW/cm2. Due to reduced laser damage in single-pulse experiments, the observed intrinsic nonlinear absorption coefficients are the highest reported to date for Au nanoparticles. We find size dependence to the nonlinear absorption enhancement for Au nanoparticles, peaking in magnitude for 80-nm nanospheres and falling off at larger sizes. The nonlinear absorption coefficients for Au and Ag spheres are comparable in magnitude. On the other hand, the nonlinear absorption for Ag disks, when corrected for volume fraction, is several times higher. These trends in nonlinear absorption are correlated to local electric field enhancement through quasi-static mean-field theory. Through variable size aperture measurements, we also separate nonlinear scattering from nonlinear absorption. For all materials tested, we find that nonlinear scattering is highly directional and that its magnitude is comparable to that of nonlinear absorption. These results indicate methods to improve the efficacy of plasmonic nanoparticles as optical limiters in pulsed laser systems.