Thermodynamics of nanosecond nanobubble formation at laser-excited metal nanoparticles

The nonlinear thermal behavior of laser-heated gold nanoparticles in aqueous suspension is determined by time-resolved optical spectroscopy and x-ray scattering. The nanoparticles can be excited transiently to high lattice temperatures owing to their large absorption cross-section and slow heat dissipation to the surrounding. A consequence is the observation of lattice expansion, changed optical transmission, vapor bubble formation or particle melting. The heat transfer equations are solved for two limiting cases of heat pulses shorter and longer than the characteristic cooling time. The results of pulsed excitation with femtosecond and nanosecond lasers are explained by the theoretical prediction, and the bubble formation is interpreted by a spinodal decomposition at the particle-liquid interface. It is shown that both the laser spectroscopy and x-ray scattering results agree qualitatively and quantitatively, underlining the validity of the comprehensive model.