The dynamics and reversibility of Ag nanoparticle photodissolution into As2S3 chalcogenide thin films have uniquely been directly measured by continuous AFM imaging during patterned optical illumination. The surface morphology, roughness and particle size distribution have thus been spatially and statistically monitored as a function of time, both during and following optical exposure. Photodissolution was observed to proceed via two mechanisms. In one case, nanoparticles abruptly and nearly completely disappeared along a sharp dissolution front traveling laterally at ∼0.19 μm s(-1). Following illumination, similarly sized nanoparticles uniformly reformed on the surface. A more inhomogeneous photodissolution process was separately recorded, clearing irregular ∼1-2 μm patches that grew with time until most of the surface was free of nanoparticles. Post-illumination, surface nanoparticle development and coverage were similarly inhomogeneous, with larger but 50% fewer particles in the final distribution. In every experiment, an initial roughening was detected before the nanoparticle surface coverage visually diminished, indicating the onset of photodissolution at widely distributed energetically and kinetically favored sites which temporarily enhances nanoscale roughness. Such direct studies of surface dynamics are crucial to understanding and ultimately optimizing chalcogenide film applications such as photomasks, optoelectronics media and bio-chemical sensors.