AbstractUltra-fast pulsed laser deposition using high-repetition-rate short-pulse lasers has been shown to provide high optical quality, super smooth thin films free of scattering centres. The optimized process conditions require short ps or sub-ps pulses with repetition rate in the range 1-100 MHz, depending on the target material. Ultra-fast pulsed laser deposition was used to successfully deposit atomically-smooth, 5micron thick As2S3 films. The as-deposited films were photosensitive at wavelengths close to the band edge (≈520 nm) and waveguides could be directly patterned into them by photo-darkening using an Argon ion or frequency doubled Nd:YAG laser. The linear and nonlinear optical properties of the films were measured as well as the photosensitivity of the material. The optical losses in photo-darkened waveguides were <0.2 dB/cm at wavelengths beyond 1200nm and <0.1 dB/cm in as-deposited films. The third order nonlinearity, n2,As2S3, was measured using both four-wave mixing and the z-scan technique and varied with wavelength from 100 to 200 times fused silica (n2,Silica ≈3×10-16 cm2/W) between 1500nm and 1100nm with low nonlinear absorption.Encouraged by the Ultrafast laser deposition results, we have built a new specialized modelocked picosecond laser system for deposition of optical films and for laser formation of nanoclusters. The newly developed “state of the art” powerful Nd:YVO laser can operate over a wide range of wavelengths, intensities, and repetition rates in MHz range. A brief description of the 50W laser installation is presented.