Non-volatile phase-change materials with large optical contrast are essential for future tunable nanophotonic applications. Antimony trisulfide (Sb2S3) has recently gained popularity in this field due to its low absorption in the visible spectral region. Although several Sb2S3 deposition techniques have been reported in the literature, none of them was optimized with respect to stoichiometry, lowest possible absorption, and large refractive index contrast (Δn) upon the phase change. Here we present a comprehensive multi-parameter optimization of pulsed laser deposition of Sb2S3 towards this end. We correlate the specific deposition with the resulting compositional and optical properties and report parameters leading to films with extraordinary qualities (Δn = 1.2 at 633 nm). Additionally, we suggest crystal orientations and vibrational modes associated with the largest change in the refractive index and propose them as useful large-scale indicators of the Sb2S3 switching contrast.