The structural and optical properties of AsSe chalcogenide glass, starting with As40Se60, were studied as a function of Ge or Se additions. These elements provide broad glass forming options when combined with the host matrix to allow for compositional tuning of properties. Optimization of glass composition has been shown to produce bulk glasses with a thermoptic coefficient (dn/dT) equal to zero, as well as a composition which could demonstrate a net zero change in index after precision glass molding (PGM). The bulk glass density, coefficient of thermal expansion (CTE), refractive index, and dn/dT were measured for all bulk compositions, as was the refractive index after PGM. For the bulk glasses examined, both the refractive index (measured at discrete laser wavelengths from 3.4 to10.6 μm) and dn/dT were observed to decrease as the molecular percentage of either Ge or Se is increased. Compared to the starting glass’ network, additions of either Ge or Se lead to a deviation from the “optimally constrained” binary glass’ average coordination number <r> = 2.4. Additions of Se or Ge serve to decrease or increase the average coordination number (CN) of the glass, respectively, while also changing the network’s polarizability. After a representative PGM process, glasses exhibited an “index drop” consistent with that seen for oxide glasses.1 Based on our evaluation, both the Gecontaining and Ge-free tielines show potential for developing unique compositions with either a zero dn/dT for the unmolded, bulk glass, as well as the potential for a glass that demonstrates a net zero “index drop” after molding. Such correlation of glass chemistry, network, physical and optical properties will enable the tailoring of novel compositions suitable for prototyping towards targeted molding behavior and final properties.