To utilize the excellent properties of silica (SiO2) glass for a glass laser host, neodymium‐aluminum (Nd–Al) and neodymium‐phosphorous (Nd–P) co‐doped SiO2 glasses were studied. They were prepared by plasma‐torch chemical vapor deposition (CVD). It was found that a doping level less than ten times the number of Nd for the Al co‐dopant and less than about fifteen times for the P co‐dopant was enough to remove undesirable fluorescence properties of Nd‐doped SiO2 glasses and make them suitable for laser application. The clustering Nd ions disperse well in a glass matrix and lasing fluorescence increases. The effects of the Al dopant on the density and Raman spectra were also studied to obtain structural information. On the basis of glass science and solution chemistry, the marked effects of both dopants were explained by the following model. Nd ions can be well incorporated into a SiO2 glass network through co‐dopant oxide forming a solvation shell around the Nd ions. This model leads to an expansible method for coordination control around active ions in SiO2 glass. A preliminary experiment on laser oscillation using Nd–Al co‐doped SiO2 glass was also carried out.

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