Glass structures of multicomponent oxide systems (CaO-Al2O3-SiO2) are studied using a simulated pulsed laser with molecular dynamics. The short- and intermediate-range order structures revealed a direct correlation between the transformation of Al(IV) to Al(V), regions of increased density following laser processing, inherent reduction in the average T-O-T (T = Al, Si) angle, and associated elongation of the T-O bonding distance. Variable laser pulse energies were simulated across calcium aluminosilicate glasses with high silica content (50-80%) to identify densification trends attributed to composition and laser energy. High-intensity pulsed laser effects on fictive temperature and shockwave promotion are discussed in detail for their role in glass densification. Laser-induced structural changes are found to be highly dependent on pulse energy and glass chemistry.