The use of SF6 release to excite the airglow from atomic oxygen in the ionosphere is demonstrated by experiment and by theory. Enhanced 777.4-nm emissions from O(5P) states were measured during the AFGL-sponsored Ionospheric Modification Studies campaign at Wallops Island, Virginia. For this rocket campaign, 8¿1025 molecules of SF6 were released at 350-km altitude into the midnight ionosphere on November 9, 1983. The 777.4-nm airglow increased by over 150 R. The temporal evolution of the airglow is simulated using an ion chemistry model involving six positive and negative ion species and 16 reactions. The model indicates that substantial enhancements in 844.6 nm and 135.6 nm will be triggered by SF6 injections into the ionosphere. The model also demonstrates that the intensity of the 777.4-nm line is strongly dependent of the temperature on the neutral atmosphere.