We have used in situ micro-Raman spectroscopy to clarify the mechanism of the luminescence efficiency improvement of GaAsN alloys by laser irradiation. Raman peak intensity of GaAs-like longitudinal optical (LO) mode phonon was observed to increase with the laser irradiation time. With increasing laser power density, the Raman intensity of GaAs-like LO mode phonon was found to increase more rapidly and to be saturated in a shorter time. Changes in the Raman intensity can be expressed by the same equation used for the luminescence efficiency improvement. Time constants of changes in the Raman intensity were almost in agreement with those of the luminescence efficiency improvement. This indicates that the increase in Raman intensity of GaAs-like LO phonon is closely related to the luminescence efficiency improvement. (c) 2006 Published by Elsevier B.V.