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Vanadium pentoxide (V 2 O 5) films were deposited on sapphire substrates by radio frequency (R.F.) magnetron sputtering at 450 °C and annealed in various ambient atmospheres. The influence of ambient atmospheres on the structure, optical properties, and morphology of the thin films after annealing were characterized, and the transition behaviors in the annealing process were investigated by DSC, temperature-dependent Raman and FTIR. The results demonstrated that V 2 O 5 films underwent four different transition behaviors during post-deposition annealing due to the different oxygen proportion of ambient. Different products (VO 2 (B), VO 2 (R)) in the transition process were the main reason for the evolution of optical properties. No transition behaviors occurred because of the oxygen-rich ambient when annealed in air, and no significant change in infrared transmittance was observed. When annealed in 0.1% O 2 /Ar, the film was converted to VO 2 (B) with the decrease of infrared transmittance. In the case of 0.01% O 2 /Ar, metastable VO 2 (B) and VO 2 (R) were observed as intermediate crystalline phases before V 2 O 5 finally transformed to VO 2 (M), and the changes in the three stages of two drops and one rise were shown in infrared transmittance. While annealed in pure argon ambient, V 2 O 5 was turned into VO 2 (R) and VO 2 (M) without VO 2 (B) phase production, accompanied by a single change of infrared transmittance reduction and recovery. This provides a more detailed vanadium oxide thermal transition process and shows data reference for the preparation technology and application of vanadium oxide materials. • V 2 O 5 films were deposited on sapphire substrates by radio frequency (R.F.) magnetron sputtering; • Effect of the different oxygen proportion during annealing on thermal transition behaviors was investigated in detail by temperature-dependent Raman and FTIR; • The annealed V 2 O 5 films were transformed into V 2 O 5 , VO 2 (B), and VO 2 (M) by different thermal transition behaviors; • VO 2 (M) films with excellent thermochromic properties can be obtained by controlling the annealing atmosphere and temperature. [ABSTRACT FROM AUTHOR]