The phenomenological Landau-Teller vibrational relaxation model, used in CFD, and the Larsen-Borgnakke model, used in DSMC, are compared to newly available ab-initio calculations of O2 + O collisions in 0D and 1D test cases. Chemical reactions are not included in our analysis. As long as the vibrational relaxation parameter is properly calibrated, the Landau-Teller model accurately reproduces ab-initio calculations. The vibrational energy during the vibrational relaxation appears bimodal and it does not follow the Boltzmann distribution. Therefore, a bimodal model is proposed in this work that can calculate vibrational distribution functions based on local translational temperature, local vibrational energy and the free stream vibrational energy. The Larsen-Borgnakke model also accurately reproduces the ab-initio calculations, but only when the Gimelshein correction is applied to the relaxation number calibration. In addition, this work discusses a consistent implementation of ab-initio vibrational relaxation models to the DSMC algorithm.