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During transport by advection, atmospheric non-spherical particles, such as volcanic ash, desert dust or sea-salt particles experience several chemical and physical processes, leading to a complex vertical atmospheric layering at remote sites where intrusion episodes occur. In this paper, a new methodology is proposed to analyse this complex vertical layering in the case of a two/three-component particle external mixtures. This methodology relies on an analysis of the spectral and polarization properties of the light backscattered by atmospheric particles. It is based on combining a sensitive and accurate UV-VIS polarization lidar experiment with T-matrix numerical simulations and air mass back trajectories. The Lyon UV-VIS polarization lidar is used to efficiently partition the particle mixture into its nonspherical components, while the T-matrix method is used for simulating the backscattering and depolarization properties of nonspherical volcanic ash, desert dust and sea-salt particles. It is shown that the particle mixtures’ depolarization ratio delta(p) differs from the nonspherical particles’ depolarization ratio delta(ns) due to the presence of spherical particles in the mixture. Hence, after identifying a tracer for nonspherical particles, particle backscattering coefficients specific to each nonspherical component can be retrieved in a two-component external mixture. For three-component mixtures, the spectral properties of light must in addition be exploited by using a dual-wavelength polarization lidar. Hence, for the first time, in a three-component external mixture, the nonsphericity of each particle is taken into account in a so-called 2 beta + 2 delta formalism. Applications of this new methodology are then demonstrated in two case studies carried out in Lyon, France, related to the mixing of Eyjafjallajokull volcanic ash with sulfate particles (case of a two-component mixture) and to the mixing of dust with sea-salt and water-soluble particles (case of a three-component mixture). This new methodology, which is able to provide separate vertical profiles of backscattering coefficient for mixed atmospheric dust, sea-salt and water-soluble particles, may be useful for accurate radiative forcing assessments.