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The “Carbonaceous Aerosol in Rome and Environs” (CARE) experiment took place at a Mediterranean urban background site in Rome (Italy) deploying a variety of instrumentation to assess aerosol physical-chemical and optical properties with high-time resolution (from 1 min to 2 h). In this study, aerosol optical properties, chemical composition, and size distribution data were examined with a focus on the analysis of several intensive optical properties obtained from multi-wavelength measurements of aerosol scattering and absorption coefficients. The spectral behaviour of several quantities related to both aerosol composition and size was explored, analysing their high-time resolved temporal patterns and combining them in order to extract the maximum information from all the available data. A methodology to separate aerosol types using optical data only is here proposed and applied to an urban area characterised by a complex mixture of particles. A key is given to correctly disentangle cases that could not be distinguished observing only one or few parameters, but that can be clearly separated using a suitable ensemble of optical properties. The SSCAAE, i.e. the wavelength dependence of the Single Scattering co-albedo 1-SSA (where SSA is the Single Scattering Albedo) - that efficiently responds to both aerosol size and chemical composition – resulted to be the best optical intensive parameter to look at for the discrimination between episodes characterised by specific aerosol types (e.g. sea salt, Saharan dust) and more mixed conditions dominated by local emissions. However, this study also highlighted that it is necessary to combine temporal patterns of different optical parameters to robustly associate SSCAAE features to specific aerosol types. In addition, the complete chemical speciation and the high-time resolved size distribution were used to confirm the aerosol types identified via a combination of aerosol optical properties. Look-up tables with most suitable ranges of values for optical variables were produced; therefore, these pieces of information can be used at the same site or at locations with similar features to quickly identify the occurrence of aerosol episodes. Graphical frameworks (both from the literature and newly designed) are also proposed; for each scheme features, advantages, and limitations are discussed.