Advances on analytical strategies for targeted and untargeted profiling of organic aerosols: Lessons learned and future challenges

•Advanced multimethod and multidimensional analytical strategies for profiling OAs.•Major challenges in targeted/untargeted analysis of OAs in outdoor and indoor air.•Need for rapid molecular-level measures, methods optimization & analytical expertise.•Findings will assist in better understanding OAs dynamics in outdoor and indoor air. Atmospheric organic aerosols (OAs) are among the most complex environmental matrices known. Given OAs have well documented atmospheric and health effects, it is crucial to understand the complexity and composition of this organic matrix. On the quest to unravel this information, advanced analytical approaches have been developed for the characterization of OAs complexity. This Perspective revisits the most important state-of-the-art multidimensional analytical strategies, namely those that use a second or third dimension in spectroscopic, spectrometric, and chromatographic methods, for the targeted and untargeted profiling of the complex OAs from both outdoor and indoor environments. This insight also comments on the major challenges ahead concerning OAs analysis, including processing and extraction of chemical information from the voluminous amount of data generated from those multidimensional analytical approaches. [Display omitted]