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Size-segregated aerosol vertical profiles in the troposphere are critically important for source attribution, transformation processes, atmospheric stability, and radiative forcing. For the first time, the development of a 6-stage impactor for real-time balloon-borne measurements of size-segregated (cutoff diameter [Dae]: 0.15-5 µm) aerosol mass concentrations in the free troposphere was tested during spring 2016 over Hyderabad, India, is presented. Total aerosol mass concentrations obtained with the 6-stage impactor (MTI) and a co-located optical particle counter (MTOPC) measurements at the surface under ambient conditions agreed to within 15%. The effect of aerosol particle growth on the MTI data are assessed using an urban aerosol particle model by scaling mass concentration of water-soluble (hydrophilic) aerosol particles at ambient relative humidity (RH) to that at RH = 50%. An overall uncertainty of the measurement of the MTI was estimated to be about 19%. The altitude variation of size-segregated mass concentrations of aerosol particles along with thermodynamic variables depicted convectively well-mixed layer extending up to about 4.5 km within which aerosol particles showed two distinct layers, one at ∼2 km and another at about 4.5 km. The size-resolved air samples containing aerosol particles collected using the balloon-borne 6-stage impactor will be useful for their chemical characterization and also long-range transport studies. Copyright © 2019 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]