Abstract
Urban aerosol-haze over fast-growing Asian mega-cities pose health and aviation-related problems requiring a combination of large-scale multidisciplinary field experiments as well as numerical modelling to address them holistically. Although a repository of rain and cloud microphysical data is available over the Asian sub-continent, data related to haze microphysics remain scanty. Heterogeneously processed sulphate increases the solubility of existing aerosol mixtures through non-ideal interactions over micron as well as sub-micron regimes. The methodology followed in this paper combines in-situ aircraft-based microphysical observations followed by heterogeneous cloud processing procedures. It is shown for the first time that the extent of processed sulphate accretion is comparable to the original aerosol sulphate contents to the extent that some hydrophobic black carbon particles are rendered hydrophilic after cloud processing. It is also shown that haze-mediated cloud droplets are acidic with a solution pH range of 0.5–4.0 and that solution non-ideal behaviour over the smallest haze droplets is around 29%. Modelled spectra match up with the observed spectra after two cycles of cloud processing only when the effects of a variable composition of a multi-modal spectrum growing in concentrated ionic solutions are accounted for. Importantly, the study shows that although 35.6% of the aerosols are activated, 78.6% of the smallest particles (Mode I—modal radius 0.03 μm) fall within a restricted Köhler growth regime. The results from this study are also likely to impact new research through better model parameterisations and linking haze processes into large-scale atmospheric models.
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All data generated or analysed during this study are included in this published article (and its supplementary information files).
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Acknowledgements
The CAIPEEX project and IITM are fully funded by the Ministry of Earth Sciences, Government of India. The authors would like to express their gratitude to Prof. Ravi Nanjundiah, Director of IITM, Pune for his support. The Dean, School of Mechanical Engineering (SMEC), VIT Vellore is sincerely thanked for support and encouragement. The authors would like to acknowledge High Speed Computing facilities under the ERASMUS+ Capacity Building Scheme for Higher Education. Thanks are also due to the Centre for Technical Support (CTS), VIT, Vellore. Prof. Satyajit Ghosh is grateful to the School of Earth and Environment, University of Leeds, U.K. for providing a Visiting Professorship during the tenure of this work. S.G. and S.G. are grateful to the IITM, Pune for providing accommodation, subsistance, and access to IITM data and facilities.
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SG and SG planned and executed all the simulations and related modelled results with observations. TP and SB are involved in CAIPEEX mission and contributed to microphysical data interpretation. SG and TP conceived this investigation. All authors reviewed the manuscript.
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Gumber, S., Ghosh, S., Bera, S. et al. On the importance of non-ideal sulphate processing of multi-component aerosol haze over urban areas. Meteorol Atmos Phys 134, 37 (2022). https://doi.org/10.1007/s00703-022-00877-7
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DOI: https://doi.org/10.1007/s00703-022-00877-7