The manuscript provides a comprehensive review of the physico-chemical processes at the ocean-atmosphere interface. These processes are more important as they have an impact on atmospheric chemistry. The authors focus their article on sea surface microlayers and their impact on aerosol production. This review is particularly interesting and gives a state of the art of current research in this field. I suggest only a few minor changes before publication in ACP.

1) The authors mention some papers in which the photochemical impact was studied under not-relevant wavelength conditions. For example, in line 219... the paper cited used experiments under UVC radiation which is far from the solar irradiation spectrum.

2) Another article (line 231...) reports the effect of ozone photolysis at 254 nm and its effect on the deliquescence of sea salt particles.

if publishers wish to cite these articles, it should be specified that the results were obtained at wavelengths below the solar spectrum.

Wang and Gligorovski report the review paper on the physical and chemical properties of the atmospheric-ocean interfaces or specifically the multiphase and heterogeneous processes of the sea surface microlayer. The text is generally written well and hence, is publishable after addressing the following minor issues.

This text briefly mentions the deposition of gaseous species on the ocean surface. I am wondering if there are any effects of SML on the aerosol deposition onto the ocean surface, particularly for iron-containing aerosols. It would be great if the authors provided the current understanding.

For the section 5.1, can the authors provide a more general view about the photosensitized processes? The authors discussed several reaction systems individually, but there is a similarity in terms of processes involving the triplets.

Lines 891: The discussion about the ionic strength effect is quite limited in the present text, although the authors present the corresponding figure (Fig.4). The authors need to elaborate. What is the direct and indirect role of ionic strength?

Minor comments

Please define “CLAW“