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The structural characterization of microgels at interfaces is fundamental tounderstand both their 2D phase behavior and their role as stabilizers thatenable emulsions to be broken on demand. However, this characterization isusually limited by available experimental techniques, which do not allow adirect investigation at interfaces. To overcome this difficulty, here we employneutron reflectometry, which allows us to probe the structure andresponsiveness of the microgels in-situ at the air-water interface. Weinvestigate two types of microgels with different cross-link density, thushaving different softness and deformability, both below and above their volumephase transition temperature, combining experiments with computer simulationsof realistic in silico synthesized microgels. We find that temperature onlyaffects the portion of microgels in water, while the strongest effect of themicrogels softness is observed in their ability to protrude into the air. Inparticular, standard microgels have an apparent contact angle of few degrees,while ultra-low cross-linked microgels form a flat polymeric layer with zerocontact angle. Altogether, this study provides an in-depth microscopicdescription of how different microgel architectures affect their arrangementsat interfaces, and will be the foundation for a better understanding of theirphase behavior and assembly. This manuscript has been accepted for publicationin Nature Communications (open access). The final version of the manuscriptincluding the Supplementary Information will be available in the future.

In-situ study of the impact of temperature and architecture on the interfacial structure of microgels