This dataset contains raw and processed data corresponding to all the atomic force microscopy (AFM), scanning electron microscopy (SEM), polarization-modulation infrared reflection absorption spectroscopy (PM-IRRAS), angle-resolved, and temperature-dependent X-ray photoelectron spectroscopy (XPS) measurements. Data from collaborating groups can be found in a separate dataset. The numbering of the individual files follows the sequence of figures in the publication (and supporting information). The following data types are included: .xlsx, .dpt, .jpg, and .tif.