Incorporation of novel materials, such as molecular layers or 2D layers, into electronic paradigms enables transformative potential in applications ranging from memory, batteries, catalysts, flexible devices, alternate computing paradigms, and quantum phenomena. In order to take advantage of the promising properties of these heterogeneous systems, holistic study of the fundamental constituents as well as their impact on the final device properties are important. As interfaces continue to dominate performance, the ability to adjust the interface for desired properties become more and more critical.  Molecular layers offer a versatile means of tuning interfacial electronic, chemical, physical, and magnetic properties. We are advancing surface characterization by using vibrational spectroscopy, photoelectron spectroscopy, contact angle, and eGaIn electrical measurements to address technology barriers which will enable successful development and subsequent manufacture of next-generation technologies.