The development of next generation spintronic devices, sensors, and neuromorphic computing devices requires the development of materials with new functional properties not found in conventional bulk materials. A novel route involves harnessing the unexpected physical phenomena that result from the changes in structure and chemistry which occur over nanometer scales at surfaces and interfaces. The approach of this work utilizes laser-assisted growth to control interfacial properties with atomic layer precision in combination with state-of-the-art techniques for characterizing the structural, chemical, magnetic, and electrical properties. In this way, a full understanding of the origins of new magnetic and electronic properties derived from interfacial mechanisms can be determined.