Tailoring the electronic properties of graphene-based 2D materials via heterostructures engineering

Since the discovery of graphene in 2004, both theoretical and experimental research on 2D materials has experienced exponential growth that continues to this day. The exceptional electronic, thermal, and mechanical properties, as well as a plethora of exotic physical phenomena that can originate from them, are the main reasons for the great interest that low-dimensional systems have garnered from the beginning. One of the main advantages of 2D materials is the ability to stack them more or less arbitrarily to form heterostructures in which the planes are linked by weak Van der Waals interactions. In this way, innovative heterostructures can be created, without a bulk counterpart, with different properties compared to the individual layers that compose them. Thanks to their versatility, it is possible to create new materials with on-demand properties based on the required application. In this sense, it is of fundamental importance to have theoretical tools to design these systems, being able to calculate with appropriate precision their stability, formation thermodynamics, and electronic properties, and many other aspects. In this doctoral thesis, various Van der Waals heterostructures have been studied using ab-initio methods, with the aim of understanding how to finely modify their electronic properties by altering their geometry and composition. This research focuses on both the study of graphene/hBN heterostructures and the thermodynamics of formation of non graphene-based 2D systems, such as plumbene and pnictogens.