F.G. would like to thank the Generalitat Valenciana for the "Santiago Grisolía" Scholarship (GRISOLIA/2014/018) for funding the Ph.D. position that has permitted carry out the research. F.G. would like to thank the Gonel-Balaguer Hermanos Foundation from the Universitat Jaume I and the COST Action MP 1202: Rational design of hybrid organic-inorganic interfaces (HINT) for the economical contributions as a scholarship and stipend, towards the short stay at the Université Pierre et Marie Curie in Paris that has permitted to promote high impact research partnerships between the Instituto de nanomaterials Avanzados (INAM-UJI), Química Inorgánica y Órganica department and UJI as institution and the former. F.G. would like to thank the COST Action MP 1202: Rational design of hybrid organic-inorganic interfaces (HINT) for financing in form of scholarship the COST school "Bottom-up approaches of hybrid materials: preparation and design", held at the Jozef Stefan Institute, in Ljubljana, Slovenia, 26-28/05/2015. "The principles of physics, as far as I can see, do not speak against the possibility of maneuvering things atom by atom. It is not an attempt to violate any laws; it is something, in principle, that can be done, but in practice it has not been done because we are too big." Richard P. Feynman (1959) A me stesso, per la forza che ho avuto a rialzarmi A mia moglie Ana Cecilia, che ha avuto la forza di aspettarmi Alla mia famiglia, che non ha mai smesso di aiutarmi This work (2014-2018) is dedicated to my family, which moral and sometimes financial support has been of great help in difficult moments, to my wife Ana that had the patience to wait for this day to happen and to me, who, after a long time of sacrifices and depression, finally realize this dream. It is also dedicated to all the people who encouraged me not to give up, starting from my thesis director, Beatriz Julián-López. This work, outcome of a three years journey in a wonderful part of Spain, has been carried out by me. However, as always, it could not be done without the help of people both in the private and in the working life that helped me growing both as a man and as a professional. Therefore, here there is a list of persons that I want to thank. First of all I want to thankequallymy family, dad (Salvatore), mum (Vincenza), brother (Giorgio), my wife (Ana Cecilia), and my thesis director, Beatriz Julián-López to have given me this opportunity and to have believed in me when no one would have bet a penny in my favor. Furthermore I want to thank my advisor to have helped me in understanding the academic world far better than I previously did and to have been present both in my academic and private life as a friend. Secondly I want to thank the Generalitat Valenciana, from which I have benefitted economically these three years through a Grisolía doctoral scholarship. I want to thank the personnel at the Servicio Central de Instrumentación Científica whose friendship and technical knowledge has helped me in achieving the amazing results presented...