The primary goal of ExIStENcE is the development of novel evolutionary algorithms (EAs) and protocols, based on deeper principles than currently available, for the optimisation, design and exploitation of molecular self-assembly. Evolutionary algorithms are nowadays well established techniques that have shown their worth on a large variety of applications that range from timetabling and scheduling problems to robotics and space antenna design. Surprisingly, EAs have not yet been systematically analised in the context of molecular tile design. At the core of our approach lies the assumption that self-assembly can be understood as an information-driven process and hence be better exploited by directly linking it to computational phenomena. Taken as an operational hypothesis, which our research programme will analyse both theoretically and experimentally, this assumption implies that with suitable tools, desired emergent phenomena could in principle be programmed into self-assembling nanosystems. Our experimental target is based around molecular tiles as these have been shown to be computationally complete. Hence, they can potentially be programmed to perform any set of discrete information processing steps which in turn could induce a specific emergent pattern of complex behaviour.