Abstract We discuss different methods to grow organic single crystalline thin films from solution. Specifically, we address exploratory developments and apply them on the highly nonlinear material DAST (4′-dimethylamino-N-methyl-4-stilbazolium tosylate) in a DAST/methanol system. We describe the nucleation and growth thermodynamics in solution using a solubility diagram and its Ostwald–Meiers metastable region. The important experimental parameters for bidimensional growth are discussed and first promising results are presented. To cite this article: S. Manetta et al., C. R. Physique 3 (2002) 449–462.