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The formation of thin films of molecular systems on substrates where the thickness of the material goes beyond the initial influence of the interface between adsorbate and adsorbent will be presented. This growth of material means that the supramolecular interactions between the component molecules can vary in their importance during the process, in a process that is out of equilibrium, leading to a dependence of film quality on the substrates that are used. Deposition of relatively light material from the gas phase leads to clean and high quality films. The multilayers can be probed in situ with a variety of techniques so that the way in which the final structure is reached can be understood. Diffraction techniques become a viable method for probing growth and structure. In addition, it is possible to construct multilayers of different material with ease. Particular attention is given here to this “heteroepitaxy”. Deposition from solution can lead to high quality films and is especially suited for large area production of films of materials that might be sensitive to evaporation. In all cases, the wetting of substrate by the adsorbate and the importance of non-covalent interactions in the organisation of the molecules will be discussed for specific cases. The preparation of layers of materials that can present some property is an important pursuit with regard to the applications of the systems, and the influence of the growth method on the performance of materials will be shown.

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