An influential factor for the microstructure of semiconductor polymer films is the solvent chosen for their processing and subsequent performance as an active layer in electronic and optical devices. In this paper, we address the solvent-polymer interplays by reporting a comparison between the microstructure of the bulk of poly(3-hexylthiophene) (P3HT) films formed from two different simulation methodologies: using the o-dichlorobenzene (ODCB) as an aggregation chain parameter and a solvent-free protocol. In comparison to the length of an ideal planar chain, the solvent caused an average reduction of 12% of oligomer chains. Whereas, in the other film, the reduction was around 30%. Furthermore, the solvent allowed pathways of π-interactions due to the cohesional-like distribution of the chains, indicating that the solvent also induces chain orientation affecting its microstructure.
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