Multiscale molecular simulations of the morphological evolution of small-molecule organic solar cells during the vacuum codeposition process

The mesoscale morphologies of organic small molecular films fabricated via vacuum deposition processes are critical to the performance of small-molecule solar cells and organic light-emitting diodes. In the present study, the morphological evolution of the active layer of DPDCPB:${\mathrm{C}}_{70}$ small-molecule solar cells during vacuum codeposition processes was revealed by a series of GPU-accelerated coarse-grained molecular-dynamics simulations. The ${\mathrm{C}}_{70}$ and DPDCPB molecules were coarsened into ellipsoids and bonded ellipsoids, respectively. The interactions between ellipsoids were described by the Gay-Berne formulation and were parametrized to reproduce potential energy surfaces from all-atom atomistic simulations using a genetic algorithm. Due to the significantly reduced overall degrees of freedom, this coarse-grained scheme allowed us to simulate the vacuum codeposition processes and monitor the morphological evolution of systems with system length scales compatible with those of the experiments (\ensuremath{\sim}30 nm). Our simulations indicate that the film morphologies are closely correlated with the DPDCPB:${\mathrm{C}}_{70}$ blending ratio. High ${\mathrm{C}}_{70}$ concentration leads to a rough film surface, which is in accordance with experimental observations and can be attributed to the strong self-aggregation behavior of ${\mathrm{C}}_{70}$ molecules. The morphological property analysis indicates that the rough film surface has an almost negligible impact on the DPDCPB/${\mathrm{C}}_{70}$ domain percolations, and the device with the optimal deposition ratio should give the most balanced hole/electron transfer in respective DPDCPB/${\mathrm{C}}_{70}$ domains. The present study demonstrates that by using the ellipsoid-based coarse-grained model, it is possible to study the morphological evolution of small-molecule organic thin film during vacuum deposition processes with molecular scale details, which can provide valuable insights for experimental teams to further optimize device fabrication protocols for the next generation of organic optoelectronic devices.