We probe the energetic landscape at a model pentacene/fullerene (C60) interface to investigate the interactions between positive and negative charges, which are critical to the processes of charge separation and recombination in organic solar cells. Using a polarizable force field, we find that polarization energy, i.e., the stabilization a charge feels due to its environment, is larger at the interface than in the bulk for both a positive and a negative charge. The combination of the charge being more stabilized at the interface and the Coulomb attraction between the charges results in a barrier to charge separation at the pentacene/C60 interface that can be in excess of 0.7 eV for static configurations of the donor and acceptor locations. However, the impact of molecular motions, i.e., the dynamics, at the interface at room temperature results in a distribution of polarization energies and in charge separation barriers that can be significantly reduced. The dynamic nature of the interface is thus critical, with the polarization energy distributions indicating that sites along the interface shift in time between favorable and unfavorable configurations for charge separation.
|Number of pages||11|
|Journal||ACS Applied Materials and Interfaces|
|State||Published - Jun 22 2016|
Bibliographical noteFunding Information:
This work has been supported by King Abdullah University of Science and Technology (KAUST), the KAUST Competitive Research Grant program, and the Office of Naval Research Global (Award N62909-15-1-2003). We acknowledge the IT Research Computing Team and Supercomputing Laboratory at KAUST for providing computational and storage resources. This work has also used the computing resources of the Garnet, Spirit, and Copper supercomputing systems through the DoD HPCMP. C.R. thanks the University of Kentucky Vice President of Research for start-up funds. We wish to thank Mahesh Kumar Ravva and Naga Rajesh Tummala for stimulating discussions and assistance with technical elements of the molecular dynamics simulations.
© 2016 American Chemical Society.
- charge separation and recombination
- energetic disorder
- molecular dynamics
- multiscale modeling
- organic photovoltaics
- organic-organic interfaces
ASJC Scopus subject areas
- Materials Science (all)