No abstract

Polymer-based photovoltaic devices have the potential for widespread usage due to their low cost per watt and mechanical flexibility. Efficiencies close to 9.0% have been achieved recently in conjugated polymer based organic solar cells (OSCs). These devices were fabricated using solvent-based processing of electron-donating and electron-accepting materials into the so-called bulk heterojunction (BHJ) architecture. Experimental evidence suggests that a key property determining the power-conversion efficiency of such devices is the final morphological distribution of the donor and acceptor constituents. In order to understand the role of morphology on device performance, we develop a scalable computational framework that efficiently interrogates OSCs to investigate relationships between the morphology at the nano-scale with the device performance. In this work, we extend the Buxton and Clarke model (2007 Modelling Simul. Mater. Sci. Eng. 15 13–26) to simulate realistic devices with complex active layer morphologies using a dimensionally independent, scalable, finite-element method. We incorporate all stages involved in current generation, namely (1) exciton generation and diffusion, (2) charge generation and (3) charge transport in a modular fashion. The numerical challenges encountered during interrogation of realistic microstructures are detailed. We compare each stage of the photovoltaic process for two microstructures: a BHJ morphology and an idealized sawtooth morphology. The results are presented for both two- and three-dimensional structures.

Charge carrier recombination due to carrier trapping is not often considered in polymer based solar cells, except in those using non-fullerene acceptors or new donor polymers with limited short-range order. However, we show that even for the canonical poly(3-hexylthiophene): phenyl-C61-butyric acid methyl ester (P3HT:PCBM) system, relative strengths of bimolecular and trap-assisted recombination are strongly dependent on processing conditions. For slow-grown active-layers, bimolecular recombination is indeed the major loss mechanism under one sun illumination. However, for fast-grown active-layers, trap-assisted recombination dominates over bimolecular recombination by an order of magnitude, and recombination strength at short-circuit condition is 3-4 times higher, leading to loss of photocurrent and lowering of fill factor.

No abstract

No abstract