Spin-cast 2,4-bis[4-(N,N-diisobutylamino)-2,6-dihydroxyphenyl]squaraine (SQ) thin films only 62 A thick are converted from amorphous to polycrystalline via postannealing at elevated temperatures. The surface roughness of the SQ films increases by a factor of 2, while selected area electron diffraction spectra indicate an increase in the extent of postannealed film crystallinity. Dichloromethane solvent annealing is also demonstrated to increase the exciton diffusion length of SQ by a factor of 3 over thermally annealed SQ films as a result of further enhancement in crystalline order. We find that the roughened surface features have a length scale on the order of the exciton diffusion length. Hence, coating the donor SQ with the acceptor, C(60), results in a nearly optimum controlled bulk heterojunction solar cell structure. Optimized SQ/C(60) photovoltaic cells have a power conversion efficiency of eta(p) = 4.6 +/- 0.1% (correcting for solar mismatch) at 1 sun (AM1.5G) simulated solar intensity, and a corresponding peak external quantum efficiency of EQE = 43 +/- 1% even for the very thin SQ layers employed.
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