Efficient polymer-fullerene photovoltaic devices require close proximity of the two materials to ensure photoexcited electron transfer from the semiconducting polymer to the fullerene acceptor. We describe studies in which a bilayer system consisting of spin-cast 2-methoxy-5-(2′-ethylhexyloxy)-1,4-phenylenevinylene copolymer (MEH-PPV) and sublimed C60 is heated above the MEH-PPV glass transition temperature in an inert environment, inducing an interdiffusion of the polymer and the fullerene layers. With this process, a controlled, bulk, gradient heterojunction is created bringing the fullerene molecules within the exciton diffusion radius of the MEH-PPV throughout the film to achieve highly efficient charge separation. The interdiffused devices show a dramatic decrease in photoluminescence and concomitant increase in short circuit currents, demonstrating the improved interface.

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