The microstructure and chemistry of CuInSe2 single-crystals and Cu(In,Ga)Se2 thin films from high-efficiency devices are investigated by transmission electron microscopy and x-ray energy-dispersive spectroscopy. We find strong chemical fluctuations at the nanoscale, which result in a lattice comprising a mixture of relatively Cu-poor and Cu-rich nanodomains in both cases. These nanodomains are crystallographically coherent, and no structural lattice defects are found at the interfaces between them. These nanodomains may interconnect, forming three-dimensional, interpenetrating Cu-poor and Cu-rich percolation networks. Such interconnected structures may play a role in the high device performance of Cu(In,Ga)Se2 thin-film photovoltaics.

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