The optical properties of composition-spread (SrxCa1−x)2CuO3(0⩽x⩽1) films showing high third-order optical nonlinearity are systematically investigated. Desired orientations and high crystallinity are obtained for the entire composition x by employing a composition-spread [(Sr2TiO4)x(LaSrAlO4)1−x] buffer layer and a temperature-gradient method in order to compensate the change in lattice mismatch and growth temperature depending on x. Linear absorption spectra and third-harmonic intensity with an exciting wavelength of 1.56 μm are measured as a function of x. As the Cu–O bond length increases with x, the charge-transfer gap decreases and the third-harmonic intensity increases, and both the charge-transfer gap and third-harmonic intensity change almost linearly with x between Ca2CuO3 and Sr2CuO3.

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