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We report on magnetisation measurements of Sr14-xCaxCu24O41, with 0 <= x <= 12, in magnetic fields up to 16 T. The low temperature magnetic response of the CuO2 spin chains changes strongly upon doping. For x = 0, the ground state with nearly independent dimers is confirmed. Reduction of the number of holes in the chains through Ca-doping leads to an additional contribution to the magnetisation, which depends linearly on the magnetic field. Remarkably, the slope of this linear contribution increases with the Ca content. We argue that antiferromagnetic spin chains do not account for this behaviour but that the hole dynamics might be involved.

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