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Structural properties and hole distribution in the spin-ladder compound Sr(14-x)Ca(x)Cu(24)O(41) have been extensively investigated by transmission electron microscopy (TEM). The complex electron diffraction patterns and high-resolution TEM observations reveal a clear incommensurate structural modulation along the c-axis direction attributable to two mismatched sublattices; this modulation strongly depends on hole distribution in the compounds. The fine structures of the O K and Cu L(2,3) ionization edges for the Sr(14-x)Ca(x)Cu(24)O(41) compounds recorded under different conditions indicate that more doped holes reside in the chains than the ladders, and that substituting Ca for Sr atoms results in a charge redistribution between the chains and ladders. Based on the experimental findings, the theoretical results, including the partial density of states and optical conductivity spectra calculated by the density functional theory, are also discussed.

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