Single crystals of Fe(1+x)Te(1-y)Se(y) have been grown with a controlled Fe excess and Se doping, and the crystal structure has been refined for various compositions. The systematic investigation of magnetic and superconducting properties as a function of the structural parameters shows how the material can be driven into various ground states, depending on doping and the structural modifications. Our results prove that the occupation of the additional Fe site, Fe2, enhances the spin localization. By reducing the excess Fe, the antiferromagnetic ordering is weakened, and the superconducting ground state is favored. We have found that both Fe excess and Se doping in synergy determine the properties of the material and an improved 3-dimensional phase diagram is proposed.
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