The superconducting series, Fe(Te,Se), has a complex structural and magnetic phase diagram that is dependent on composition and occupancy of a secondary interstitial Fe site. In this letter, we show that superconductivity in Fe1+xTe0.7Se0.3 can be enhanced by topotactic deintercalation of the interstitial iron, demonstrating the competing roles of the two iron sites. Neutron diffraction reveals a flattening of the Fe(Te,Se)4 tetrahedron on Fe removal of iron and an increase in negative thermal

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... xpansion within the ab plane that correlates with increased lattice strain. Inelastic neutron scattering shows that a gapped excitation at 6 meV, evolves into gapless paramagnetic scattering with increasing iron; similar to the fluctuations observed for non-superconducting Fe1+xTe itself.