Improving superconductivity in BaFe2As2-based crystals by cobalt clustering and electronic uniformity

Quantum materials such as antiferromagnets or superconductors are complex in that chemical, electronic, and spin phenomena at atomic scales can manifest in their collective properties. Although there are some clues for designing such materials, they remain mainly unpredictable. In this work, we find that enhancement of transition temperatures in BaFe2As2-based crystals are caused by removing local-lattice strain and electronic-structure disorder by thermal annealing. While annealing improves Néel-ordering temperature in BaFe2As2 crystal (TN = 132 K to 136 K) by improving in-plane electronic defects and reducing overall a-lattice parameter, it increases superconducting-ordering temperature in optimally cobalt-doped BaFe2As2 crystal (Tc = 23 to 25 K) by precipitating-out the cobalt dopants and giving larger overall a-lattice parameter. While annealing improves local chemical and electronic uniformity resulting in higher TN in the parent, it promotes nanoscale phase separation in the superconductor resulting in lower disparity and strong superconducting band gaps in the dominant crystal regions, which lead to both higher overall Tc and critical-current-density, Jc.