Nanoscale defects in superconductors play a dominant role in enhancing superconducting properties through electron scattering, modulation of coherence length, and correlation with quantized magnetic flux. For ironbased superconductors (IBSCs) that are expected to be employed in high-field magnetic applications, a fundamental question is whether such defects develop an upper critical field (Hc2) similar to that of conventional BCS-type superconductors. Herein, we report the first demonstration of a significantly improved Hc2 in a 122-phase IBSC by introducing defects through high-energy milling. Co-doped Ba122 polycrystalline bulk samples (Ba(Fe,Co)2As2) were prepared by sintering powder which was partially mechanically alloyed through high-energy milling. A remarkable increase in full-width at half maximum of X-ray powder diffraction peaks, anomalous shrinkage in the a-axis, and elongation in the c-axis were observed. When lattice defects are introduced into the grains, semiconductor behavior of the electric resistivity at low temperature (T < 100 K), slight decrease in transition temperature (Tc), upturn of Hc2(T) near Tc, and a large increase in Hc2(T) slope were observed. The slope of Hc2(T) increased approximately by 50%, i.e., from 4 to 6 T/K, and exceeded that of single crystals and thin films. Defect engineering through high-energy milling is expected to facilitate new methods for the designing and tuning of Hc2 in 122-phase IBSCs.

The effect of microstructure control on intergranular critical current density (J c ) was evaluated using Co-doped Ba122 as a model material. Polycrystalline bulk samples were prepared by sintering mechanically alloyed powder prepared by planetary ball milling. Between low and intermediate milling energy, refinement of grain size, improvement in the uniformity of structure and composition, and a threefold improvement in J c were observed with increasing milling energy. These indicate that the high-energy milling is an effective method for the synthesis of single-phase Ba122 samples and improvement of J c by controlling the microstructure. At very high milling energy, the grain size of Ba122 reached as small as 30 nm, abnormal aggregates were formed, and the magnetic T c and J c decreased. Our results suggest that the suppression of the formation of large aggregates and control of grain boundary properties are necessary to achieve superior critical current properties.

The thermal properties are one of the key parameters to control phase purity and microstructure of polycrystalline materials. The melting point of the iron-based BaFe2As2 superconductor (Ba122), which foresees high-field applications, remains controversial. In this work, thermogravimetry-differential scanning calorimetry measurements (TG-DSC) of undoped and Co-doped Ba122 were carried out. Mixtures of elemental metals and pre-reacted Ba122 powders were prepared to investigate the thermal responses during in situ and ex situ synthesis routes, respectively. In addition, the phases and microstructures of the quenched samples were evaluated to elucidate the observed exothermic/endothermic peaks. Our results suggest that the melting point of Ba122 is ∼1300 °C.

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