Anomalous magneto-elastic and charge doping effects in thallium-doped BaFe2As2

Within the BaFe2As2 crystal lattice, we partially substitute thallium for barium and report the effects of interlayer coupling in Ba1-xTlxFe2As2 crystals. We demonstrate the unusual effects of magneto-elastic coupling and charge doping in this iron-arsenide material, whereby Neel temperature rises with small x, and then falls with additional x. Specifically, we find that Neel and structural transitions in BaFe2As2 (TN =Ts= 133 K) increase for x=0.05 (TN = 138 K, Ts = 140 K) from magnetization, heat capacity, resistivity, and neutron diffraction measurements. Evidence from single crystal X-ray diffraction and first principles calculations attributes the stronger magnetism in x=0.05 to magneto-elastic coupling related to the shorter intraplanar Fe-Fe bond distance. With further thallium substitution, the transition temperatures decrease for x = 0.09 (TN = Ts = 131 K), and this is due to charge doping. We illustrate that small changes related to 3d transition-metal state can have profound effects on magnetism.