We have studied the relationship between the structure and the spin Hall angle of the early 5d transition metals in X/CoFeB/MgO (X=Hf, Ta, W, Re) heterostructures. Spin Hall magnetoresistance (SMR) is used to characterize the spin Hall angle of the heavy metals.Transmission electron microscopy images show that all underlayers are amorphous-like when their thicknesses are small, however, crystalline phases emerge as the thickness is increased for certain elements. We find that the heavy metal layer thickness dependence of the SMR reflects these changes in structure. The spin Hall angle largest | SH | of Hf, Ta, W and Re (~0.11, 0.10, 0.23 and 0.07, respectively) is found when the dominant phase is amorphous-like. We find that the amorphous-like phase not only possesses large resistivity but also exhibits sizeable spin Hall conductivity, which both contribute to the emergence of the large spin Hall angle.*Email: hayashi.masamitsu@nims.go.jp 2 Heavy metals with strong spin orbit coupling are attracting great interest recently 1-3 as such elements can generate significant amount of spin current via the spin Hall effect 4 . In heterostructures that contain a heavy metal layer and a magnetic layer, the spin current generated within the heavy metal layer can diffuse into the magnetic layer and trigger current induced magnetization switching 2, 5 and domain wall motion [6][7][8][9] . Key to the development of technologies that make use of such current induced effects is the large spin Hall angle of the heavy metal layer 10, 11 .The spin Hall angle, which defines the amount of spin current generated within the layer, is known to be element specific. First principle calculations 12 show that the spin Hall angle of the transition metals depends on the electron filling of the d-orbitals if the mechanism behind it is due to an intrinsic origin (i.e., band structure related) 13 . In addition, the spin Hall effect can originate from spin dependent scattering of electrons, commonly referred to as an extrinsic effect 14,15 . Recently large spin Hall angle has been reported for the heavy transition metals 2,[16][17][18][19] and/or its alloy 20 . The large spin Hall angle for the early 5d transition metals (e.g. Ta and W) has been associated 2,16,21 with the appearance of the distorted tetragonal phase, often known as the A-15 -phase [22][23][24][25] . In order to develop viable devices utilizing the spin Hall effect, it is thus essential to understand how the structure of the heavy metal influences, if any, the size of the spin Hall angle. Identifying the relationship between the structural phase of the heavy metal layer and its spin Hall angle, however, requires thorough and systematic studies.Here we show studies on the spin Hall angle of the early 5d transition metals (Hf, Ta, W, Re) in magnetic heterostructures. Spin Hall magnetoresistance (SMR) 18,[26][27][28] and transmission electron microscopy (TEM) are used to evaluate, respectively, the spin transport properties and the structural phase of the films. We find that t...