Through a combination of aberration-corrected high-resolution scanning transmission electron microscopy and three-dimensional atom probe tomography, the true atomic-scale structure and change in chemical composition across the complex order-disorder interface in a metallic alloy has been determined. The study reveals the presence of two interfacial widths, one corresponding to an order-disorder transition, and the other to the compositional transition across the interface, raising fundamental questions regarding the definition of the interfacial width in such systems. DOI: 10.1103/PhysRevLett.102.086101 PACS numbers: 68.35.Àp, 68.37.Ma, 68.37.Vj Interfaces play an important role in determining several properties in multiphase systems [1][2][3]. Atomic-scale renditions of the interface structure have been primarily accomplished through high-resolution transmission electron microscope (HRTEM) phase-contrast images (and simulations) that allow for identification of the positions of atomic columns and structural defects at the interface [4,5]. Recent advances in HRTEM and HRSTEM have been enabled by the development of spherical aberration correctors for the electron probe as well as the image [6][7][8].In parallel, developments in first-principles based electronic structure calculations and larger scale atomistic modeling tools permit more accurate simulations of the interface structure [9,10]. Recent atomistic simulations of the interface between an ordered precipitate and disordered matrix in a nickel-base superalloy indicate that the interface is not abrupt at the atomic scale [9]. While the implications of these results on the microstructural stability [11][12][13] and high temperature mechanical properties [14][15][16][17][18][19] are substantial, there is no clear experimental evidence confirming these atomistic simulations. The limitations associated with the resolution of experimental techniques have so far prevented direct atomic-scale imaging and interpretation of the structural and compositional transition across such interfaces. Techniques such as 3D Atom Probe (3DAP) Tomography have enabled detailed exploration of nanometer-scale elemental partitioning across interphase interfaces, including the = 0 interface in nickel base alloys [20][21][22][23][24][25][26]. In addition, developments in aberrationcorrected HRSTEM now permit Z contrast imaging (arising from the differences in atomic numbers) and interpretation at atomic resolution [27][28][29]. Our study provides direct experimental evidence at the atomic scale of the true structure and composition of the = 0 interface in a nickel base alloy by coupling two advanced and complementary techniques: aberration-corrected HRSTEM and 3DAP.This work was carried out on the nickel base superalloy Rene' 88 DT [nominal composition 55.63Ni-18.02Cr-13.00Co-4.74Ti-4.45Al-2.48Mo-1.21W-0.46Nb (in at %)], with superior creep and fatigue properties for turbine disk applications [14][15][16]. The typical microstructure consists of a disordered fcc matrix with ordered ...