Several recent studies have shed light on the effect of microstructure architecture onto the macroscopic mechanical properties of materials and the possibility to use a new degree of freedom in the tailoring of multi-functional properties of structure materials: the ordering of microstructure at the mesoscale. [1,2] If this concept is extensively present in natural materials such as wood or shells, where multi-modal or multi-scale architecture can be found, it is rather recently that it is consciously applied to design modern engineering materials. [1] For example, this is the case in the steel industry where complex multi-phased microstructures are produced to provide multi-functionality such as high elastic limit for prolonged lifetime and ductility for improved formability. Similarly, nanocomposite metals are seen as strong candidates for several applications in extreme environment (high dose irradiation, severe deformation, shock, high magnetic field, high temperature, etc.) because the combination of refined microstructure, inter-phase boundaries and hierarchy provides unique macroscopic properties, not available in standard materials. [3] However, the main challenge still remains in the full understanding of the complex interaction existing between materials properties and their architecture, in particular when size effects affect the elementary physical mechanisms. In this field, combined experimental and simulation efforts are mandatory.From the experimental point of view, the full knowledge of the microstructure is necessary, from atomic to macroscopic scales; this can be obtained by a combination of standard and advanced characterization techniques. Similarly, to characterize the impact of architecture on macroscopic mechanical properties, specific testing techniques must be developed: in this field, the combination of deformation and diffraction appears to be particularly well suited. Thanks to the high penetration depth of thermal neutrons or high energy X-rays (at synchrotrons) and the crystallographic selectivity of diffraction, in-situ deformation tests under neutrons or X-rays can indeed bring deep insight into the role of internal stresses and reveal the phase-specific deformation behavior and strengthening mechanisms of complex materials. In the present article, the results obtained in the case of Cu-Nb
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