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Organic-inorganic hybrid perovskites are promising materials for the next generation photovoltaics and optoelectronics; however, their practical application has been hindered by poor structural stability mainly caused by ion migration and external stimuli. Understanding the mechanism(s) of ion migration and structure decomposition is thus critical. Here we observe the sequence of structural changes at the atomic level that precede structural decomposition in the technologically important Cs1-xFAxPbI3 using ultralow dose transmission electron microscopy. We find that these changes differ, depending upon the A-site composition. Initially, there is a random loss of FA+, complemented by the loss of I-. The remaining FA+ and I- ions then migrate, unit cell by unit cell, into an ordered and more stable phase with a √2 x √2 superstructure. Further ion loss is accompanied by A-site dependent octahedral tilt modes and associated tetragonal phases with different stabilities. These observations of the loss of FA+/I- ion pairs, ion migration, octahedral tilt modes, and the role of the A-cation, provide insights into the atomic-scale structural mechanisms that drive and block ion loss and ion migration, opening pathways to inhibit ion loss, migration and improve structural stability. Applications of perovskite solar cells have been hindered by ion migration and structural instability. Here, the authors use ultra-low dose transmission electron microscopy to reveal the process of ion migration and structural change at the atomic level in Cs1-xFAxPbI3. [ABSTRACT FROM AUTHOR]

Electronic phase separation in complex oxides is the inhomogeneous spatial distribution of electronic phases, involving length scales much larger than those of structural defects or nonuniform distribution of chemical dopants. While experimental efforts focused on phase separation and established its correlation with nonlinear responses under external stimuli, it remains controversial whether phase separation requires quenched disorder for its realization. Early theory predicted that if perfectly "clean" samples could be grown, both phase separation and nonlinearities would be replaced by a bicritical-like phase diagram. Here, using a layer-by-layer superlattice growth technique we fabricate a fully chemically ordered "tricolor" manganite superlattice, and compare its properties with those of isovalent alloyed manganite films. Remarkably, the fully ordered manganite does not exhibit phase separation, while its presence is pronounced in the alloy. This suggests that chemical-dopinginduced disorder is crucial to stabilize the potentially useful nonlinear responses of manganites, as theory predicted. [ABSTRACT FROM AUTHOR]

We present an alternative atomic resolution incoherent imaging technique derived from scanning transmission electron microscopy (STEM) using detectors in real space, in contrast to conventional STEM that uses detectors in diffraction space. The images obtained from various specimens have a resolution comparable to conventional high-angle annular dark-field (HAADF) STEM with good contrast, which seems to be very robust with respect to thickness, focus and imaging conditions. The results of the simulations are consistent with the experimental results and support the interpretation of the real-space STEM image contrast as being a result of aberration-induced displacements of the high-angle scattered electrons., (© 2011 International Union of Crystallography)

The structure of a periodic object, such as a crystal, may be described by an infinite series of Fourier coefficients and phases. In associating this with scattering theory appropriate to any radiation, a classic problem arises, namely, the determination of phases from the resulting discrete diffraction pattern. The solution to this phase problem is presented in this paper in which the first direct measurement of structural phase by inspection of convergent-beam electron diffraction patterns is described.