Caution! Static Supercell Calculations of Defect Migration in Higher Symmetry Perovskite Halides May Be Unreliable: A Case Study of Methylammonium Lead Iodide.

Activation energies of defect migration in perovskite halides are widely obtained through static supercell calculations with the nudged-elastic-band method. Taking methylammonium lead iodide (CHNHPbI, MAPbI) as an example, we demonstrate that such calculations are unreliable for the higher symmetry structures adopted by the material at temperatures relevant to device operation (tetragonal and cubic MAPbI) because, in addition to ion relaxation around the point defects, local structural modifications characteristic of the ground-state (orthorhombic) structure occur. In this way, we offer a simple explanation of why calculated activation energies of defect migration in MAPbI suffer from surprisingly large scatter.

Spectromicroscopic insights for rational design of redox-based memristive devices.

The demand for highly scalable, low-power devices for data storage and logic operations is strongly stimulating research into resistive switching as a novel concept for future non-volatile memory devices. To meet technological requirements, it is imperative to have a set of material design rules based on fundamental material physics, but deriving such rules is proving challenging. Here, we elucidate both switching mechanism and failure mechanism in the valence-change model material SrTiO3, and on this basis we derive a design rule for failure-resistant devices.

Do dislocations act as atomic autobahns for oxygen in the perovskite oxide SrTiO3?

The transport properties of edge dislocations comprising a symmetrical 6° [001] tilt grain boundary in weakly acceptor-doped SrTiO3 were investigated by means of various experimental and computational techniques. Oxygen transport along the dislocation array was probed by means of (18)O/(16)O exchange experiments under (standard) oxidising conditions (pO2 = 5 × 10(-1) bar) and also under reducing conditions (pO2 = 7 × 10(-22) bar) at T = 973 K. In both cases, isotope profiles obtained by Secondary Ion Mass Spectrometry (SIMS) indicated no evidence of fast diffusion along the dislocation array.