A mixture of CsPbI3 and FAPbI3 is thermodynamically stabilized in the perovskite phase with respect to the pure δ phases.

CH3NH3PbX3 (MAPbX3) perovskites have attracted considerable attention as absorber materials for solar light harvesting, reaching solar to power conversion efficiencies above 20%. In spite of the rapid evolution of the efficiencies, the understanding of basic properties of these semiconductors is still ongoing. One phenomenon with so far unclear origin is the so-called hysteresis in the current–voltage characteristics of these solar cells. Here we investigate the origin of this phenomenon with a combined experimental and computational approach. Experimentally the activation energy for the hysteretic process is determined and compared with the computational results. First-principles simulations show that the timescale for MA+ rotation excludes a MA-related ferroelectric effect as possible origin for the observed hysteresis. On the other hand, the computationally determined activation energies for halide ion (vacancy) migration are in excellent agreement with the experimentally determined values, suggesting that the migration of this species causes the observed hysteretic behaviour of these solar cells.

Organic-inorganic lead halide perovskites have unusual, temperature-dependent emission characteristics.

In this work, we study the wetting of a surface decorated with one nanogroove by a bulk Lennard-Jones liquid at various temperatures and densities. We used atomistic simulations aimed at computing the free energy of the stable and metastable states of the system, as well as the intermediate states separating them. We found that the usual description in terms of Cassie-Baxter and Wenzel states is insufficient, as the system presents two states of the Cassie-Baxter type. These states are characterized by different curvatures of the meniscus. The measured free energy barrier separating the Cassie-Baxter from the Wenzel state (and vice versa) largely exceeds the thermal energy, attesting the existence of Cassie-Baxter/Wenzel metastabilities. Finally, we found that the Cassie-Baxter/Wenzel transition follows an asymmetric path, with the formation of a liquid finger on one side of the groove and a vapor bubble on the opposite side.

In this Letter, we develop a continuum theory for the Cassie-Baxter-Wenzel (CB-W) transition. The proposed model accounts for the metastabilities in the wetting of rough hydrophobic surfaces, allows us to reconstruct the transition mechanism, and identifies the free energy barriers separating the CB and W states as a function of the liquid pressure. This information is crucial in the context of superhydrophobic surfaces, where there is interest in extending the duration of the metastable superhydrophobic CB state. The model is validated against free energy atomistic simulations.

We performed density functional calculations aimed at identifying the atomistic and electronic structure origin of the valence and conduction band, and band gap tunability of halide perovskites ABX3 upon variations of the monovalent and bivalent cations A and B and the halide anion X.

Halide perovskites are emerging as revolutionary materials for optoelectronics. Their ionic nature and the presence of mobile ionic defects within the crystal structure have a dramatic influence on the operation of thin‐film devices such as solar cells, light‐emitting diodes, and transistors. Thin films are often polycrystalline and it is still under debate how grain boundaries affect the migration of ions and corresponding ionic defects. Laser excitation during photoluminescence (PL) microscopy experiments leads to formation and subsequent migration of ionic defects, which affects the dynamics of charge carrier recombination. From the microscopic observation of lateral PL distribution, the change in the distribution of ionic defects over time can be inferred. Resolving the PL dynamics in time and space of single crystals and thin films with different grain sizes thus, provides crucial information about the influence of grain boundaries on the ionic defect movement. In conjunction with experimental observations, atomistic simulations show that defects are trapped at the grain boundaries, thus inhibiting their diffusion. Hence, with this study, a comprehensive picture highlighting a fundamental property of the material is provided while also setting a theoretical framework in which the interaction between grain boundaries and ionic defect migration can be understood.

The onset of cavitation is strongly enhanced by the presence of rough surfaces or impurities in the liquid. Despite decades of research, the way the geometry of these defects promote the nucleation of bubbles and its effect on the kinetics of the process remains largely unclear. We present here a comprehensive explanation of the catalytic action that roughness elements exert on the nucleation process for both pure vapor cavities and gas ones. This approach highlights that nucleation may follow nontrivial paths connected with a sharp decrease of the free energy barriers as compared to flat surfaces. Furthermore, we demonstrate the existence of intermediate metastable states that break the nucleation process in multiple steps; these states correspond to what is commonly known as cavitation nuclei. A single dimensionless parameter, the nucleation number, is found to control this rich phenomenology. The devised theory allows one to quantify the effect of the geometry and hydrophobicity of surface asperities on nucleation. Within the same framework, it is possible to treat both vapor cavitation, which is relevant, e.g., for organic liquids, and gas-promoted cavitation, which is commonly encountered in water. The theory is shown to be valid from the nano- to the macroscale.