Ultrafast physics in 2D halide perovskites for applications in optoelectronic devices

ULTRA-2DPK aims to elucidate the fundamental limitations in the power conversion efficiencies (PCEs) of two-dimensional (2D) halide perovskites (PKs), guide the optimization of 2DPK and 2DPK/3DPK solar cell devices, and further promote their development for industrial applications. The increasing demand for clean energy technologies in Europe dictates the search for optoelectronic devices with reduced fabrication costs and high PCEs. 2DPKs provide promising pathways for developing stable next-generation optoelectronics, including solar cells, light-emitting diodes, and lasing devices. In principle, understanding the physical mechanisms underpinning the transient electron flows and atomic motion in 2DPK-based devices can lead to unprecedented improvements in their PCEs. To this aim, experiments based on ultrafast pump-probe spectroscopy are making excellent progress. However, computational strategies to interpret the complex nonequilibrium phenomena manifested in this type of measurements are still lacking. In this fellowship, a novel first-principles methodology, that takes entirely into account electron-phonon and anharmonic dynamics will be developed. The recent advances in electronic structure and many-body theory approaches will be combined to study thermal equilibrium and nonequilibrium optoelectronic properties of 2DPKs with increasing layer thickness. ULTRA-2DPK also focuses on the transfer of knowledge of the experienced researcher in finite-temperature many-body approaches to the host institute, as well as the enhancement of his soft and research skills that will enable him to become a leading figure in his field. The objectives of the present project match perfectly with the European Union targets of a sustainable solar energy ecosystem, as well as the development of modern and low-cost optoelectronic technologies.