• Energy Research

Methylammonium lead halide perovskites have emerged as high performance photovoltaic materials. Most of these solar cells are prepared via solution-processing and record efficiencies (>20%) have been obtained employing perovskites with mixed halides and organic cations on (mesoscopic) metal oxides. Here, we demonstrate fully vacuum deposited planar perovskite solar cells by depositing methylammonium lead iodide in between intrinsic and doped organic charge transport molecules. Two configurations, one inverted with respect to the other, p-i-n and n-i-p, are prepared and optimized leading to planar solar cells without hysteresis and very high efficiencies, 16.5% and 20%, respectively. It is the first time that a direct comparison between these two opposite device configurations has been reported. These fully vacuum deposited solar cells, employing doped organic charge transport layers, validate for the first time vacuum based processing as a real alternative for perovskite solar cell preparation.

A generic solar cell structure using undoped charge extraction layer is presented, that lead to efficient and rather stable solar cells.

Halide perovskites have generated considerable research interest due to their excellent optoelectronic properties in the past decade. To ensure the formation of high-quality semiconductors, the deposition process for the perovskite film is a critical issue. Vacuum-based processing is considered to be a promising method, allowing, in principle, for uniform deposition on a large area. One of the benefits of vacuum processing is the control over the film composition through the use of quartz crystal microbalances (QCMs) that monitor the rates of the components in situ. In metal halide perovskites, however, one frequently employed component or precursor, CH3NH3I, exhibits nonstandard sublimation properties. Here, we study in detail the sublimation properties of CH3NH3I and demonstrate that by correcting for its complex adsorption properties and by modeling the film growth, accurate predictions of the stoichiometry of the final perovskite film can be obtained.

Abstract Planar perovskite solar cells using organic charge selective contacts were fabricated. In a vacuum deposited perovskite-based solar cell, dopant and additive free triazatruxene as the hole transport layer was introduced for device fabrication. High open-circuit voltage of 1090 mV was obtained using methylammonium lead iodide (Eg=1.55 eV) as light harvesting material, thus representing a loss of only 460 mV which is in close vicinity of mature silicon technology (400 mV). The devices showed a very competitive photovoltaic performance, monochromatic incident photon-to-electron conversion efficiency of 80% and the power conversion efficiencies in excess of 15% were measured with a negligible degree of hysteresis.

Hetero-structures for Efficient Luminescent Devices (HELD) Perovskite Thin-film Photovoltaics (PERTPV) Preparation of black formamidinium lead iodide (FAPbI3) requires high temperature annealing and the incorporation of smaller A-site cations, such as methylammonium (MA+), cesium or rubidium. A major advantage of vacuum processing is the possibility to deposit perovskite films at room temperature (RT), without any annealing step. Here we demonstrate stabilization of the cubic perovskite phase at RT, in a three-sources co-sublimation method. We found that the MA+ incorporation is a self-limiting process, where the amount of MA+ which is incorporated in the perovskite is essentially unvaried with increasing MAI deposition rate. In this way a phase-pure, cubic perovskite with a bandgap of 1.53 eV can be obtained at room temperature. When used in fully vacuum-processed perovskite solar cells, PCEs up to 18.8% were obtained. Despite the presence of MA+, the solar cells were found to be thermally stable and maintained 90% of their initial efficiency after 1 month of continuous operation. EXCELLENT SCIENCE - European Research Council (ERC)

Perovskite solar cells are analyzed by photo- and electroluminescence hyperspectral imaging. Significant spatial inhomogeneities in the quasi-Fermi level splitting are observed.

A voltage decay based method to probe ionic concentrations and diffusivities in perovskite solar cells is herein presented and verified with a newly developed drift-diffusion simulation tool.

We introduce new hole-selective contacts for next-generation perovskite photovoltaics and point to design paths for molecular engineering of perfect interfaces.