Levgen Levchuk, Florian Hoegl, Marco Brandl, Andres Osvet, Rainer Hock, Patrick Herre, Wolfgang Wolfgang, Peter Schweizer, Erdmann Spiecker, Miroslaw Batentschuk, Christoph Brabec
Organometallic halide perovskites CH3NH3BX3 (B= Pb, Sn, Ge; X = I, Br, Cl) have become one of the most promising semiconductors for solar cell applications, reaching power conversion efficiencies beyond 20%. Improving our ability to harness the full potential of organometal halide perovskites requires the development of more reliable synthesis routines of well defined, reproducible and defect free reference systems allowing to study the fundamental photo-physical processes.
In this study we present size and band gap engineering for organo-lead perovskites crystallites with various shapes and sizes ranging from the 5 nm regime all the way to 1 cm. Colloidal nano-crystals, micro-crystlline particles as well as single crystals are demonstrated with excellent purity and control in shape and size are demonstrated. The structural, optical and photo-physical properties of these reference materials are investigated and analyzed as function of their size and shape.
While the development of perovskite-based semitransparent solar cells with competitive levels of transparency and efficiency offer a promising perspective towards building integrated photovoltaics, the color perception of perovskite films is of limited visual aesthetics, compromising their applicability to facades and windows. In the present work, we develop a technique to grow crystalline, ultrathin perovskite films through a solvent-solvent extraction process featuring full crystallization within few seconds at RT and under 45%RH environmental conditions. As a result we obtained the highest combination of efficiency and transparency to date for perovskite solar cells. We further improved the visual aesthetics of our devices by implementing dielectric mirrors. EQE and UV-Vis spectroscopic measurements are performed to fully characterize the device stacks featuring four different dielectric mirror configurations. By customizing the mirror to the near-IR absorption region of the perovskite, we could increase the Jsc by 18.7%, yielding a light blue appearance and showing 31.4% transparency at 3.5% electrical power efficiency. Both, the solar cells and the dielectric mirrors are fully-solution processed under ambient conditions and are easily transferable to roll-to-roll upscaling. Optical simulations support our experimental findings and provide a global perspective emulating full device stack appearance covering all the colors in the visible spectra. Transparency, photocurrent density contribution and chromaticity are finally simulated and analyzed. Based on the detailed analysis, we give an outlook on the performance – color – transparency roadmap for perovskite solar cells.
Levgen Levchuk, Yi Hou, Marco Gruber, Patrick Herre, Marco Brandl, Andres Osvet, Rainer Hock, Wolfgang Peukert, Rik Tykwinski, Miroslaw Batentschuk, Christoph Brabec
Solution based perovskite solar cell fabrication typically involves rather complex processing sequences to yield highest performance. While most studies concentrate on the exploration of processing conditions, we have investigated the purity levels of common perovskite precursor solutions and found a number of impurities which are most critically controlling the crystallization of perovskites. Moreover, we identified these impurities at different level of concentrations is all commercially available precursors.
In detail, we present a detailed chemical study on the nature of the various impurities in CH3NH3I and explored their impact on the crystal formation. The detrimental role of the impurities is best demonstrated by comparing perovskite solar cell devices fabricated from impurity free precursors vs precursors containing different concentrations of impurities. Most interestingly, we revealed that a certain concentration of impurities is detrimental to facilitate the growth of large grained crystals. This study gives valuable insight into the rate determining steps of perovskite crystal growth and provides the basis for developing reliable and reproducible high performance recipes for Perovskite solar cell processing.
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