Nanostructuring Mixed‐Dimensional Perovskites: A Route Toward Tunable, Efficient Photovoltaics2D perovskites is one of the proposed strategies to enhance the moisture resistance, since the larger organic cations can act as a natural barrier. Nevertheless, 2D perovskites hinder the charge transport in certain directions, reducing the solar cell power conversion efficiency. A nanostructured mixed-dimensionality approach is presented to overcome the charge transport limitation, obtaining power conversion efficiencies over 9%. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
Switching the activity of Cas12a using guide RNA strand displacement circuitsThe CRISPR effector protein Cas12a has been used for a wide variety of applications such as in vivo gene editing and regulation or in vitro DNA sensing. Here, we add programmability to Cas12a-based DNA processing by combining it with strand displacement-based reaction circuits. We first establish a viable strategy for augmenting Cas12a guide RNAs (gRNAs) at their 5' end and then use such 5' extensions to construct strand displacement gRNAs (SD gRNAs) that can be activated by single-stranded RNA trigger molecules. These SD gRNAs are further engineered to exhibit a digital and orthogonal response to different trigger RNA inputs-including full length mRNAs-and to function as multi-input logic gates. We also demonstrate that SD gRNAs can be designed to work inside bacterial cells. Using such in vivo SD gRNAs and a DNase inactive version of Cas12a (dCas12a), we demonstrate logic gated transcriptional control of gene expression in E. coli.
Synthesis of Perfectly Oriented and Micrometer-Sized MAPbBr<sub>3</sub> Perovskite Crystals for Thin-Film Photovoltaic ApplicationsWide band gap perovskites such as methylammonium lead bromide are interesting materials for photovoltaic applications because of their potentially high open-circuit voltage. However, the fabrication of high-quality planar films has not been investigated in detail for this material. We report a new synthesis approach for the fabrication of bromide-based perovskite planar films based on the control of the deposition environment. We achieve dense layers with large and perfectly oriented crystallites 5–10 μm in size. Our results show that large crystal sizes can be achieved only for smooth indium-doped tin oxide substrates, whereas lateral perovskite crystal growth is limited for the rougher fluorine-doped tin oxide substrates. We additionally correlate photocurrent and perovskite crystal properties in photovoltaic devices and find that this parameter is maximized for ordered systems, with internal quantum efficiencies approaching unity. Hence, our work not only gives a new pathway to tune morphology and crystal orientation but also demonstrates its importance for planar perovskite solar cells.
Toward Tailored Film Morphologies: The Origin of Crystal Orientation in Hybrid Perovskite Thin FilmsEfficient perovskite solar cells can be produced by a wide variety of different methods. Previous results show that controlling the film morphology is critical to enhance the efficiency of the prepared devices. Here, grazing‐incidence wide‐angle X‐ray scattering (GIWAXS) is used to study the morphology and especially the orientation distribution of CH 3 NH 3 PbI 3 (MAPI) perovskite films prepared by five typical methods. We find that the investigated one‐step methods produce non‐oriented films, while the two‐step deposition methods produce varying degrees of orientation depending on the method chosen to convert the highly oriented PbI 2 precursor, providing direct evidence for different perovskite conversion mechanisms. In particular, we show that the morphology and crystal orientation of MAPI films is tunable by varying the spin‐coating temperature and by adding chloride to the conversion solution. By relating the precursor morphology to the resulting MAPI film morphology, we link the observed preferential orientations to specific conversion mechanisms, thereby establishing GIWAXS as an important tool toward a rational development of new synthesis methods.
In Situ Monitoring the Uptake of Moisture into Hybrid Perovskite Thin FilmsJohannes Schlipf, Lorenz Bießmann, Lukas Oesinghaus et al.|The Journal of Physical Chemistry Letters|2018 Solution-processed hybrid perovskites are of great interest for use in photovoltaics. However, polycrystalline perovskite thin films show strong degradation in humid atmospheres, which poses an important challenge for large-scale market introduction. With in situ grazing incidence neutron scattering (GISANS) we analyzed water content, degradation products, and morphological changes during prolonged exposure to several humidity levels. In high humidity, the formation of metastable hydrate phases is accompanied by domain swelling, which transforms the faceted crystals to a round-washed, pebble-like form. The films incorporate much more water than is integrated into the hydrates, with smaller crystals being more affected, making the degradation strongly dependent on film morphology. Even at low humidity, water is adsorbed on the crystal surfaces without the formation of crystalline degradation products. Thus, although production in an ambient atmosphere is of interest for industrial production it might lead to long-term degradation without appropriate countermeasures like postproduction drying below 30% RH.