Is it possible for a perovskite p-n homojunction to persist in the presence of mobile ionic charge?

Recently Cui et al. reported on the fabrication a p-n homojunction perovskite solar cell (PSC) using stoichiometric control of sequentially-deposited perovskite layers. The authors propose that the junction leads to an enhanced electric field in the perovskite absorber resulting in improved charge separation. In this response to Cui et al. 2019 we show that the experimental data presented in the paper does not directly support this claim. Furthermore, Cui et al.'s thesis is not compatible with the large body of existing literature showing that mobile ionic defects present in methyl-ammonium lead iodide (MAPI) and its derivatives are highly mobile at room temperature. Using drift diffusion device simulations we show that large densities of mobile ionic charge in the system are likely to the screen any beneficial effects of a p-n homojunction.Comment: 17 pages, 5 figures, Response to a published article by Cui et a

Relationship between fill factor and light intensity in solar cells based on organic disordered semiconductors: The role of tail states

The origin of the relationship between fill factor and light intensity (FF-I) in organic disordered-semiconductor based solar cells is studied. An analytical model describing the balance between transport and recombination of charge carriers, parameterized with a factor

Generalised Framework for Controlling and Understanding Ion Dynamics with Passivated Lead Halide Perovskites

Metal halide perovskite solar cells have gained widespread attention due to their high efficiency and high defect tolerance. The absorbing perovskite layer is as a mixed electron-ion conductor that supports high rates of ion and charge transport at room temperature, but the migration of mobile defects can lead to degradation pathways. We combine experimental observations and drift-diffusion modelling to demonstrate a new framework to interpret surface photovoltage (SPV) measurements in perovskite systems and mixed electronic ionic conductors more generally. We conclude that the SPV in mixed electronic ionic conductors can be understood in terms of the change in electric potential at the surface associated with changes in the net charge within the semiconductor system. We show that by modifying the interfaces of perovskite bilayers, we may control defect migration behaviour throughout the perovskite bulk. Our new framework for SPV has broad implications for developing strategies to improve the stability of perovskite devices by controlling defect accumulation at interfaces. More generally, in mixed electronic conductors our framework provides new insights into the behaviour of mobile defects and their interaction with photoinduced charges, which are foundational to physical mechanisms in memristivity, logic, impedance, sensors and energy storage

The Unique Lipidomic Signatures of Saccharina latissima Can Be Used to Pinpoint Their Geographic Origin

The aquaculture of macroalgae for human consumption and other high-end applications is experiencing unprecedented development in European countries, with the brown algae Saccharina latissima being the flag species. However, environmental conditions in open sea culture sites are often unique, which may impact the biochemical composition of cultured macroalgae. The present study compared the elemental compositions (CHNS), fatty acid profiles, and lipidomes of S. latissima originating from three distinct locations (France, Norway, and the United Kingdom). Significant differences were found in the elemental composition, with Norwegian samples displaying twice the lipid content of the others, and significantly less protein (2.6%, while French and UK samples contained 6.3% and 9.1%, respectively). The fatty acid profiles also differed considerably, with UK samples displaying a lower content of n-3 fatty acids (21.6%), resulting in a higher n-6/n-3 ratio. Regarding the lipidomic profile, samples from France were enriched in lyso lipids, while those from Norway displayed a particular signature of phosphatidylglycerol, phosphatidylinositol, and phosphatidylcholine. Samples from the UK featured higher levels of phosphatidylethanolamine and, in general, a lower content of galactolipids. These differences highlight the influence of site-specific environmental conditions in the shaping of macroalgae biochemical phenotypes and nutritional value. It is also important to highlight that differences recorded in the lipidome of S. latissima make it possible to pinpoint specific lipid species that are likely to represent origin biomarkers. This finding is relevant for future applications in the field of geographic origin traceability and food controlpublishedVersio

Interpretation of inverted photocurrent transients in organic lead halide perovskite solar cells: proof of the field screening by mobile ions and determination of the space charge layer widths

In Methyl Ammonium Lead Iodide (MAPI) perovskite solar cells, screening of the built-in field by mobile ions has been proposed as part of the cause of the large hysteresis observed in the current/voltage scans in many cells. We show that photocurrent transients measured immediately (e.g. 100 μs) after a voltage step can provide direct evidence that this field screening exists. Just after a step to forward bias, the photocurrent transients are reversed in sign (i.e. inverted), and the magnitude of the inverted transients can be used to find an upper bound on the width of the space charge layers adjacent to the electrodes. This in turn provides a lower bound on the mobile charge concentration, which we find to be ≳1 × 1017 cm−3. Using a new photocurrent transient experiment, we show that the space charge layer thickness remains approximately constant as a function of bias, as expected for mobile ions in a solid electrolyte. We also discuss additional characteristics of the inverted photocurrent transients that imply either an unusually stable deep trapping, or a photo effect on the mobile ion conductivity

RAC1(P29S) Induces a Mesenchymal Phenotypic Switch via Serum Response Factor to Promote Melanoma Development and Therapy Resistance

RAC1 P29 is the third most commonly mutated codon in human cutaneous melanoma, after BRAF V600 and NRAS Q61. Here, we study the role of RAC1P29S in melanoma development and reveal that RAC1P29S activates PAK, AKT, and a gene expression program initiated by the SRF/MRTF transcriptional pathway, which results in a melanocytic to mesenchymal phenotypic switch. Mice with ubiquitous expression of RAC1P29S from the endogenous locus develop lymphoma. When expressed only in melanocytes, RAC1P29S cooperates with oncogenic BRAF or with NF1-loss to promote tumorigenesis. RAC1P29S also drives resistance to BRAF inhibitors, which is reversed by SRF/MRTF inhibitors. These findings establish RAC1P29S as a promoter of melanoma initiation and mediator of therapy resistance, while identifying SRF/MRTF as a potential therapeutic target

Quantum coherent control of a hybrid superconducting circuit made with graphene-based van der Waals heterostructures

Quantum coherence and control is foundational to the science and engineering of quantum systems. In van der Waals (vdW) materials, the collective coherent behavior of carriers has been probed successfully by transport measurements. However, temporal coherence and control, as exemplified by manipulating a single quantum degree of freedom, remains to be verified. Here we demonstrate such coherence and control of a superconducting circuit incorporating graphene-based Josephson junctions. Furthermore, we show that this device can be operated as a voltage-tunable transmon qubit, whose spectrum reflects the electronic properties of massless Dirac fermions traveling ballistically. In addition to the potential for advancing extensible quantum computing technology, our results represent a new approach to studying vdW materials using microwave photons in coherent quantum circuits

Transient optoelectronic characterisation and simulation of perovskite solar cells

Lead halide perovskites are a class of solution-processable semiconductor materials showing great potential for photovoltaic applications. While perovskite solar cell (PSC) efficiencies have escalated rapidly to beyond 22% in recent years, the materials suffer from a number of chemical instabilities and the processes underlying the optoelectronic response of devices are not well understood. This thesis investigates the device physics of PSCs using novel transient optoelectronic measurements combined with device simulation. A one-dimensional numerical drift-diffusion model capable of solving for electrons, holes and a single ionic charge carrier was developed to simulate perovskite devices. The inclusion of a high density of mobile ionic species in the absorber layer is found to have important consequences on both device performance and the interpretation of established measurements. Transient optoelectronic measurements are presented showing that mobile ions are present in architectures of PSC that do not exhibit current-voltage hysteresis. Simulations of p-i-n structured devices indicate that a combination of mobile ions and field-dependent interfacial recombination rates are critical to reproducing hysteresis. Transient ideality factor measurements are used to identify the dominant recombination mechanisms in PSCs. Changes in the perceived ideality factor are correlated to localised recombination, the charge carrier population overlap, and ion density profiles in simulated devices. Simulations are used to assess the validity of a zero-dimensional model applied to small perturbation transient photovoltage (TPV) measurements on perovskite devices. Two analytical models are proposed to explain the different regimes of behaviour in devices with high rates of interfacial recombination. The TPV decay in perovskites is identified as being predominantly a measure of the transport properties of the absorber layer. Together these findings demonstrate the combined power of experimental measurements and simulation to improve our physical understanding of new semiconductor technologies.Open Acces