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Architected Metal Selenides via Sequential Cation and Anion Exchange on Self-Organizing Nanocomposites
Get PDFShape-preserving conversion reactions have the potential to unlock new routes for self-organization of complex three-dimensional (3D) nanomaterials with advanced functionalities. Specifically, developing such conversion routes toward shape-controlled metal selenides is of interest due to their photocatalytic properties and because these metal selenides can undergo further conversion reactions toward a wide range of other functional chemical compositions. Here, we present a strategy toward metal selenides with controllable 3D architectures using a two-step self-organization/conversion approach. First, we steer the coprecipitation of barium carbonate nanocrystals and silica into nanocomposites with controllable 3D shapes. Second, using a sequential exchange of cations and anions, we completely convert the chemical composition of the nanocrystals into cadmium selenide (CdSe) while preserving the initial shape of the nanocomposites. These architected CdSe structures can undergo further conversion reactions toward other metal selenides, which we demonstrate by developing a shape-preserving cation exchange toward silver selenide. Moreover, our conversion strategy can readily be extended to convert calcium carbonate biominerals into metal selenide semiconductors. Hence, the here-presented self-assembly/conversion strategy opens exciting possibilities toward customizable metal selenides with complex user-defined 3D shapes
Recruiting Unicellular Algae for the Mass Production of Nanostructured Perovskites
Get PDFFunctional capacities of lead halide perovskites are strongly dependent on their morphology, crystallographic texture, and internal ultrastructure on the nano- and the meso-scale. In the last decade, significant efforts are directed towards the development of novel synthesis routes that would overcome the morphological constraints provided by the physical and crystallographic properties of these materials. In contrast, various living organisms, such as unicellular algae, have the ability to mold biogenic crystals into a vast variety of intricate nano-architectured shapes while keeping their single crystalline nature. Here, using the cell wall of the dinoflagellate L. granifera as a model, sustainably harvested biogenic calcite is successfully transformed into nano-structured perovskites. Three variants of lead halide perovskites CH3NH3PbX3 are generated with X = Cl−, Br− and I−; exhibiting emission peak-wavelength ranging from blue, to green, to near-infrared, respectively. The approach can be used for the mass production of nano-architectured perovskites with desired morphological, textural and, consequently, physical properties exploiting the numerous templates provided by calcite forming unicellular organisms
Emerging topics in nanophononics and elastic, acoustic, and mechanical metamaterials: an overview
Get PDFThis broad review summarizes recent advances and "hot"research topics in nanophononics and elastic, acoustic, and mechanical metamaterials based on results presented by the authors at the EUROMECH 610 Colloquium held on April 25-27, 2022 in Benicássim, Spain. The key goal of the colloquium was to highlight important developments in these areas, particularly new results that emerged during the last two years. This work thus presents a "snapshot"of the state-of-the-art of different nanophononics- and metamaterial-related topics rather than a historical view on these subjects, in contrast to a conventional review article. The introduction of basic definitions for each topic is followed by an outline of design strategies for the media under consideration, recently developed analysis and implementation techniques, and discussions of current challenges and promising applications. This review, while not comprehensive, will be helpful especially for early-career researchers, among others, as it offers a broad view of the current state-of-the-art and highlights some unique and flourishing research in the mentioned fields, providing insight into multiple exciting research directions
Optical Characterization of Plasmonic Indium Lattices Fabricated via Electrochemical Deposition
Get PDFThe optical properties of periodic metallic nanoparticle lattices have found many exciting applications. Indium is an emerging plasmonic material that offers to extend the plasmonic applications given by gold and silver from the visible to the ultraviolet spectral range, with applications in imaging, sensing, and lasing. Due to the high vapor pressure/low melting temperature of indium, nanofabrication of ordered metallic nanoparticles is nontrivial. In this work, we show the potential of selective area electrochemical deposition to generate large-area lattices of In pillars for plasmonic applications. We study the optical response of the In lattices by means of angle-dependent extinction measurements demonstrating strong plasmonic surface lattice resonances and a good agreement with numerical simulations. The results open avenues toward high-quality lattices of plasmonic indium nanoparticles and can be extended to other promising plasmonic materials that can be electrochemically grown
The K2: Open-source simultaneous triple-color TIRF microscope for live-cell and single-molecule imaging
Get PDFImaging the dynamics and interactions of biomolecules at the single-molecule level in live cells and reconstituted systems has generated unprecedented knowledge about the biomolecular processes underlying many cellular functions. To achieve the speed and sensitivity needed to detect and follow individual molecules, these experiments typically require custom-built microscopes or custom modifications of commercial systems. The costs of such single-molecule microscopes, their technical complexity and the lack of open-source documentation on how to build custom setups therefore limit the accessibility of single-molecule imaging techniques. To advance the adaptation of dynamic single-molecule imaging by a wider community, we present the “K2”: an open-source, simultaneous triple-color total internal reflection fluorescence (TIRF) microscope specifically designed for live-cell and single-molecule imaging. We explain our design considerations and provide step-by-step building instructions, parts list and full CAD models. The modular design of this TIRF microscope allows users to customize it to their scientific and financial needs, or to re-use parts of our design to improve the capabilities of their existing setups without necessarily having to build a full copy of the K2 microscope
Self-Tracking Solar Concentrator with Absorption of Diffuse Sunlight
Get PDFThe highest solar cell efficiencies are obtained with concentrating systems. However, these systems have two major drawbacks: solar tracking is needed and diffuse sunlight is poorly absorbed. Here, a system that overcomes both limitations is presented, by exploiting light-induced halide segregation in mixed halide perovskite films. A monolayer of silica microspheres focuses direct sunlight in a mixed halide perovskite film below. Through light-induced phase segregation a low bandgap region forms in the focal point. Together with funneling of excited states toward the low bandgap regions, this results in a voltage increase characteristic for concentrating systems. Diffuse sunlight is still absorbed by the high bandgap material, avoiding the loss of diffuse sunlight characteristic for conventional concentrators. The formation of low bandgap regions in the perovskite is dynamic, and can follow the position of the focus as the sun moves throughout the day, making solar tracking unnecessary. With detailed optical and electrical simulations, it is shown that this concept can lead to an increase in both voltage and current. This leads to a 6.6% absolute increase in power conversion efficiency compared to the film without microspheres. Absorption and emission measurements confirm the concentration effect, showing the promising potential for a self-optimizing concentrating system
AI et al.: Machines Are About to Change Scientific Publishing Forever
Get PDFArtificial intelligence (AI)-powered text generation will change scientific publishing fundamentally. In the past year, multiple AI systems have showcased production of visual and textual content increasingly indistinguishable from human-generated work, creating almost overnight new possibilities for intellectual workers, and at the same time raising similarly potent concerns. While artists and journalists are more evidently at the forefront of this incipient revolution, it is not hard to imagine a researcher looking away from the frustratingly sparse draft of a research article and wondering: “Could a machine write it for me?
Hybrid cavity-antenna architecture for strong and tunable sideband-selective molecular Raman scattering enhancement
Get PDFPlasmon resonances at the surface of metallic antennas allow for extreme enhancement of Raman scattering. Intrinsic to plasmonics, however, is that extreme field confinement lacks precise spectral control, which would hold great promise in shaping the optomechanical interaction between light and molecular vibrations. We demonstrate an experimental platform composed of a plasmonic nanocube-on-mirror antenna coupled to an open, tunable Fabry-Perot microcavity for selective addressing of individual vibrational lines of molecules with strong Raman scattering enhancement. Multiple narrow and intense optical resonances arising from the hybridization of the cavity modes and the plasmonic broad resonance are used to simultaneously enhance the laser pump and the local density of optical states, and are characterized using rigorous modal analysis. The versatile bottom-up fabrication approach permits quantitative comparison with the bare nanocube-on-mirror system, both theoretically and experimentally. This shows that the hybrid system allows for similar SERS enhancement ratios with narrow optical modes, paving the way for dynamical backaction effects in molecular optomechanics
Toward Improving Triplet Energy Transfer from Tetracene to Silicon Using a Covalently Bound Tetracene Seed Layer
Get PDFSilicon solar cells are operating close to the theoretical maximum efficiency limit. To increase their efficiency beyond this limit, it is necessary to decrease energy losses occurring for high-energy photons. A sensitizing layer of singlet-fission material can in principle double the current generated by high-energy photons, and significantly reduce energy losses from high-energy photons within the solar cell. Here, we construct a model of such a solar cell, using Si(111) surfaces and tetracene. To increase the energy transfer between the two layers, a series of tetracene derivatives was synthesized, and the molecules were covalently attached onto the silicon surface as a seed layer. Using X-ray diffraction, a shift in crystal structure and ordering of the tetracene close to the seed layer can be observed. Unfortunately, the effect on the energy transfer was limited, showing a need for further investigations into the effect of the seed layer
Evolution with recombination as Gibbs sampling
Get PDFThis work presents a population genetic model of evolution, which includes haploid selection, mutation, recombination, and drift. The mutation-selection equilibrium can be expressed exactly in closed form for arbitrary fitness functions without resorting to diffusion approximations. Tractability is achieved by generating new offspring using n-parent rather than 2-parent recombination. While this enforces linkage equilibrium among offspring, it allows analysis of the whole population under linkage disequilibrium. We derive a general and exact relationship between fitness fluctuations and response to selection. Our assumptions allow analytical calculation of the stationary distribution of the model for a variety of non-trivial fitness functions. These results allow us to speak to genetic architecture, i.e., what stationary distributions result from different fitness functions. This paper presents methods for exactly deriving stationary states for finite and infinite populations. This method can be applied to many fitness functions, and we give exact calculations for four of these. These results allow us to investigate metastability, tradeoffs between fitness functions, and even consider error-correcting codes