A detailed analysis of ptychography for three-dimensional (3D) phase reconstructions of thick specimens is performed. We introduce multi-focus ptychography, which incorporates a 4D-STEM defocus series to enhance the quality of 3D reconstructions along the beam direction through a higher overdetermination ratio. This method is compared with established multi-slice ptychography techniques, such as conventional ptychography, regularized ptychography, and multi-mode ptychography.
View Article and Find Full Text PDFCovalent organic frameworks (COFs) containing well-defined redox-active groups have become competitive materials for next-generation batteries. Although high potentials and rate performance can be expected, only a few examples of p-type COFs have been reported for charge storage to date with even fewer examples on the use of COFs in multivalent ion batteries. Herein, we report the synthesis of a p-type highly porous and crystalline azatruxene-based COF and its application as a positive electrode material in Li- and Mg-based batteries.
View Article and Find Full Text PDFAntiaromaticity is a fundamental concept in chemistry, but the study of molecular wires incorporating antiaromatic units is limited. Despite initial predictions, very few studies show that antiaromaticity has a beneficial effect on electron transport. Dibenzo[a,e]pentalene (DBP) is a stable structure that displays appreciable antiaromaticity within the five-membered rings of the pentalene core.
View Article and Find Full Text PDFAntiferromagnets hosting structural or magnetic order that breaks time reversal symmetry are of increasing interest for "beyond von Neumann" computing applications because the topology of their band structure allows for intrinsic physical properties, exploitable in integrated memory and logic function. One such group are the noncollinear antiferromagnets. Essential for domain manipulation is the existence of small net moments found routinely when the material is synthesized in thin film form and attributed to symmetry breaking caused by spin canting, either from the Dzyaloshinskii-Moriya interaction or from strain.
View Article and Find Full Text PDFLocally aromatic alkyl--substituted squarephaneic tetraimide (SqTI) conjugated macrocycles are four-electron reducible, owing to global aromaticity and presumed global Baird aromaticity of the dianion and tetraanion states, respectively. However, their good solubility inhibits their application as a battery electrode material. By applying sidechain removal as a strategy to reduce SqTI solubility, we report the development of its unsubstituted derivative SqTI-H, which was obtained directly from squarephaneic tetraanhydride by facile treatment with hexamethyldisilazane and MeOH.
View Article and Find Full Text PDFDiamond's unique properties on the nanoscale make it one of the most important materials for use in biosensors and quantum computing and for components that can withstand the harsh environments of space. We synthesize oriented, faceted diamond particles by flash laser heating of glassy carbon at 16 GPa and 2300 K. Detailed transmission electron microscopy shows them to consist of a mosaic of diamond nanocrystals frequently joined at twin boundaries forming microtwins.
View Article and Find Full Text PDFOrganic battery electrode materials offer the unique opportunity for full cells to operate in an anion-rocking chair mode. For this configuration a pair of p-type redox-active electrode materials is required with a substantial potential gap between their redox processes. We herein investigate viologen-functionalized polystyrenes as negative electrode paired with a phenothiazine polymer as positive electrode in all-organic full cells.
View Article and Find Full Text PDFWith their bent π-systems, cyclic conjugation and inherent cavities, conjugated nanohoops are attractive for organic electronics applications. For ease of processing and morphological stability, an incorporation into polymers is desirable, but to date was hampered with few exceptions by synthetic difficulties. We herein present a unique strategy for the synthesis of conjugated nanohoop polymers using a dibenzo[a,e]pentalene (DBP) as central connector.
View Article and Find Full Text PDFSustainable battery concepts are of great importance for the energy storage demands of the future. Organic batteries based on redox-active polymers are one class of promising storage systems to meet these demands, in particular when combined with environmentally friendly and safe electrolytes. Deep Eutectic Solvents (DESs) represent a class of electrolytes that can be produced from sustainable sources and exhibit in most cases no or only a small environmental impact.
View Article and Find Full Text PDFIntegrated, on-chip lasers are vital building blocks in future optoelectronic and nanophotonic circuitry. Specifically, III-V materials that are of technological relevance have attracted considerable attention. However, traditional microcavity laser fabrication techniques, including top-down etching and bottom-up catalytic growth, often result in undesirable cavity geometries with poor scalability and reproducibility.
View Article and Find Full Text PDFObjective: Digital health applications can be prescribed since 2019 in Germany, which is likely to facilitate a broad use of epilepsy self-management applications, possibly directly connected to clinical systems via telematics infrastructures. This article reports on patients' interest in digital support for epilepsy self-management, influencing factors and patients' knowledge about digitization of health care in Germany.
Methods: This work is based on self-reported data from 115 people with epilepsy participating in an anonymous online survey with a total of 54 questions covering several topics, including sociodemographics and epilepsy manifestation, use of technology in general and for treatment support, training programs, affinity for technology, knowledge on the digital infrastructure in Germany, and self-efficacy in dealing with chronic illness.
Organic electrode materials based on conjugated dicarboxylate moieties are particularly attractive to develop metal-ion organic batteries. Exhibiting good stability properties in liquid electrolytes, such organic electrode materials can reversibly store alkali metal ions (Li, Na or K) at low working potential. Although many molecular designs have been investigated in the last decade, conjugated dicarboxylates are impeded by low coulombic efficiencies, especially at the first cycle, and sluggish kinetics in most cases.
View Article and Find Full Text PDFDespite their inherent instability, 4 π systems have recently received significant attention due to their unique optical and electronic properties. In dibenzopentalene (DBP), benzanellation stabilizes the highly antiaromatic pentalene core, without compromising its amphoteric redox behavior or small HOMO-LUMO energy gap. However, incorporating such molecules in organic devices as discrete small molecules or amorphous polymers can limit the performance (e.
View Article and Find Full Text PDFThe increasing energy demand for diverse applications requires new types of devices and materials. Multifunctional materials that can fulfill different roles are of high interest as they can allow fabricating devices that can both convert and store energy. Herein, organic donor-acceptor redox polymers that can function as charge storage materials in batteries and as donor materials in bulk heterojunction (BHJ) photovoltaic devices are investigated.
View Article and Find Full Text PDFScanning transmission electron microscopy (STEM) has a broad range of applications in materials characterization, including real-space imaging, spectroscopy, and diffraction, at length scales from the micron to sub-Ångström. The recent development and adoption of high-speed, direct electron STEM detectors has enabled diffraction patterns to be collected at each probe position, generating four-dimensional STEM (4D-STEM) datasets and opening new imaging modalities. However, the limited pixel numbers in these detectors enforce a tradeoff between angular resolution and maximum collection angle.
View Article and Find Full Text PDFConjugated nanohoops incorporating nonalternant hydrocarbons have altered optoelectronic properties compared to []cycloparaphenylenes or other purely aromatic hoops. We synthesized []cyclo-1,5-dibenzopentalenes ( = 4, 5), in which nonalternant dibenzo[,]pentalenes are connected through their pentalene units. This leads to an increase in antiaromatic character and low-lying LUMO energies.
View Article and Find Full Text PDFCharge-transfer emitters are attractive due to their color tunability and potentially high photoluminescence quantum yields (PLQYs). We herein present tetraaminospirenes as donor moieties, which, in combination with a variety of acceptors, furnished 12 charge-transfer emitters with a range of emission colors and PLQYs of up to 99 %. The spatial separation of their frontier molecular orbitals was obtained through careful structural design, and two DA structures were confirmed by X-ray crystallography.
View Article and Find Full Text PDFChem Commun (Camb)
September 2021
The efficiency of the photo-induced electron transfer in photoredox catalysis is limited by the diffusional collision of the excited catalyst and the substrate. We herein present cavity-bound photoredox catalysts, which preassociate the substrates, leading to significantly shortened reaction times. A pillar[5]arene serves as the cavity and phenothiazine as a catalyst in the reductive dehalogenation of aliphatic bromides as a proof of concept reaction.
View Article and Find Full Text PDFStrained conjugated nanohoops are attractive synthetic targets due to the bending of their π-system, which leads to intriguing optoelectronic properties, among others. By incorporating non-mirror-symmetric aromatic panels, chiral nanohoops can be obtained. We herein present a strategy to enantiopure nanohoops by racemic resolution through chiral derivatization of diketone-embedded hoops.
View Article and Find Full Text PDFConjugated nanohoops provide a platform to study structure-property relationships; they are attractive hosts for supramolecular chemistry as well as promising candidates as new organic materials. We herein present []cyclodibenzopentalenes ([]CDBPs) as antiaromatic analogues of []cycloparaphenylenes. Platinum-mediated macrocyclization of dibenzopentalene boronic esters provided the trimer and tetramer with strain energies of up to 80 kcal mol.
View Article and Find Full Text PDFWe have developed and implemented an undergraduate microbiology course in which students isolate, characterize, and perform whole genome assembly and analysis of from stream sediments and poultry litter. In the development of the course and over three semesters, successive teams of undergraduate students collected field samples and performed enrichment and isolation techniques specific for the detection of . Eighty-eight strains were confirmed using standard microbiological methods and PCR of the gene.
View Article and Find Full Text PDFOrganic redox polymers are attractive electrode materials for more sustainable rechargeable batteries. To obtain full-organic cells with high operating voltages, redox polymers with low potentials (<2 V versus Li|Li ) are required for the negative electrode. Dibenzo[a,e]cyclooctatetraene (DBCOT) is a promising redox-active group in this respect, since it can be reversibly reduced in a two-electron process at potentials below 1 V versus Li|Li .
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