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51.
Piermaria Pinter Christoph M. Schüßlbauer Fabian A. Watt Nicole Dickmann Regine Herbst-Irmer Bernd Morgenstern Annette Grünwald Tobias Ullrich Michael Zimmer Stephan Hohloch Dirk M. Guldi Dominik Munz 《Chemical science》2021,12(21):7401
We report on the convenient synthesis of a CNC pincer ligand composed of carbazole and two mesoionic carbenes, as well as the corresponding lithium- and magnesium complexes. Mono-deprotonation affords a rare “naked” amide anion. In contrast to the proligand and its mono-deprotonated form, tri-deprotonated s-block complexes show bright luminescence, and their photophysical properties were therefore investigated by absorption- and luminescence spectroscopy. They reveal a quantum yield of 16% in solution at ambient temperature. Detailed quantum-chemical calculations assist in rationalizing the emissive properties based on an Intra-Ligand-Charge-Transfer (ILCT) between the carbazolido- and mesoionic carbene ligands. (Earth-)alkali metals prevent the distortion of the ligand following excitation and, thus, by avoiding non-radiative deactivation support bright luminescence.Lithium- and magnesium complexes of a CNC pincer ligand composed of carbazole and two mesoionic carbenes are bright luminescent, because the metals prevent molecular distortions upon excitation. 相似文献
52.
K. M. Munz 《Zeitschrift für Physik B Condensed Matter》1991,84(3):393-396
The dc and ac conductivity of a tunneling junction between two impure quasi-one-dimensional charge density wave (CDW) systems is calculated. The non-magnetic impurities are considered in the self-consistent Born approximation (SCBA). Impurities modify the density of states (DOS) of the pure CDW system for quasiparticles inside the energy region of the gap 2(T). As in the pure case, the theory predicts in addition to a tunneling current which is proportional to the product of the DOS a term proportional to the cosine of the order parameter phase difference. In the case of a normal state/CDW junction, analytical expressions are obtained forT=0 showing deviations from the pure case. The linear ac conductivity is obtained by the scaling relation between the dc and the ac response. 相似文献
53.
R. M. Sandstedt W. J. Eva W. F. Geddes B. Frisell M. J. Blish M. M. Rainess A. I. Krupkin L. Reimers L. Karácsonyi E. Unna D. K. Mecham C. E. Bode C. O. Swanson E. Munz C. H. Bailey L. H. Bailey Fr. Láska B. Rund P. A. Wawilin B. I. Rudoschewskaja G. A. Weiss A. L. Schinkarenko W. A. Ignatowitsch P. Glassmann J. Kantorer W. Whale 《Analytical and bioanalytical chemistry》1939,116(7-8):256-261
54.
Wagner T Kohl CD Morandi S Malagù C Donato N Latino M Neri G Tiemann M 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(26):8216-8223
A model is proposed for the drop in electronic resistance of n-type semiconducting indium oxide (In(2)O(3)) upon illumination with light (350?nm, 3.5?eV) as well as for the (light-enhanced) sensitivity of In(2)O(3) to oxidizing gases. Essential features of the model are photoreduction and a rate-limiting oxygen-diffusion step. Ordered, mesoporous In(2)O(3) with a high specific surface area serves as a versatile system for experimental studies. Analytical techniques comprise conductivity measurements under a controlled atmosphere (synthetic air, pure N(2)) and temperature-resolved in-situ Fourier transform infrared (FTIR) spectroscopy. IR measurements reveal that oxygen vacancies form a donor level 0.18?eV below the conduction band. 相似文献
55.
Coupling of compressible and incompressible flow regions using the multiple pressure variables approach
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Markus Boger Felix Jaegle Rupert Klein Claus‐Dieter Munz 《Mathematical Methods in the Applied Sciences》2015,38(3):458-477
In many cases, multiphase flows are simulated on the basis of the incompressible Navier–Stokes equations. This assumption is valid as long as the density changes in the gas phase can be neglected. Yet, for certain technical applications such as fuel injection, this is no longer the case, and at least the gaseous phase has to be treated as a compressible fluid. In this paper, we consider the coupling of a compressible flow region to an incompressible one based on a splitting of the pressure into a thermodynamic and a hydrodynamic part. The compressible Euler equations are then connected to the Mach number zero limit equations in the other region. These limit equations can be solved analytically in one space dimension that allows to couple them to the solution of a half‐Riemann problem on the compressible side with the help of velocity and pressure jump conditions across the interface. At the interface location, the flux terms for the compressible flow solver are provided by the coupling algorithms. The coupling is demonstrated in a one‐dimensional framework by use of a discontinuous Galerkin scheme for compressible two‐phase flow with a sharp interface tracking via a ghost‐fluid type method. The coupling schemes are applied to two generic test cases. The computational results are compared with those obtained with the fully compressible two‐phase flow solver, where the Mach number zero limit is approached by a weakly compressible fluid. For all cases, we obtain a very good agreement between the coupling approaches and the fully compressible solver. Copyright © 2014 John Wiley & Sons, Ltd. 相似文献
56.
Tobias Ullrich Piermaria Pinter Julian Messelberger Philipp Haines Ramandeep Kaur Max M. Hansmann Dominik Munz Dirk M. Guldi 《Angewandte Chemie (International ed. in English)》2020,59(20):7906-7914
Herein, we present a new class of singlet fission (SF) materials based on diradicaloids of carbene scaffolds, namely cyclic (alkyl)(amino)carbenes (CAACs). Our modular approach allows the tuning of two key SF criteria: the steric factor and the diradical character. In turn, we modified the energy landscapes of excited states in a systematic manner to accommodate the needs for SF. We report the first example of intermolecular SF in solution by dimer self‐assembly at cryogenic temperatures. 相似文献
57.
The second-order accurate LaxWendroff scheme is basedon the first three terms of a Taylor expansion in time in whichthe time derivatives are replaced by space derivatives usingthe governing evolution equations. The space derivatives arethen approximated by central differencing. In this paper, weextend this idea and truncate the Taylor expansion at an arbitraryorder. One main building block is the so-called CauchyKovalevskayaprocedure to replace all the time derivatives by space derivativeswhich can be formulated for a general system of linear equationswith arbitrary order and in two- or three-space dimensions.The linear case is the main focus of this paper because theproposed high-order schemes are good candidates for the approximationof linear wave motion over long distances and times with importantapplications in aeroacoustics and electromagnetics. The stabilityand the efficiency of LaxWendroff-type schemes are examined.The numerical results are compared with a standard scheme foraeroacoustical applications with respect to their quality andthe computational effort. The extensions of the schemes to generalgrids, nonconstant and nonlinear cases are alsoaddressed. 相似文献
58.
The deformability of red blood cells (RBCs) is an important property that allows the cells to squeeze through small capillary vessels and can be used as an indicator for disease. We present a microfluidic based technique to quantify the deformability of RBCs by stretching a collection of RBCs on a timescale of tens of microseconds in a microfluidic chamber. This confinement constrains the motion of the cell to the imaging plane of the microscope during a transient cavitation bubble event generated with a focused and pulsed laser. We record and analyze the shape recovery of the cells with a high-speed camera and obtain a power law in time, consistent with other dynamic rheological results of RBCs. The extracted exponents are used to characterize the elastic properties of the cells. We obtain statistically significant differences of the exponents between populations of untreated RBCs and RBCs treated with two different reagents: neuraminidase reduces the cell rigidity, while wheat germ agglutinin stiffens the cell confirming previous experiments. This cavitation based technique is a candidate for high-throughput screening of elastic cell properties because many cells can be probed simultaneously in situ, thus with no pre-treatment. 相似文献
59.
60.
Sadig Aghazada Matthias Miehlich Julian Messelberger Frank W. Heinemann Dominik Munz Karsten Meyer 《Angewandte Chemie (International ed. in English)》2019,58(51):18547-18551
A novel method for the N?N bond cleavage of trimethylsilyl diazomethane is reported for the synthesis of terminal nitride complexes. The lithium salt of trimethylsilyl diazomethane was used to generate a rare terminal nitrilimine transition metal complex with partially occupied d‐orbitals. This iron complex 2 was characterized by CHN combustion analysis, 1H and 13C NMR spectroscopic analysis, single‐crystal X‐ray crystallography, SQUID magnetometry, 57Fe Mössbauer spectroscopy, and computational analysis. The combined results suggest a high‐spin d 6 (S=2) electronic configuration and an allenic structure of the nitrilimine ligand. Reduction of 2 results in release of the nitrilimine ligand and formation of the iron(I) complex 3 , which was characterized by CHN combustion analysis, 1H NMR spectroscopic analysis, and single‐crystal X‐ray crystallography. Treatment of 2 with fluoride salts quantitatively yields the diamagnetic FeIV nitride complex 4 , with concomitant formation of cyanide and trimethylsilyl fluoride through N?N bond cleavage. 相似文献