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111.
Li Zhang Dr. Julie Jung Dr. Peng Zhang Mei Guo Dr. Lang Zhao Prof. Dr. Jinkui Tang Prof. Dr. Boris Le Guennic 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(4):1392-1398
Elaborate chemical design is of utmost importance in order to slow down the relaxation dynamics in single‐molecule magnets (SMMs) and hence improve their potential applications. Much interest was devoted to the study of distinct relaxation processes related to the different crystal fields of crystallographically independent lanthanide ions. However, the assignment of the relaxation processes to specific metal sites remains a challenging task. To address this challenge, a new asymmetric Dy2 SMM displaying a well‐separated two‐step relaxation process with the anisotropic centers in fine‐tuned local environments was elaborately designed. For the first time a one‐to‐one relationship between the metal sites and the relaxation processes was evidenced. This work sheds light on complex multiple relaxation and may direct the rational design of lanthanide SMMs with enhanced magnetic properties. 相似文献
112.
Mikhail N. Feofanov Boris A. Lozhkin Maksim V. Anokhin Alexey D. Averin Irina P. Beletskaya 《Mendeleev Communications》2018,28(4):429-430
Magnesium iodide-catalyzed addition of electron-rich (het)arenes to ethyl glyoxylate proceeds at room temperature with high chemoselectivity to afford ethyl 2-(het)aryl- 2-hydroxyacetates in yields up to 95%. 相似文献
113.
Ludmila A. Oparina Oksana V. Vysotskaya Lidiya N. Parshina Nina K. Gusarova Boris A. Trofimov 《Phosphorus, sulfur, and silicon and the related elements》2013,188(9):2087-2093
Under acid- or base-catalyzed conditions, thiols add regio- and chemos-electively either to vinyloxy or methacrylate group of vinyloxyalkyl-methacrylates to give polyfunctional methacrylates or polyfunctional vinyl ethers, respectively. 相似文献
114.
Nina Gusarova Lambert Brandsma Svetlana Malysheva Svetlana Arbuzova Boris Trofimov 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-4)
Abstract Nucleophilic addition of phosphide anions generated from phosphorus red or phosphine to ethenes and ethynes in the presence of super bases to afford organylphosphines and -oxides has been performed. 相似文献
115.
Dr. Jessica Flores Gonzalez Vincent Montigaud Dr. Vincent Dorcet Dr. Kevin Bernot Dr. Boris Le Guennic Dr. Fabrice Pointillart Prof. Olivier Cador 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(39):10160-10168
Single-Molecule Magnet (SMM) property is by essence molecular, while commonly measured in solid crystalline state. Solvent crystallization molecules are usually neglected in the analysis and interpretation of solid-state properties. The solvation/desolvation process in the polyoxometalate(POM)-based Na9[Er(W5O18)2] ⋅ 35 H2O SMM demonstrates that the dehydrated form relaxes more than 1000 times faster than the initial state, while the rehydration process allows the quasi complete recovering of the initial magnetic behaviour. This dehydration process is monitored by thermogravimetric analysis (TGA) and temperature-dependent X-ray powder diffraction, and rationalized by periodic quantum chemical calculations evidencing the tremendous role of the labile water molecules in the stability of the edifice. Ab-initio calculations highlight that sodium ions localization in the structure drive the magnetic responses. Isotopic enrichment with nuclear spin free (166Er, I=0) ErIII ions shows that the relaxation dynamics in the quantum regime depends on the nuclear spin. 相似文献
116.
This paper considers the formation of dead zones in the porous catalyst pellets due to the chemical reaction and diffusion. We established and investigated the model with nonisothermal reaction of fractional order and activated temperature-dependent diffusivity. The effects of process parameters, catalyst shape, and reaction and diffusion parameters on the formation of the dead zone are studied numerically and characterized by the critical Thiele modulus. The lower bounds for the critical Thiele modulus are derived analytically in terms of process parameters for exothermic and endothermic reactions and verified numerically. The critical Thiele modulus increases with increasing Arrhenius number for diffusion and decreasing Arrhenius number for reaction in the case of exothermic reactions, whereas the opposite trends hold for the endothermic reactions. The critical Thiele modulus also increases with increasing fractional reaction order as well as with decreasing energy generation function, and increasing Biot numbers for heat and mass transfer. Moreover, the critical Thiele modulus is the highest for spherical pellets and the lowest for pellets with planar shape. 相似文献
117.
Dr. Siddhartha De Dr. Alexandrine Flambard Dr. Delphine Garnier Patrick Herson Dr. Frank H. Köhler Dr. Abhishake Mondal Dr. Karine Costuas Dr. Béatrice Gillon Prof. Rodrigue Lescouëzec Dr. Boris Le Guennic Dr. Frédéric Gendron 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(52):12120-12136
The local magnetic structure in the [FeIII(Tp)(CN)3]− building block was investigated by combining paramagnetic Nuclear Magnetic Resonance (pNMR) spectroscopy and polarized neutron diffraction (PND) with first-principle calculations. The use of the pNMR and PND experimental techniques revealed the extension of spin-density from the metal to the ligands, as well as the different spin mechanisms that take place in the cyanido ligands: Spin-polarization on the carbon atoms and spin-delocalization on the nitrogen atoms. The results of our combined density functional theory (DFT) and multireference calculations were found in good agreement with the PND results and the experimental NMR chemical shifts. Moreover, the ab-initio calculations allowed us to connect the experimental spin-density map characterized by PND and the suggested distribution of the spin-density on the ligands observed by NMR spectroscopy. Interestingly, significant differences were observed between the pseudo-contact contributions of the chemical shifts obtained by theoretical calculations and the values derived from NMR spectroscopy using a simple point-dipole model. These discrepancies underline the limitation of the point-dipole model and the need for more elaborate approaches to break down the experimental pNMR chemical shifts into contact and pseudo-contact contributions. 相似文献
118.
Gerold Jäger Changxing Dong Boris Goldengorin Paul Molitor Dirk Richter 《Journal of Heuristics》2014,20(1):107-124
We introduce a reduction technique for large instances of the traveling salesman problem (TSP). This approach is based on the observation that tours with good quality are likely to share many edges. We exploit this observation by neglecting the less important tour space defined by the shared edges, and searching the important tour subspace in more depth. More precisely, by using a basic TSP heuristic, we obtain a set of starting tours. We call the set of edges which are contained in each of these starting tours as pseudo-backbone edges. Then we compute the maximal paths consisting only of pseudo-backbone edges, and transform the TSP instance to another one with smaller size by contracting each such path to a single edge. This reduced TSP instance can be investigated more intensively, and each tour of the reduced instance can be expanded to a tour of the original instance. Combining our reduction technique with the currently leading TSP heuristic of Helsgaun, we experimentally investigate 32 difficult VLSI instances from the well-known TSP homepage. In our experimental results we set world records for seven VLSI instances, i.e., find better tours than the best tours known so far (two of these world records have since been improved upon by Keld Helsgaun and Yuichi Nagata, respectively). For the remaining instances we find tours that are equally good or only slightly worse than the world record tours. 相似文献
119.
Malte Braack Martin F. Quaas Benjamin Tews Boris Vexler 《Journal of Optimization Theory and Applications》2018,178(3):950-972
The behavior of a fishing fleet and its impact onto the biomass of fish can be described by a nonlinear parabolic diffusion–reaction equation. Looking for an optimal fishing strategy leads to a non-convex optimal control problem with a bilinear control action. In this work, we present such an optimal control formulation, prove its well-posedness and derive first- and second-order optimality conditions. These results provide a basis for tailored finite element discretization as well as for Newton type optimization algorithms. First numerical test problems show typical features as so-called No-Take-Zones and maximal fishing quota (total allowable catches) as parts of an optimal fishing strategy. 相似文献
120.
Boris I. Kvasov 《Numerical Algorithms》2014,67(4):863-888
This paper presents methods for shape preserving spline interpolation. These methods are based on discrete weighted cubic splines. The analysis results in two algorithms with automatic selection of the shape control parameters: one to preserve the data monotonicity and other to retain the data convexity. Discrete weighted cubic B-splines and control point approximation are also considered. 相似文献