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Dendritic and fractal patterns in electrolytic metal deposits 总被引:1,自引:0,他引:1
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In this B3 LYP model study, homoleptic nickel(0) ethyne complexes have been predicted as the catalyst resting state for the title reaction. Ethyne ligand coupling of Ni(C(2)H(2))(3) yields monoethyne nickelacyclopentadiene in the rate-determining step. Ethyne coordination is followed by insertion of an ethyne ligand into the Ni--C sigma bond. A highly strained monoethyne trans-nickelacycloheptatriene is formed. This trans intermediate is unable to reductively eliminate benzene without prior isomerization to a cis-structure. Instead, it rapidly collapses to a nickelacyclononatetraene. Ethyne coordination induces reductive elimination to the cyclooctatetraene complex Ni(eta(2)-C(2)H(2))(eta(2)-C(8)H(8)), followed by facile ligand exchange. Other ethyne coupling pathways have been computed to be less favored. The cyclooctatetraene ligand binds significantly weaker to nickel(0) than ethyne, both for mononuclear, and for dinuclear species. For this reason, C--C bond formation steps at Ni(2)(micro-cot) fragments have been predicted to feature prohibitively high overall reaction barriers. 相似文献
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The curvature field is measured from tracer-particle trajectories in a two-dimensional fluid flow that exhibits spatiotemporal chaos and is used to extract the hyperbolic and elliptic points of the flow. These special points are pinned to the forcing when the driving is weak, but wander over the domain and interact in pairs at stronger driving, changing the local topology of the flow. Their behavior reveals a two-stage transition to spatiotemporal chaos: a gradual loss of spatial and temporal order followed by an abrupt onset of topological changes. 相似文献
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Nordstrom KN Verneuil E Arratia PE Basu A Zhang Z Yodh AG Gollub JP Durian DJ 《Physical review letters》2010,105(17):175701
The rheology near jamming of a suspension of soft colloidal spheres is studied using a custom microfluidic rheometer that provides the stress versus strain rate over many decades. We find non-Newtonian behavior below the jamming concentration and yield-stress behavior above it. The data may be collapsed onto two branches with critical scaling exponents that agree with expectations based on Hertzian contacts and viscous drag. These results support the conclusion that jamming is similar to a critical phase transition, but with interaction-dependent exponents. 相似文献
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We present a modified optimal control scheme based on the Krotov method, which allows for strict limitations on the spectrum of the optimized laser fields. A frequency constraint is introduced and derived mathematically correct, without losing monotonic convergence of the algorithm. The method guarantees a close link to learning loop control experiments and is demonstrated for the challenging control of nonresonant Raman transitions, which are used to implement a set of global quantum gates for molecular vibrational qubits. 相似文献
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By extending traditional particle tracking techniques, we study the dynamics of neutrally buoyant finite-sized particles in a spatiotemporally chaotic flow. We simultaneously measure the flow field and the trajectories of millimeter-scale particles so that the two can be directly compared. While the single-point statistics of the particles are indistinguishable from the flow statistics, the particles often move in directions that are systematically different from the underlying flow. These differences are especially evident when Lagrangian statistics are considered. 相似文献