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611.
Using a density matrix approach, we study the simplest systems that display both gain and feedback: clusters of 2 to 5 atoms, one of which is pumped. The other atoms supply feedback through multiple scattering of light. We show that, if the atoms are in each other's near field, the system exhibits large gain narrowing and spectral mode redistribution. The observed phenomena are more pronounced if the feedback is enhanced. Our system is to our knowledge the simplest exactly solvable microscopic system which shows the approach to laser oscillation. 相似文献
612.
Georgieva I Trendafilova N Aquino AJ Lischka H 《The journal of physical chemistry. A》2007,111(1):127-135
TDDFT, RI-CC2, and CIS calculations have been performed for the nondissociative excited-state proton transfer (ESPT) in the S1 state of 7-hydroxy-4-methylcoumarin (7H4MC) along a H-bonded water wire of three water molecules bridging the proton donor (OH) and the proton acceptor (C[double bond]O) groups (7H4MC.(H2O)3). The observed structural reorganization in the water-wire cluster is interpreted as a proton-transfer (PT) reaction along the H2O solvent wire. The shift of electron density within the organic chromophore 7H4MC due to the optical excitation appears to be the driving force for ESPT. All the methods used show that the reaction path occurs in the 1pipi* state, and no crossing with a Rydberg-type 1pisigma* state is found. TDDFT and RI-CC2 calculations predict an exoergic reaction of the excited-state enol-to-keto transformation. The S1 potential energy curve reveals well-defined Cs minima of enol- and keto-clusters, separated by a single barrier with a height of 17-20 kcal/mol. After surmounting this barrier, spontaneous PT along the water wire is observed, leading without any further barrier to the keto structure. The TDDFT and RI-CC2 methods appear to be reliable approaches to describe the energy surfaces of ESPT. The CIS method predicts an endoergic ESPT reaction and an energy barrier, which is too high. 相似文献
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615.
Dr. Ciril Jimeno Dr. Ute Christmann Eduardo C. Escudero‐Adán Prof. Ramon Vilar Prof. Miquel A. Pericàs 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(51):16510-16516
Combined spectroscopic, crystallographic, and kinetic studies of the mechanism of aromatic amination with the efficient dinuclear Pd precatalyst [Pd2Cl(μ‐Cl)PtBu2(Bph‐Me)] (Bph‐Me=2′‐methyl‐[1,1′‐biphenyl]‐2‐yl) have revealed overlapping, yet cooperative, mechanistic scenarios, the relative weights of which are strongly influenced by the products formed as the reaction proceeds. The stability and evolution of the precatalyst in solution has been studied and several metalation pathways that point to a single monoligated intermediate have been identified. Our work sheds light on the nature of the catalytic species involved in the process and on the structure of the corresponding catalytic network. 相似文献
616.
Existence results for periodic solutions of integro-dynamic equations on time scales 总被引:1,自引:0,他引:1
Using the topological degree method and Schaefer’s fixed point theorem, we deduce the existence of periodic solutions of nonlinear
system of integro-dynamic equations on periodic time scales. Furthermore, we provide several applications to scalar equations,
in which we develop a time scale analog of Lyapunov’s direct method and prove an analog of Sobolev’s inequality on time scales
to arrive at a priori bound on all periodic solutions. Therefore, we improve and generalize the corresponding results in Burton
et al. (Ann Mat Pura Appl 161:271–283, 1992)
相似文献
617.
N Probst A Madarász A Valkonen I Pápai K Rissanen A Neuvonen PM Pihko 《Angewandte Chemie (International ed. in English)》2012,51(34):8495-8499
Hold them tight: Guided by X-ray structures, bifunctional thiourea catalysts containing an activating intramolecular hydrogen bond were redesigned. The new catalysts were used to effect a highly enantioselective Mannich reaction between malonates and both aliphatic and aromatic imines (see scheme; Boc=tert-butoxycarbonyl). 相似文献
618.
Anton Bovier Véronique Gayrard Adéla Švejda 《Probability Theory and Related Fields》2013,157(1-2):251-283
This paper extends recent results on ageing in mean field spin glasses on short time scales, obtained by Ben Arous and Gün (Commun Pure Appl Math 65:77–127, 2012) in law with respect to the environment, to results that hold almost surely, respectively in probability, with respect to the environment. It is based on the methods put forward in (Gayrard in Aging in reversible dynamics of disordered systems. II. Emergence of the arcsine law in the random hopping time dynamics of the REM, 2010; Electron J Probab 17(58): 1–33, 2012) and naturally complements (Bovier and Gayrard in Ann Probab, 2012). 相似文献
619.
There are some contradictions in the literature on the structure of micelles formed by the BRIJ-35 surfactant in water. One can find reasonable differences in the aggregation numbers and micellar sizes, but there is a lack of data on the intermicellar structure. In this study, we reevaluated the small-angle neutron scattering experiments performed previously on the BRIJ-35 surfactant in the concentration range of 5-200 g/dm3 at 20, 40, and 60 degrees C. The data were analyzed with a reverse Monte Carlo-type method developed recently for colloids. The micelles were modeled as spherical cores representing the hydrophobic parts and number of balls put on the cores to mimic the hydrated hydrophilic chains. The simulations provided data on the mean aggregation number and on the extent of hydration of the hydrophilic shell of the micelles. We obtained intermicellar pair-correlation functions indicating different micelle-micelle interactions from the usually assumed hard-sphere ones. 相似文献
620.
We show that time-independent scattering coefficients calculated from the standard extrapolation of Mie theory to the gain regime have physical meaning up to the laser threshold. The theoretical width of a resonance decreases linearly with increasing gain and becomes zero at the laser threshold. We performed experiments on dielectric microspheres with gain, trapped with optical tweezers. The width of the mode was measured to narrow as a function of the gain up to the lasing threshold, confirming both the validity of the extrapolation of Mie theory to the gain regime below threshold and our interpretation of its point of divergence as the laser threshold. 相似文献