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941.
Models of surface enhancement of molecular electronic response properties are challenging for two reasons: (a) molecule-surface interactions require a simultaneous solution of the molecular and the surface dynamic response (a daunting task), and (b) when solving for the electronic structure of the combined molecule + surface system, it is not trivial to single out the particular physical effects responsible for enhancement. To tackle this problem, in this work, we apply a formally exact decomposition of the system's response function into subsystem contributions by using subsystem density functional theory (DFT), which grants access to dynamic polarizabilities and optical spectra. In order to access information about the interactions between the subsystems, we extend a previously developed subsystem-based adiabatic connection fluctuation-dissipation theorem of DFT to separate the additive from the nonadditive correlation energy and identify the nonadditive correlation as the van der Waals interactions. As an example, we choose benzene adsorbed on monolayer MoS2. We isolate the contributions to benzene's dynamic response arising from the interaction with the surface, and for the first time, we evaluate the enhancements to the effectiveness of C6 coefficients as a function of benzene-MoS2 distance and adsorption site. We also quantify the spectral broadening of the benzene's electronic excited states due to their interaction with the surface. We find that the broadening has a similar decay law with the molecule-surface distance as the leading van der Waals interactions (ie, R−6 ) and that the surface enhancement of dispersion interactions between benzene molecules is less than 5% but is still large enough (0.5 kcal/mol) to likely play a role in the prediction of interface morphologies. 相似文献
942.
Christian T. McHugh Phillip G. Durham Michele Kelley Prof. Paul A. Dayton Prof. Rosa T. Branca 《Chemphyschem》2021,22(12):1219-1228
Gas microbubbles are an established clinical ultrasound contrast agent. They could also become a powerful magnetic resonance (MR) intravascular contrast agent, but their low susceptibility-induced contrast requires high circulating concentrations or the addition of exogenous paramagnetic nanoparticles for MR detection. In order to detect clinical in vivo concentrations of raw microbubbles via MR, an alternative detection scheme must be used. HyperCEST is an NMR technique capable of indirectly detecting signals from very dilute molecules (concentrations well below the NMR detection threshold) that exchange hyperpolarized 129Xe. Here, we use quantitative hyperCEST to show that microbubbles are very efficient hyperCEST agents. They can accommodate and saturate millions of 129Xe atoms at a time, allowing for their indirect detection at concentrations as low as 10 femtomolar. The increased MR sensitivity to microbubbles achieved via hyperCEST can bridge the gap for microbubbles to become a dual modality contrast agent. 相似文献
943.
Journal of Statistical Physics - We consider self-propelled particles confined between two parallel plates, moving with a constant velocity while their moving direction changes by rotational... 相似文献
944.
In this paper we show how techniques coming from stochastic analysis, such as stochastic completeness (in the form of the weak maximum principle at infinity), parabolicity and L p -Liouville type results for the weighted Laplacian associated to the potential may be used to obtain triviality, rigidity results, and scalar curvature estimates for gradient Ricci solitons under L p conditions on the relevant quantities. 相似文献
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948.
In correspondence with the manifolds of quasi-constant sectional curvature defined (cf [5], [9]) in the Riemannian context,
we introduce in the K?hlerian framework the geometric notion of quasi-constant holomorphic sectional curvature. Some characterizations
and properties are given. We obtain necessary and sufficient conditions for these manifolds to be locally symmetric, Ricci
or Bochner flat, K?hler η-Einstein or K?hler-Einstein, etc. The characteristic classes are studied at the end and some examples are provided throughout.
相似文献
949.
Chancel und Landwirthschaftliche Versuchsstation San Michele 《Fresenius' Journal of Analytical Chemistry》1893,32(1):116-117
Ohne Zusammenfassung 相似文献
950.