The capability to study the dynamic formation of plasmonic molecular junction is of fundamental importance, and it will provide new insights into molecular electronics/plasmonics, single‐entity electrochemistry, and nanooptoelectronics. Here, a facile method to form plasmonic molecular junctions is reported by utilizing single gold nanoparticle (NP) collision events at a highly curved gold nanoelectrode modified with a self‐assembled monolayer. By using time‐resolved electrochemical current measurement and surface‐enhanced Raman scattering spectroscopy, the current changes and the evolution of interfacial chemical bonding are successfully observed in the newly formed molecular tunnel junctions during and after the gold NP “hit‐n‐stay” and “hit‐n‐run” collision events. The results lead to an in‐depth understanding of the single NP motion and the associated molecular level changes during the formation of the plasmonic molecular junctions in a single NP collision event. This method also provides a new platform to study molecular changes at the single molecule level during electron transport in a dynamic molecular tunnel junction. 相似文献
Ultraviolet (UV) light can be used in versatile applications ranging from photoelectronic devices to biomedical imaging. In the development of new UV light sources, in this study, stable UV emission at ≈350 nm is unprecedentedly obtained from carbon nanospheres (CNSs). The origin of the UV fluorescence is comprehensively investigated via various characterization methods, including Raman and Fourier transform infrared analyses, with comparison to the visible emission of carbon nanodots. Based on the density functional calculations, the UV fluorescence is assigned to the carbon nanostructures bonded to bridging O atoms and dangling –OH groups. Moreover, a twofold enhancement in the UV emission is acquired for Au‐carbon core‐shell nanospheres (Au‐CNSs). This remarkable modification of the UV emission is primarily ascribed to charge transfer between the CNSs and the Au surface. 相似文献
Nickel-iron layered double hydroxide (NiFe-LDH) nanosheets have shown optimal oxygen evolution reaction (OER) performance; however, the role of the intercalated ions in the OER activity remains unclear. In this work, we show that the activity of the NiFe-LDHs can be tailored by the intercalated anions with different redox potentials. The intercalation of anions with low redox potential (high reducing ability), such as hypophosphites, leads to NiFe-LDHs with low OER overpotential of 240 mV and a small Tafel slope of 36.9 mV/dec, whereas NiFe-LDHs intercalated with anions of high redox potential (low reducing ability), such as fluorion, show a high overpotential of 370 mV and a Tafel slope of 80.8 mV/dec. The OER activity shows a surprising linear correlation with the standard redox potential. Density functional theory calculations and X-ray photoelectron spectroscopy analysis indicate that the intercalated anions alter the electronic structure of metal atoms which exposed at the surface. Anions with low standard redox potential and strong reducing ability transfer more electrons to the hydroxide layers. This increases the electron density of the surface metal sites and stabilizes their high-valence states, whose formation is known as the critical step prior to the OER process.
The median graph has been shown to be a good choice to obtain a representative of a set of graphs. However, its computation is a complex problem. Recently, graph embedding into vector spaces has been proposed to obtain approximations of the median graph. The problem with such an approach is how to go from a point in the vector space back to a graph in the graph space. The main contribution of this paper is the generalization of this previous method, proposing a generic recursive procedure that permits to recover the graph corresponding to a point in the vector space, introducing only the amount of approximation inherent to the use of graph matching algorithms. In order to evaluate the proposed method, we compare it with the set median and with the other state-of-the-art embedding-based methods for the median graph computation. The experiments are carried out using four different databases (one semi-artificial and three containing real-world data). Results show that with the proposed approach we can obtain better medians, in terms of the sum of distances to the training graphs, than with the previous existing methods. 相似文献
Although there is a debate about whether designers should draw a distinction between perceptual affordances and cultural conventions, there are few behavioral studies. We examined the impact of working memory load and expected button-to-action mapping congruency on affordances and conventions. The findings suggest both sides of the debate are correct. Learned conventions were found to structure responses towards expected actions, just like affordances, but affordance-based interactions were not affected by memory load while convention-based actions were. Therefore, designers ought to employ perceptual affordances when possible and when not feasible they ought to reuse established conventions. Additionally, evidence is presented that violating expected affordance-based and convention-based button-to-action mappings caused a similar performance cost. We believe that after the initial learning period, conventions play a critical role in the perception of a design’s available actions just as perceptual affordances do. 相似文献