The localized surface-plasmon resonance of metal nanoparticles and clusters corresponds to a collective charge oscillation of the quasi-free metal electrons. The polarization of the more localized d electrons opposes the overall polarization of the electron cloud and thus screens the surface plasmon. By contrast, a static electric external field is well screened, as even very small noble-metal clusters are highly metallic: the field inside is practically zero except for the effect of the Friedel-oscillation-like modulations which lead to small values of the polarization of the d electrons. In the present article, we present and compare representations of the induced densities (i) connected to the surface-plasmon resonance and (ii) resulting from an external static electric field. The two cases allow for an intuitive understanding of the differences between the dynamic and the static screening.
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http://dx.doi.org/10.1039/d2cp04316e | DOI Listing |
J Chem Theory Comput
January 2025
Department of Chemistry, Brandeis University, 415 South Street, Waltham, Massachusetts 02453, United States.
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Department of Chemistry, University of Central Florida, Orlando, Florida 32816 (USA).
Understanding the origin of enhanced catalytic activity is critical to heterogeneous catalyst design. This is especially important for non-noble metal-based catalysts, notably metal oxides, which have recently emerged as viable alternatives for numerous thermal catalytic processes. For thermal catalytic reduction/hydrogenation using metal oxide nanoparticles, enhanced catalytic performance is typically attributed to increased surface area and oxygen vacancies.
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School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, Shandong University, Ji'nan, 250100, People's Republic of China.
Developing thermally activated delayed fluorescence (TADF)-active silver clusters with near-unity quantum efficiency is of practical importance in cutting-edge optoelectronic devices, but remains a tremendous challenge due to the difficulty of de novo synthesis and uncertainty of properties. Herein, we demonstrate a lattice modulation on parent TADF- active silver cluster, achieving TADF-driven photoluminescence quantum yield (PLQY) from 12 % to near-unity. Systematic experimental and calculated results reveal that the lattice modulation effectively lowers the singlet-triplet splitting (ΔE) from 718 to 549 cm, thereby facilitating thermally activated reverse intersystem crossing: T→S, leading to extremely efficient TADF by surpassing both phosphorescence and non-radiative decay, thus boosting the near-unity PLQY.
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School of Pharmacy, Shandong Second Medical University, Weifang 261053, China.
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View Article and Find Full Text PDFAngew Chem Int Ed Engl
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State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, 710049, Shaanxi, P.R. China.
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