There is fundamental interest in understanding the coupled nuclear and electronic dynamics associated with charge transfer processes in complex molecules and materials, which are often mediated by electron, electron hole or proton motion. With dramatic improvements in the techniques to generate extreme ultraviolet (XUV) and X-ray femtosecond pulses, it now becomes possible to trigger and probe these kinds of processes in real time. Here we study the dynamics of an electron hole created by photoionization in the valence shell of protonated water clusters H(+)(H(2)O)(n). We demonstrate that the electron hole is strongly correlated with the protons forming the hydrogen bond network. We show that it is possible to probe key aspects of the valence electron hole dynamics and the coupled nuclear motion with femtosecond time resolution by resonantly exciting K-shell 1s electrons to fill the electron hole. This represents an opportunity for X-ray transient absorption spectroscopy.
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http://dx.doi.org/10.1039/c4fd00078a | DOI Listing |
Dalton Trans
January 2025
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518060, P. R. China.
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO/CoO, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO and CoO layers ALD, which enhances electron-hole pair separation and minimizes their recombination.
View Article and Find Full Text PDFAdv Mater
January 2025
National & Local Joint Engineering Research Center for High-efficiency Display and Lighting Technology, Key Lab for Special Functional Materials of Ministry of Education, School of Nanoscience and Materials Engineering, Henan University, Kaifeng, 475004, China.
The poor efficiency and stability of blue Quantum Dot Light-Emitting diodes (QLED) hinders the practical applications of QLEDs full-color displays. Excessive electron injection, insufficient hole injection, and abundant defects on the surface of quantum dots (QD) are the main issues limiting the performance of blue devices. Herein, an in situ treatment with bipolar small molecule polydentate ligand-guanidine chloride (GACl) is proposed to simultaneously suppress excessive electron injection, patch surface defects of QDs and enhance hole injection.
View Article and Find Full Text PDFChem Sci
January 2025
School of Chemistry and Chemical Engineering, Shandong University Jinan 250100 PR China
Noncovalent forces have a significant impact on photophysical properties, and the flexible employment of weak forces facilitates the design of novel luminescent materials with a variety of applications. The arene-perfluoroarene (AP) force, as one type of π-hole/π interaction, shows unique directionality, involving an electron-deficient π-hole interacting with a π-electron-rich region, facilitating precise orientation and stabilization in supramolecular structures. Here we present an amination engineering protocol to build a perfluoroarene library based on an octafluoronaphthalene skeleton with various steric and electronic properties.
View Article and Find Full Text PDFNat Commun
January 2025
Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden.
One of the key advantages of perovskite light-emitting diodes (PeLEDs) is their potential to achieve high performance at much higher current densities compared to conventional solution-processed emitters. However, state-of-the-art PeLEDs have not yet reached this potential, often suffering from severe current-efficiency roll-off under intensive electrical excitations. Here, we demonstrate bright PeLEDs, with a peak radiance of 2409 W sr m and negligible current-efficiency roll-off, maintaining high external quantum efficiency over 20% even at current densities as high as 2270 mA cm.
View Article and Find Full Text PDFCarbohydr Polym
March 2025
College of Food Science and Engineering, Northwest A&F University, Yangling 712100, Shaanxi, China; School of Chemistry, Guangzhou Key Laboratory of Analytical Chemistry for Biomedicine, South China Normal University, Guangzhou 510006, China. Electronic address:
The management of wounds infected with drug-resistant bacteria represents a significant challenge to public health globally. Nanotechnology-functionalized photothermal hydrogel with good thermal stability, biocompatibility and tissue adhesion exhibits great potential in treating these infected wounds. Herein, a novel photothermal hydrogel (mCS-Cu-Ser) was prepared through in situ mineralization in the hydrogel networks and ion cross-linking driven by copper ions (∼3 mM).
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