This paper demonstrates the increased light absorption efficiency of semiconducting atom probe tips resulting from focused-ion-beam (FIB) preparation. We use transmission electron microscopy to show that semiconducting tips prepared with FIB are surrounded with an amorphized shell. Photomodulated optical reflectance measurements then provide evidence that FIB-induced damage leads to an increase in both sub- and supra-bandgap light absorption efficiency. Using laser-assisted atom probe tomography (La-APT) measurements, we finally show that, for a nanoscale tip geometry, the laser-induced heating of a tip during La-APT is enhanced by the FIB preparation. We conclude that, upon supra-bandgap illumination, the presence of a FIB-amorphized surface dramatically increases the light-induced heat generation inside semiconducting tips during La-APT. Furthermore, we also deduce that, in the intriguing case of sub-bandgap illumination, the amorphization plays a crucial role in the unexpected light absorption.
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http://dx.doi.org/10.1016/j.ultramic.2018.03.001 | DOI Listing |
J Am Chem Soc
January 2025
Department of Chemistry, University of Wisconsin─Madison, 1101 University Avenue, Madison, Wisconsin 53706, United States.
The adenosylcobalamin (AdoCbl)-dependent enzyme ethanolamine ammonia-lyase (EAL) catalyzes the conversion of ethanolamine to acetaldehyde and ammonia. As is the case for all AdoCbl-dependent isomerases, the catalytic cycle of EAL is initiated by homolytic cleavage of the cofactor's Co-C bond, producing Cocobalamin (CoCbl) and an adenosyl radical that serves to abstract a hydrogen atom from the substrate. Remarkably, in the presence of substrate, the rate of Co-C bond homolysis of enzyme-bound AdoCbl is increased by 12 orders of magnitude.
View Article and Find Full Text PDFMolecules
December 2024
High & New Technology Research Center of Henan Academy of Sciences, No. 56 Hongzhuan Road, Zhengzhou 450002, China.
A series of colorful binuclear Schiff bases derived from the different diamine bridges including 1,2- ethylenediamine (bis-Et-SA, bis-Et-4-NEt, bis-Et-5-NO, bis-Et-Naph), 1,2-phenylenediamine (bis-Ph-SA, bis-Ph-4-NEt, bis-Ph-5-NO, bis-Ph-Naph), dicyano-1,2-ethenediamine (bis-CN-SA, bis-CN-4-NEt, bis-CN-5-NO, bis-CN-Naph) have been designed and prepared. The optical properties of these binuclear Schiff base ligands were fully determined by UV-Vis absorption spectroscopy, fluorescence emission spectroscopy, and time-dependent-density functional theory (TD-DFT) calculations. The inclusion of D-A systems and/or π-extended systems in these binuclear Schiff base ligands not only enables adjustable RGB light absorption and emission spectra (300~700 nm) but also yields high fluorescence quantum efficiencies of up to 0.
View Article and Find Full Text PDFSci Total Environ
January 2025
Institute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, China; State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Chang Ping, Beijing 102249, China.
The transformation and risk assessment of flavonoids triggered by free radicals deserve extensive attention. In this work, the degradation mechanisms, kinetics, and ecotoxicity of kaempferol and quercetin mediated by ∙OH, ∙OCH, ∙OOH, and O in gaseous and aqueous environments were investigated using cell experiments and quantum chemical calculations. Three radical scavenging mechanisms, including hydrogen atom transfer (HAT), radical adduct formation (RAF) and single electron transfer (SET) were discussed.
View Article and Find Full Text PDFPhys Rev Lett
December 2024
Key Laboratory of Quantum Information, University of Science and Technology of China, Hefei, Anhui 230026, China.
The identification of tipping points is essential for the prediction of collapses or other sudden changes in complex systems. Applications include studies of ecology, thermodynamics, climatology, and epidemiology. However, detecting early signs of proximity to a tipping is made challenging by complexity and nonlinearity.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
December 2024
Department of Chemical Science and Technology, Kunming University, Kunming, Yunnan 650214, China. Electronic address:
The signal intensity ratio (SIR) is a crucial factor in advancing probe technology due to its direct impact on sensitivity and precision, particularly in applications such as medical imaging, environmental monitoring, and food safety testing. However, the development of high-SIR probes is challenged by complexities in fabrication, cost, and mechanical stability. In this study, we address these limitations by investigating the role of halogen atom substitutions in modulating the intermolecular binding energy and aggregation behavior of Ce-Salen Schiff base complexes.
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