We investigated the stability of gold clusters doped with open 3d-shell atoms (Sc, Ti, V, Cr, Mn, Fe, Co, Ni). Steps, peaks, and odd-even staggering in mass abundance spectra upon photofragmentation provide evidence for enhanced stability for specific cluster sizes. The observed magic numbers are explained in terms of size- and dopant-dependent modifications of the effective mean-field potential within a phenomenological shell-model approach. Element-dependent 3d electron delocalization and odd-even staggering amplitudes are related to the dopant-atom structure.
Download full-text PDF |
Source |
---|---|
http://dx.doi.org/10.1103/PhysRevLett.90.033401 | DOI Listing |
Angew Chem Int Ed Engl
December 2024
Shenzhen institute of advanced technology Chinese Academy of Sciences, Functional Thin Films Research Centre, 1068 Xueyuan Avenue, Shenzhen University Town, 518000, SHENZHEN, CHINA.
Organics electrode materials offer multi-electron reactivity, flexible structures, and redox reversibility, but encounter poor conductivity and durability in electrolytes. To overcome above barriers, we propose a dual elongation strategy of π-conjugated motifs with active sites, involving extended carbazole and electropolymerized crosslinked polymer, which enhances electronic conductivity by the electronic delocalization of electron-withdrawing conjugated groups, boosts theoretical capacity by increasing redox-active site density, and endows robust electrochemical stability attributed to crosslinked organic structures. As a proof-of-concept, 5,11-dihydridoindolo[3,2-b]carbazole (DHIC) is selected as the model cathode material for a dual-ion battery, with elongated carbazole groups functioning both as redox-active centers and polymerization anchors.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Institut Chimie radicalaire ICR-UMR 7273, Facult� de Saint jerome, avenue Escadrille-Normandie-Niemen, service 562, 13397, Marseille, FRANCE.
Efforts to understand radical stability have led to considerable progress in radical chemistry. In this article, we investigated a novel approach to enhancing the radical stability of carbon-centered radicals through space electron delocalization within [2,2]-paracyclophanes. Alkoxyamines possessing a paracyclophane scaffold exploit face-to-face π-π-interactions between the aromatic rings to effectively lower bond dissociation energy (BDE) for NO-C bond homolysis.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Institute of Atomic and Molecular Physics, Jilin University, Changchun 130023, China.
While planar tetracoordinate (pt) centers have been extensively explored from carbon to other octal-row elements or their heavier analogs, their counterparts involving alkali (A) and alkaline-earth metals (Ae) remain elusive due to the large atomic radius and absence of p orbitals. In this work, we found six hitherto unknown anionic ptA (A4A-) and neutral ptAe (A4Ae) centers through an extensive exploration of potential energy surfaces. The D4h-symmetry ptBe structures in Li4Be and Na4Be emerge as the lowest-energy configurations, and all the other ptA/ptAe structures are higher in energy or saddle points.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Center for Advanced Materials Research, Beijing Normal University, Zhuhai 519087, China.
Proton transfer plays a crucial role in various chemical and biological processes. A major theoretical challenge in simulating proton transfer arises from the quantum nature of the proton. The constrained nuclear-electronic orbital (CNEO) framework was recently developed to efficiently and accurately account for nuclear quantum effects, particularly quantum nuclear delocalization effects, in quantum chemistry calculations and molecular dynamics simulations.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Materials Science, Fudan University Shanghai 200433 China
A cation exchange (CE) reaction offers a remarkable opportunity to create versatile metal sulfide nanocrystals (NCs) with arbitrary complexity in composition, structure, and functionality. The concept of regioselectivity has been discovered and developed to build the target heterostructures through CE reactions, yet a general principle of regioselectivity remains unclear. In this work, we establish connections between experimental results and theoretical insights to elucidate the determinants of regioselectivity using designed aliovalent CE reactions on a two-dimensional template.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!