Perspective: Bonding and electronic origin of Au atomic-undercoordination-derivacy and nanoscale-size-dependency

Sun, Chang Q.

doi:10.1016/j.vacuum.2021.110061

Cited by 10 publications

(10 citation statements)

References 62 publications

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“…This unusual selectivity toward the Au−N bonding is likely due to the unique nanostructure of the metal surface created by the STM-BJ technique. 36,37 Similar Au−N bonding reactions are also observed for other iminyl radicals with different backbone lengths (Figures 4b,c, S10, and S11). For instance, monophenylene-and terphenylene-substituted aminyl radicals generated through photolysis of oxime esters Al-1 and Al-3 can also bind to Au electrodes and lead to the formation of similar covalent Au−N bonded single-molecule junctions.…”

Section: ■ Results and Discussionsupporting

confidence: 68%

“…However, our STM-BJ measurements based on oxime ester precursors only show signals of the Au–N bonded single-molecule junctions, indicating that the possible side reactions may occur to a very limited extent. This unusual selectivity toward the Au–N bonding is likely due to the unique nanostructure of the metal surface created by the STM-BJ technique. , …”

Section: Resultsmentioning

confidence: 99%

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Iminyl-Radical-Mediated Formation of Covalent Au–N Bonds for Molecular Junctions

et al. 2023

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The interaction between organic radicals and transition metals plays a crucial role in radical-mediated chemical reactions, functional devices, and biocatalysis. Characterizing such interactions, however, remains a long-standing challenge due to the inherently high reactivity of radical species. Here, using a scanning tunneling microscope breaking junction (STM-BJ) technique, we are able to detect the interaction mode between iminyl radicals and the gold surface at a single molecule level. We show that the free iminyl radicals generated through photochemical N−O bond homolysis of oxime esters react toward the gold electrode surface and produce covalent Au−N bonds. Intriguingly, we find that the Au−N bonding reactions lead to the formation of robust and highly conductive single-molecule junctions. These findings provide not only insights into the mechanism of iminyl-radical-involved reactions but also a facile photolysis method to create a new type of covalent electrode−molecule bonding contact for molecular devices.

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Section: ■ Results and Discussionsupporting

confidence: 68%

Section: Resultsmentioning

confidence: 99%

Iminyl-Radical-Mediated Formation of Covalent Au–N Bonds for Molecular Junctions

et al. 2023

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“…The spherical Cu-Au nanoparticles with different sizes might exhibit both atomically ordered and atomically disordered structures, and nanoparticles form the core-shell structure as the degree of atomically ordered increases [21]. The lattice strains and vacancies exist in the surface shell layers, while the internal cores have the similar atomic structure as the bulk material [28,29]. The main potential function applied an embedded atom method (EAM) potential for the binary Cu-Au system developed by Gola [30].…”

Section: Methodsmentioning

confidence: 99%

Molecular dynamics study on the structural properties and phase transformation of Cu-Au nanoparticles

Cui

Meng

2023

Mater. Res. Express

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The electroreduction of CO2 to carbon-containing products carries considerable significance. Cu-Au alloys have been considered as potential bimetallic catalysts recently. However, the current theoretical study of obtaining Cu-Au alloys that could enhance the catalytic activity is insufficiently thorough. Herein, the structural properties and phase transition rules of Cu-Au nanoparticles are investigated utilizing molecular dynamics. The results indicate that the percentage of disordered atoms in Cu-Au nanoparticles decreases and the melting temperature increases with the growth of particle size. Moreover, the coordination number decreases with increasing radial distance. Cu-Au nanoparticles are coexisting in crystalline and amorphous states during melting. The structural properties of Cu-Au catalysts could be regulated by the phase transition rules, which provided a theoretical basis for the modification of surface activity.

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“…Furthermore, the R is not limited to H but any atom less electronegative, such as the situation of the four-stage O:Cu−O bond formation and relaxation in the Cu(001; 110) surface chemisorption. 27 It is expected the HBCP and the BOLS regulations are dominant in single-atom catalysis 29 and the topological and high-T C superconductivity. 30 DFT computations derive information on the O:H−N segmental length and the bond angle relaxation and intramolecular electron redistribution as well under compression, 31 in terms of the bond order: 32…”

mentioning

confidence: 99%

“…Furthermore, the R is not limited to H but any atom less electronegative, such as the situation of the four-stage O:Cu–O bond formation and relaxation in the Cu(001; 110) surface chemisorption . It is expected the HBCP and the BOLS regulations are dominant in single-atom catalysis and the topological and high- T C superconductivity …”

mentioning

confidence: 99%

Discriminative Mechanical and Thermal Response of the H–N Bonds for the Energetic LLM-105 Molecular Assembly

Wang,

Zeng,

Zheng

et al. 2023

J. Phys. Chem. Lett.

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Molecular interactions in energetic materials form the key not only to the "structure stability, energy storage, ignition, and detonation" dynamics but also to the sensitivity to the loading of perturbation and the power intensity of radiation for the energetic substance, with the nature of the interactions remaining elusive. With the aid of perturbative Raman spectroscopy and the pressure-resolved density functional theory, we uncovered that the H−N bond of the intermolecular O:H−N bonds for LLM-105 shares the same negative compressibility and thermal expansivity of the H−O bond for the coupling O:H−O bond of water [Phys. Rep. 2023, 998, 1− 68]. In contrast, the dangling H−N bond vibrating at a 3440 cm −1 high frequency does otherwise due to the absence of coupling interaction and the undercoordination-driven bond contraction. These findings should deepen our insight into interactions involving electron lone pairs and offer an efficient means for discriminating the performance of individual bonds.

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Perspective: Bonding and electronic origin of Au atomic-undercoordination-derivacy and nanoscale-size-dependency

Cited by 10 publications

References 62 publications

Iminyl-Radical-Mediated Formation of Covalent Au–N Bonds for Molecular Junctions

Iminyl-Radical-Mediated Formation of Covalent Au–N Bonds for Molecular Junctions

Molecular dynamics study on the structural properties and phase transformation of Cu-Au nanoparticles

Discriminative Mechanical and Thermal Response of the H–N Bonds for the Energetic LLM-105 Molecular Assembly

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