Discovering highly stable metal fullerenes such as the celebrated C 60 is interesting in cluster science as they have potential applications as building blocks in new nanostructures.We here investigated the structural...Discovering highly stable metal fullerenes such as the celebrated C 60 is interesting in cluster science as they have potential applications as building blocks in new nanostructures.We here investigated the structural and electronic properties of the fullerenes M 12 @Au 20（M=Na,Al,Ag,Sc,Y,La,Lu,and Au）,using a first-principles investigation with the density functional theory.It is found that these compound clusters possess a similar cage structure to the icosahedral Au 32 fullerene.La 12 @Au 20 is found to be particularly stable among these clusters.The binding energy of La 12 @Au 20 is 3.43 eV per atom,1.05 eV larger than that in Au 32.The highest occupied molecular orbital-lowest unoccupied molecular orbital（HOMO-LUMO） gap of La 12 @Au 20 is only 0.31 eV,suggesting that it should be relatively chemically reactive.展开更多
The common Au nanostructures(nanospheres,nanorods and nanosheets)were prepared by the seed growth method to explore the cold welding phenomenon of these non-single crystal nanostructures at room temperature.Systematic...The common Au nanostructures(nanospheres,nanorods and nanosheets)were prepared by the seed growth method to explore the cold welding phenomenon of these non-single crystal nanostructures at room temperature.Systematic studies show that the concentration of surfactant cetyltrimethylammonium bromide(CTAB)and drying conditions are important factors to determine the evolution and final configuration of nanostructures during welding.The key factor of cold welding is the concentration of surfactant as low as 0.3 mm/L,and the welding should be carried out under the condition of slow evaporation and sufficient relaxation time,rather than rapid drying process.At the same time,the structural evolution during the welding process of gold rod head and tail is simulated by combining the electronic microscope characterization and density functional theory,which reveals that the stability of the welding nanostructure is better than that of the dispersed nanostructure.In the slow evaporation process of Au nanostructures with the same crystal structure,the low surfactant attached to the surface of the nanoparticles increases the attraction between the nanoparticles,which makes the nanoparticles close to each other adhere due to the interaction,and improves the physical properties of the intersection due to the diffusion,epitaxy and surface relaxation of the metal surface atoms.The results provide a research basis for the physical property analysis of nanostructures and the construction of defect devices.展开更多
Employing first-principles methods, based on the density functional theory, this paper investigates the ground state geometric and electronic properties of pure gold clusters, pure yttrium clusters and gold clusters d...Employing first-principles methods, based on the density functional theory, this paper investigates the ground state geometric and electronic properties of pure gold clusters, pure yttrium clusters and gold clusters doped each with one yttrium atom. It is shown that the average bond lengths in the Aun-1Y（n≤9） bimetallic clusters are shorter than those in the corresponding pure gold and yttrium clusters. The most stable isomers of the yttrium-doped gold clusters tend to equally delocalize valence s, p and d electrons of the constituent atoms over the entire structure. The Y atom has maximum number of neighbouring Au atom, which tends to be energetically favourable in the lowest-energy equilibrium structures, because the Au-Y bond is stronger than the Au-Au bond. The three-dimensional isomers of Aun-1Y structures are found in an early appearance starting at n=5 （Au4Y）. Calculated vertical ionization potential and electron affinities as a function of the cluster size show odd-even oscillatory behaviour, and resemble pure gold clusters. However, one of the most striking feature of pure yttrium clusters is the absence of odd-even alternation, in agreement with mass spectrometric observations. The HOMO LUMO gap of Au3Y is the biggest in all the doped Aun-1Y（n≤9） bimetallic clusters.展开更多
The general features of the geometries and electronic properties for 3d, 4d, and 5d transition-metal atom doped Au6 clusters are systematically investigated by using relativistic all-electron density functional theory...The general features of the geometries and electronic properties for 3d, 4d, and 5d transition-metal atom doped Au6 clusters are systematically investigated by using relativistic all-electron density functional theory in the generalized gradient approximation （CGA）. A number of structural isomers are considered to search the lowest-energy structures of M@Au6 clusters （M=3d, 4d and 5d transition-metal atoms）, and the transition metal atom locating in the centre of an Au6 ring is found to be in the ground state for all the M@Au6 clusters. All doped clusters, expect for Pd@Au6, show large relative binding energies compared with a pure Au7 cluster, indicating that doping by 3d, 4d, 5d transition-metal atoms could stabilize the Au6 ring and promote the formation of a new binary alloy cluster.展开更多
基金Project supported by the National Natural Science Foundation of China (Grant No. 11104075)the Fundamental Research Funds for the Central Universities of China (Grant No. WM0911005)
文摘Discovering highly stable metal fullerenes such as the celebrated C 60 is interesting in cluster science as they have potential applications as building blocks in new nanostructures.We here investigated the structural and electronic properties of the fullerenes M 12 @Au 20（M=Na,Al,Ag,Sc,Y,La,Lu,and Au）,using a first-principles investigation with the density functional theory.It is found that these compound clusters possess a similar cage structure to the icosahedral Au 32 fullerene.La 12 @Au 20 is found to be particularly stable among these clusters.The binding energy of La 12 @Au 20 is 3.43 eV per atom,1.05 eV larger than that in Au 32.The highest occupied molecular orbital-lowest unoccupied molecular orbital（HOMO-LUMO） gap of La 12 @Au 20 is only 0.31 eV,suggesting that it should be relatively chemically reactive.
基金supported by the National Natural Science Foundations of China (Nos. 11774171,11874220,21805137)the Open Funds of Key Laboratory for Intelligent Nano Materials and Devices of the Ministry of Education (Nos. INMD-2019M02, INMD2020M03)+1 种基金the Scientific Foundation of Nanjing Institute of Technology(No. CKJB201708)the Fundamental Research Funds for the Central Universities(No.NS2017047) provided by Nanjing University of Aeronautics and Astronautics
文摘The common Au nanostructures(nanospheres,nanorods and nanosheets)were prepared by the seed growth method to explore the cold welding phenomenon of these non-single crystal nanostructures at room temperature.Systematic studies show that the concentration of surfactant cetyltrimethylammonium bromide(CTAB)and drying conditions are important factors to determine the evolution and final configuration of nanostructures during welding.The key factor of cold welding is the concentration of surfactant as low as 0.3 mm/L,and the welding should be carried out under the condition of slow evaporation and sufficient relaxation time,rather than rapid drying process.At the same time,the structural evolution during the welding process of gold rod head and tail is simulated by combining the electronic microscope characterization and density functional theory,which reveals that the stability of the welding nanostructure is better than that of the dispersed nanostructure.In the slow evaporation process of Au nanostructures with the same crystal structure,the low surfactant attached to the surface of the nanoparticles increases the attraction between the nanoparticles,which makes the nanoparticles close to each other adhere due to the interaction,and improves the physical properties of the intersection due to the diffusion,epitaxy and surface relaxation of the metal surface atoms.The results provide a research basis for the physical property analysis of nanostructures and the construction of defect devices.
基金Project supported by the Education Committee of Chongqing (Grant No KJ051105)the National Natural Science Foundation of China (Grant No 10276028)
文摘Employing first-principles methods, based on the density functional theory, this paper investigates the ground state geometric and electronic properties of pure gold clusters, pure yttrium clusters and gold clusters doped each with one yttrium atom. It is shown that the average bond lengths in the Aun-1Y（n≤9） bimetallic clusters are shorter than those in the corresponding pure gold and yttrium clusters. The most stable isomers of the yttrium-doped gold clusters tend to equally delocalize valence s, p and d electrons of the constituent atoms over the entire structure. The Y atom has maximum number of neighbouring Au atom, which tends to be energetically favourable in the lowest-energy equilibrium structures, because the Au-Y bond is stronger than the Au-Au bond. The three-dimensional isomers of Aun-1Y structures are found in an early appearance starting at n=5 （Au4Y）. Calculated vertical ionization potential and electron affinities as a function of the cluster size show odd-even oscillatory behaviour, and resemble pure gold clusters. However, one of the most striking feature of pure yttrium clusters is the absence of odd-even alternation, in agreement with mass spectrometric observations. The HOMO LUMO gap of Au3Y is the biggest in all the doped Aun-1Y（n≤9） bimetallic clusters.
文摘The general features of the geometries and electronic properties for 3d, 4d, and 5d transition-metal atom doped Au6 clusters are systematically investigated by using relativistic all-electron density functional theory in the generalized gradient approximation （CGA）. A number of structural isomers are considered to search the lowest-energy structures of M@Au6 clusters （M=3d, 4d and 5d transition-metal atoms）, and the transition metal atom locating in the centre of an Au6 ring is found to be in the ground state for all the M@Au6 clusters. All doped clusters, expect for Pd@Au6, show large relative binding energies compared with a pure Au7 cluster, indicating that doping by 3d, 4d, 5d transition-metal atoms could stabilize the Au6 ring and promote the formation of a new binary alloy cluster.
