Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications.During oriented attach me nt of semic on ductor nano crystals,neck can...Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications.During oriented attach me nt of semic on ductor nano crystals,neck can be formed betwee n nan ocrystals and it strongly influe nces the properties of the resulting superlattice.However,the neck formation mechanism is poorly understood.Here,we use in situ liquid cell transmission electro n microscopy(TEM)to directly observe the initiatio n and growth of homoepitaxial n ecks betwee n PbSe nano crystals with atomic details.We find that neck initiatio n occurs slowly(~10 s)whe n two nano crystals approach to each other within an edge-to-edge dista nee of 0.6 nm.During neck initiation,Pb and Se atoms defuse from other facets into the gap,forming"dynamic reversible"filaments.Once the filament(n eck)width is larger than a critical size of 0.9 nm,it gradually(15 s)widens into a 3-nm-wide n eck.The atomic structure of the neck is further obtained using ex situ aberration-corrected seanning TEM imaging.Neck initiation and growth mechanisms are elucidated with density functional theory calculati ons.Our direct unveiling of the atomic pathways of neck formatio n duri ng oriented attach me nt shed light into the fabrication of nanocrystal superlattices with improved structural order and electronic properties.展开更多
Two-dimensional metal-organic layers(MOLs)from alternatively connected benzene-tribenzoate ligands and Zr6(μ3-O)_(4)(μ3-OH)_(4) or Hf6(μ3-O)_(4)(μ3-OH)_(4) secondary building units can be prepared in gram scale vi...Two-dimensional metal-organic layers(MOLs)from alternatively connected benzene-tribenzoate ligands and Zr6(μ3-O)_(4)(μ3-OH)_(4) or Hf6(μ3-O)_(4)(μ3-OH)_(4) secondary building units can be prepared in gram scale via solvothermal synthesis.However,the reason why the monolayers did not pack to form thick crystals is unknown.Here we investigated the surface structure of the MOLs by a combination of sum-frequency generation spectroscopy,nanoscale infrared microscopy,atomic force microscopy,aberration-corrected transmission electron microscopy,and compositional analysis.We found a partial coverage of the monolayer surface by dangling tricarboxylate ligands,which prevent packing of the monolayers.This finding illustrates low-density surface modification as a strategy to prepare new two-dimensional materials with a high percentage of exposed surface.展开更多
文摘Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications.During oriented attach me nt of semic on ductor nano crystals,neck can be formed betwee n nan ocrystals and it strongly influe nces the properties of the resulting superlattice.However,the neck formation mechanism is poorly understood.Here,we use in situ liquid cell transmission electro n microscopy(TEM)to directly observe the initiatio n and growth of homoepitaxial n ecks betwee n PbSe nano crystals with atomic details.We find that neck initiatio n occurs slowly(~10 s)whe n two nano crystals approach to each other within an edge-to-edge dista nee of 0.6 nm.During neck initiation,Pb and Se atoms defuse from other facets into the gap,forming"dynamic reversible"filaments.Once the filament(n eck)width is larger than a critical size of 0.9 nm,it gradually(15 s)widens into a 3-nm-wide n eck.The atomic structure of the neck is further obtained using ex situ aberration-corrected seanning TEM imaging.Neck initiation and growth mechanisms are elucidated with density functional theory calculati ons.Our direct unveiling of the atomic pathways of neck formatio n duri ng oriented attach me nt shed light into the fabrication of nanocrystal superlattices with improved structural order and electronic properties.
基金support from the Ministry of Science and Technology of China(No.2016YFA0200702)the National Natural Science Foundation of China(No.21671162 and No.21721001)the XMU Training Program of Innovation and Entrepreneurship for Undergraduates and NFFTBS(No.J1310024).
文摘Two-dimensional metal-organic layers(MOLs)from alternatively connected benzene-tribenzoate ligands and Zr6(μ3-O)_(4)(μ3-OH)_(4) or Hf6(μ3-O)_(4)(μ3-OH)_(4) secondary building units can be prepared in gram scale via solvothermal synthesis.However,the reason why the monolayers did not pack to form thick crystals is unknown.Here we investigated the surface structure of the MOLs by a combination of sum-frequency generation spectroscopy,nanoscale infrared microscopy,atomic force microscopy,aberration-corrected transmission electron microscopy,and compositional analysis.We found a partial coverage of the monolayer surface by dangling tricarboxylate ligands,which prevent packing of the monolayers.This finding illustrates low-density surface modification as a strategy to prepare new two-dimensional materials with a high percentage of exposed surface.
