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Title: In situ TEM observation of neck formation during oriented attachment of PbSe nanocrystals

Journal Article · · Nano Research
 [1];  [2];  [3];  [4];  [3];  [4];  [4];  [3];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Xiamen Univ., Xiamen (China)
  3. Univ. of California, Irvine, CA (United States)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
+ Show Author Affiliations

Oriented attachment of nanocrystals is an important route to constructing epitaxially-connected nanocrystal superlattices for various applications. During oriented attachment of semiconductor nanocrystals, neck can be formed between nanocrystals and it strongly influences the properties of the resulting superlattice. However, the neck formation mechanism is poorly understood. Here, we use in situ liquid cell transmission electron microscopy to directly observe the initiation and growth of homoepitaxial necks between PbSe nanocrystals with atomic details. We find that neck initiation occurs slowly (~ 10 s) when two nanocrystals approach to each other within an edge-to-edge distance 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 (neck) width is larger than a critical size of 0.9 nm, it gradually (15 s) widens into a 3-nm-wide neck. The atomic structure of the neck is further obtained using ex situ aberration-corrected scanning TEM imaging. Neck initiation and growth mechanisms are elucidated with density functional theory calculations. As a result, our direct unveiling of the atomic pathways of neck formation during oriented attachment shed light into the fabrication of nanocrystal superlattices with improved structural order and electronic properties.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1563993
Journal Information:
Nano Research, Journal Name: Nano Research Journal Issue: 10 Vol. 12; ISSN 1998-0124
Publisher:
SpringerCopyright Statement
Country of Publication:
United States
Language:
English

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  • Anderson, Nicholas C.; Hendricks, Mark P.; Choi, Joshua J.
  • Journal of the American Chemical Society, Vol. 135, Issue 49, p. 18536-18548 https://doi.org/10.1021/ja4086758
journal November 2013
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Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
PbSe nanocrystals
liquid cell transmission electron microscopy (TEM)
necking
oriented attachment
quantum dots
superlattices