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Title: Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks

Abstract

Here, the goal of this work is to identify favored pathways for preparation of defect-resilient attached wurtzite CdX (X = S, Se, Te) nanocrystals. We seek guidelines for oriented attachment of faceted nanocrystals that are most likely to yield pairs of nanocrystals with either few or no electronic defects or electronic defects that are in and of themselves desirable and stable. Using a combination of in situ high-resolution transmission electron microscopy (HRTEM) and electronic structure calculations, we evaluate the relative merits of atomic attachment of wurtzite CdSe nanocrystals on the {1$$\bar{10}$$0} or {11$$\bar{20}$$} family of facets. Pairwise attachment on either facet can lead to perfect interfaces, provided the nanocrystal facets are perfectly flat and the angles between the nanocrystals can adjust during the assembly. Considering defective attachment, we observe for {1$$\bar{10}$$0} facet attachment that only one type of edge dislocation forms, creating deep hole traps. For {11$$\bar{20}$$} facet attachment, we observe that four distinct types of extended defects form, some of which lead to deep hole traps whereas others only to shallow hole traps. HRTEM movies of the dislocation dynamics show that dislocations at {1$$\bar{10}$$0} interfaces can be removed, albeit slowly. Whereas only some extended defects at {11$$\bar{20}$$} interfaces could be removed, others were trapped at the interface. Based on these insights, we identify the most resilient pathways to atomic attachment of pairs of wurtzite CdX nanocrystals and consider how these insights can translate to the creation of electronically useful materials from quantum dots with other crystal structures.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [2]; ORCiD logo [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tel Aviv Univ. (Israel)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1616975
Grant/Contract Number:  
AC02-05CH11231; DMR-1808151
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; nanocrystals; oriented attachment; dislocations; CdSe; electronic structure; in situ TEM

Citation Formats

Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, and Alivisatos, A. Paul. Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks. United States: N. p., 2019. Web. https://doi.org/10.1021/acsnano.9b03052.
Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, & Alivisatos, A. Paul. Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks. United States. https://doi.org/10.1021/acsnano.9b03052
Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, and Alivisatos, A. Paul. Thu . "Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks". United States. https://doi.org/10.1021/acsnano.9b03052. https://www.osti.gov/servlets/purl/1616975.
@article{osti_1616975,
title = {Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks},
author = {Ondry, Justin C. and Philbin, John P. and Lostica, Michael and Rabani, Eran and Alivisatos, A. Paul},
abstractNote = {Here, the goal of this work is to identify favored pathways for preparation of defect-resilient attached wurtzite CdX (X = S, Se, Te) nanocrystals. We seek guidelines for oriented attachment of faceted nanocrystals that are most likely to yield pairs of nanocrystals with either few or no electronic defects or electronic defects that are in and of themselves desirable and stable. Using a combination of in situ high-resolution transmission electron microscopy (HRTEM) and electronic structure calculations, we evaluate the relative merits of atomic attachment of wurtzite CdSe nanocrystals on the {1$\bar{10}$0} or {11$\bar{20}$} family of facets. Pairwise attachment on either facet can lead to perfect interfaces, provided the nanocrystal facets are perfectly flat and the angles between the nanocrystals can adjust during the assembly. Considering defective attachment, we observe for {1$\bar{10}$0} facet attachment that only one type of edge dislocation forms, creating deep hole traps. For {11$\bar{20}$} facet attachment, we observe that four distinct types of extended defects form, some of which lead to deep hole traps whereas others only to shallow hole traps. HRTEM movies of the dislocation dynamics show that dislocations at {1$\bar{10}$0} interfaces can be removed, albeit slowly. Whereas only some extended defects at {11$\bar{20}$} interfaces could be removed, others were trapped at the interface. Based on these insights, we identify the most resilient pathways to atomic attachment of pairs of wurtzite CdX nanocrystals and consider how these insights can translate to the creation of electronically useful materials from quantum dots with other crystal structures.},
doi = {10.1021/acsnano.9b03052},
journal = {ACS Nano},
number = 11,
volume = 13,
place = {United States},
year = {2019},
month = {6}
}

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