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Title: Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks

Abstract

Conspectus. Oriented atomic attachment of colloidal inorganic nanocrystals represents a powerful synthetic method for preparing complex inorganic superstructures. Examples include fusion of nanocrystals into dimer and superlattice structures. If the attachment were perfect throughout, then the resulting materials would have single crystal-like alignment of the individual nanocrystals' atomic lattices. While individual colloidal nanocrystals typically are free of many defects, there are a multitude of pathways that can generate defects upon nanocrystal attachment. These attachment generated defects are typically undesirable, and thus developing strategies to favor defect-free attachment or heal defective interfaces are essential. There may also be some cases where attachment-derived defects are desirable. In this Account, we summarize our current understanding of how these defects arise, in order to offer guidance to those who are designing nanocrystal derived solids. The small size of inorganic nanocrystals means short diffusion lengths to the surface, which favor the formation of nanocrystal building blocks with pristine atomic structures. Upon attachment, however, there are numerous pathways that can lead to atomic scale defects, and bulk crystal dislocation theory provides an invaluable guide to understanding these phenomena. As an example, an atomic step edge can be incorporated into the interface leading to an extra half-planemore » of atoms, known as an edge dislocation. These dislocations can be well described by the Burgers vector description of dislocations, which geometrically identifies planes in which a dislocation can move. Our in situ measurements have verified that bulk dislocation theory predictions for 1D defects hold true at few-nanometer length scales in PbTe and CdSe nanocrystal interfaces. Ultimately, the applicability of dislocation theory to nanocrystal attachment enables the predictive design of attachment to prevent or facilitate healing of defects upon nanocrystal attachment. We applied similar logic to understand formation of planar (2D) defects such as stacking faults upon nanocrystal attachment. Again concepts from bulk crystal defect crystallography can identify attachment pathways that can prevent or deterministically form planar defects upon nanocrystal attachment. The concepts we discuss work well for identifying favorable attachment geometries for nanocrystal pairs; however it is currently unclear how to translate these ideas to near-simultaneous multiparticle attachment. Geometric frustration, which prevents nanocrystal rotation, and yet-to-be considered defect generation pathways unique to multiparticle attachment complicate defect-free superlattice attachment. New imaging methods now allow for the direct observation of local attachment trajectories and may enable improved understanding of such multiparticle phenomena. With further refinement, a unified framework for understanding and ultimately eliminating structural defects in fused nanocrystal superstructures may well be achievable in coming years.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Kavli Energy NanoScience Institute, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Kavli Energy NanoScience Institute, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
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; National Science Foundation (NSF)
OSTI Identifier:
1814618
Grant/Contract Number:  
AC02-05CH11231; DMR-1808151
Resource Type:
Accepted Manuscript
Journal Name:
Accounts of Chemical Research
Additional Journal Information:
Journal Volume: 54; Journal Issue: 6; Journal ID: ISSN 0001-4842
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Ondry, Justin C., and Alivisatos, A. Paul. Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks. United States: N. p., 2021. Web. https://doi.org/10.1021/acs.accounts.0c00719.
Ondry, Justin C., & Alivisatos, A. Paul. Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks. United States. https://doi.org/10.1021/acs.accounts.0c00719
Ondry, Justin C., and Alivisatos, A. Paul. Fri . "Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks". United States. https://doi.org/10.1021/acs.accounts.0c00719.
@article{osti_1814618,
title = {Application of Dislocation Theory to Minimize Defects in Artificial Solids Built with Nanocrystal Building Blocks},
author = {Ondry, Justin C. and Alivisatos, A. Paul},
abstractNote = {Conspectus. Oriented atomic attachment of colloidal inorganic nanocrystals represents a powerful synthetic method for preparing complex inorganic superstructures. Examples include fusion of nanocrystals into dimer and superlattice structures. If the attachment were perfect throughout, then the resulting materials would have single crystal-like alignment of the individual nanocrystals' atomic lattices. While individual colloidal nanocrystals typically are free of many defects, there are a multitude of pathways that can generate defects upon nanocrystal attachment. These attachment generated defects are typically undesirable, and thus developing strategies to favor defect-free attachment or heal defective interfaces are essential. There may also be some cases where attachment-derived defects are desirable. In this Account, we summarize our current understanding of how these defects arise, in order to offer guidance to those who are designing nanocrystal derived solids. The small size of inorganic nanocrystals means short diffusion lengths to the surface, which favor the formation of nanocrystal building blocks with pristine atomic structures. Upon attachment, however, there are numerous pathways that can lead to atomic scale defects, and bulk crystal dislocation theory provides an invaluable guide to understanding these phenomena. As an example, an atomic step edge can be incorporated into the interface leading to an extra half-plane of atoms, known as an edge dislocation. These dislocations can be well described by the Burgers vector description of dislocations, which geometrically identifies planes in which a dislocation can move. Our in situ measurements have verified that bulk dislocation theory predictions for 1D defects hold true at few-nanometer length scales in PbTe and CdSe nanocrystal interfaces. Ultimately, the applicability of dislocation theory to nanocrystal attachment enables the predictive design of attachment to prevent or facilitate healing of defects upon nanocrystal attachment. We applied similar logic to understand formation of planar (2D) defects such as stacking faults upon nanocrystal attachment. Again concepts from bulk crystal defect crystallography can identify attachment pathways that can prevent or deterministically form planar defects upon nanocrystal attachment. The concepts we discuss work well for identifying favorable attachment geometries for nanocrystal pairs; however it is currently unclear how to translate these ideas to near-simultaneous multiparticle attachment. Geometric frustration, which prevents nanocrystal rotation, and yet-to-be considered defect generation pathways unique to multiparticle attachment complicate defect-free superlattice attachment. New imaging methods now allow for the direct observation of local attachment trajectories and may enable improved understanding of such multiparticle phenomena. With further refinement, a unified framework for understanding and ultimately eliminating structural defects in fused nanocrystal superstructures may well be achievable in coming years.},
doi = {10.1021/acs.accounts.0c00719},
journal = {Accounts of Chemical Research},
number = 6,
volume = 54,
place = {United States},
year = {2021},
month = {2}
}

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Works referenced in this record:

Stacking-fault energy of II–VI compounds
journal, February 1985


Direction-Specific Interactions Control Crystal Growth by Oriented Attachment
journal, May 2012


Partial dislocations in the wurtzite lattice
journal, January 1971


X-ray determination of threading dislocation densities in GaN/Al 2 O 3 (0001) films grown by metalorganic vapor phase epitaxy
journal, February 2014

  • Kopp, Viktor S.; Kaganer, Vladimir M.; Baidakova, Marina V.
  • Journal of Applied Physics, Vol. 115, Issue 7
  • DOI: 10.1063/1.4865502

Defects in Semiconductors: Some Fatal, Some Vital
journal, August 1998


Imperfect Oriented Attachment: Dislocation Generation in Defect-Free Nanocrystals
journal, August 1998


Comment on “Self-Purification in Semiconductor Nanocrystals”
journal, May 2008


Dalpian and Chelikowsky Reply:
journal, May 2008


The compound Sr 3 Ti 2 O 7 and its structure
journal, January 1958


Collective topo-epitaxy in the self-assembly of a 3D quantum dot superlattice
journal, October 2019


Imperfect Oriented Attachment:  Accretion and Defect Generation of Nanosize Rutile Condensates
journal, July 2004

  • Tsai, M. H.; Chen, S. Y.; Shen, P.
  • Nano Letters, Vol. 4, Issue 7
  • DOI: 10.1021/nl0495763

Diffusion of Cd in CdS
journal, April 1964


Long-range orientation and atomic attachment of nanocrystals in 2D honeycomb superlattices
journal, May 2014


Open‐core screw dislocations in GaN epilayers observed by scanning force microscopy and high‐resolution transmission electron microscopy
journal, October 1995

  • Qian, W.; Rohrer, G. S.; Skowronski, M.
  • Applied Physics Letters, Vol. 67, Issue 16
  • DOI: 10.1063/1.115127

Mechanistic Insights into Superlattice Transformation at a Single Nanocrystal Level Using Nanobeam Electron Diffraction
journal, June 2020


Steps on surfaces: experiment and theory
journal, September 1999


Self-Purification in Semiconductor Nanocrystals
journal, June 2006


The Electronic Structure of Semiconductor Nanocrystals
journal, August 2000


Low-Dimensional Semiconductor Superlattices Formed by Geometric Control over Nanocrystal Attachment
journal, November 2012

  • Evers, Wiel H.; Goris, Bart; Bals, Sara
  • Nano Letters, Vol. 13, Issue 6
  • DOI: 10.1021/nl303322k

Symmetry of Annealed Wurtzite CdSe Nanocrystals: Assignment to the C3v Point Group
journal, November 1995

  • Shiang, J. J.; Kadavanich, A. V.; Grubbs, R. K.
  • The Journal of Physical Chemistry, Vol. 99, Issue 48
  • DOI: 10.1021/j100048a017

Atomistic Insights into the Oriented Attachment of Tunnel-Based Oxide Nanostructures
journal, December 2015


Setting Carriers Free: Healing Faulty Interfaces Promotes Delocalization and Transport in Nanocrystal Solids
journal, November 2019


Melting in Semiconductor Nanocrystals
journal, June 1992


Colloidal quantum dot molecules manifesting quantum coupling at room temperature
journal, December 2019


Quantifying Atomic-Scale Quantum Dot Superlattice Behavior Upon in situ Heating
journal, August 2019

  • Smeaton, Michelle A.; Balazs, Daniel M.; Hanrath, Tobias
  • Microscopy and Microanalysis, Vol. 25, Issue S2
  • DOI: 10.1017/S1431927619008420

Radiation damage in the TEM and SEM
journal, August 2004


Zinc Blende 0D Quantum Dots to Wurtzite 1D Quantum Wires: The Oriented Attachment and Phase Change in ZnSe Nanostructures
journal, September 2013

  • Sarkar, Suresh; Acharya, Shinjita; Chakraborty, Arup
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 19
  • DOI: 10.1021/jz401816e

Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks
journal, June 2019


Charge transport and localization in atomically coherent quantum dot solids
journal, February 2016

  • Whitham, Kevin; Yang, Jun; Savitzky, Benjamin H.
  • Nature Materials, Vol. 15, Issue 5
  • DOI: 10.1038/nmat4576

The buckling of a thin plate due to the presence of an edge dislocation
journal, January 1962


Perfect Dislocations in the Wurtzite Lattice
journal, January 1968


Significantly Enhanced Emission Stability of CsPbBr 3 Nanocrystals via Chemically Induced Fusion Growth for Optoelectronic Devices
journal, October 2018

  • Morrell, Maria V.; He, Xiaoqing; Luo, Guangfu
  • ACS Applied Nano Materials, Vol. 1, Issue 11
  • DOI: 10.1021/acsanm.8b01298

High-Resolution EM of Colloidal Nanocrystal Growth Using Graphene Liquid Cells
journal, April 2012


Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield
journal, March 2019

  • Hanifi, David A.; Bronstein, Noah D.; Koscher, Brent A.
  • Science, Vol. 363, Issue 6432
  • DOI: 10.1126/science.aat3803

Confined-but-Connected Quantum Solids via Controlled Ligand Displacement
journal, June 2013

  • Baumgardner, William J.; Whitham, Kevin; Hanrath, Tobias
  • Nano Letters, Vol. 13, Issue 7
  • DOI: 10.1021/nl401298s

Dirac Cones, Topological Edge States, and Nontrivial Flat Bands in Two-Dimensional Semiconductors with a Honeycomb Nanogeometry
journal, January 2014


Observation of two atomic configurations for the {12̄10} stacking fault in wurtzite (Ga, Al) nitrides
journal, February 1999

  • Vermaut, P.; Nouet, G.; Ruterana, P.
  • Applied Physics Letters, Vol. 74, Issue 5
  • DOI: 10.1063/1.122990

Dynamics and Removal Pathway of Edge Dislocations in Imperfectly Attached PbTe Nanocrystal Pairs: Toward Design Rules for Oriented Attachment
journal, February 2018

  • Ondry, Justin C.; Hauwiller, Matthew R.; Alivisatos, A. Paul
  • ACS Nano, Vol. 12, Issue 4
  • DOI: 10.1021/acsnano.8b00638

Crystal Phase Engineering in Single InAs Nanowires
journal, September 2010

  • Dick, Kimberly A.; Thelander, Claes; Samuelson, Lars
  • Nano Letters, Vol. 10, Issue 9
  • DOI: 10.1021/nl101632a

Propagation of Structural Disorder in Epitaxially Connected Quantum Dot Solids from Atomic to Micron Scale
journal, August 2016


Oleic Acid-Induced Atomic Alignment of ZnS Polyhedral Nanocrystals
journal, March 2016


Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite
journal, December 2018

  • Thind, Arashdeep Singh; Luo, Guangfu; Hachtel, Jordan A.
  • Advanced Materials, Vol. 31, Issue 4
  • DOI: 10.1002/adma.201805047