Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices
Abstract
By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.
- Authors:
-
[1];
[4];
[5]
- Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Harvard Univ., Cambridge, MA (United States)
- Univ. of California, Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel)
- Univ. of California, Berkeley, CA (United States); Kavli Energy NanoScience Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), 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)
- OSTI Identifier:
- 1839253
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 2; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; self-assembly; oriented attachment; nanocrystal superlattices; quantum dots; CdSe; thickness; lattices; physical and chemical processes; transmission electron microscopy; nanocrystals
Citation Formats
Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, and Alivisatos, A. Paul. Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices. United States: N. p., 2020.
Web. doi:10.1021/acsnano.0c07202.
Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, & Alivisatos, A. Paul. Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices. United States. https://doi.org/10.1021/acsnano.0c07202
Ondry, Justin C., Philbin, John P., Lostica, Michael, Rabani, Eran, and Alivisatos, A. Paul. Wed .
"Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices". United States. https://doi.org/10.1021/acsnano.0c07202. https://www.osti.gov/servlets/purl/1839253.
@article{osti_1839253,
title = {Colloidal Synthesis Path to 2D Crystalline Quantum Dot Superlattices},
author = {Ondry, Justin C. and Philbin, John P. and Lostica, Michael and Rabani, Eran and Alivisatos, A. Paul},
abstractNote = {By combining colloidal nanocrystal synthesis, self-assembly, and solution phase epitaxial growth techniques, we developed a general method for preparing single dot thick atomically attached quantum dot (QD) superlattices with high-quality translational and crystallographic orientational order along with state-of-the-art uniformity in the attachment thickness. The procedure begins with colloidal synthesis of hexagonal prism shaped core/shell QDs (e.g., CdSe/CdS), followed by liquid subphase self-assembly and immobilization of superlattices on a substrate. Solution phase epitaxial growth of additional semiconductor material fills in the voids between the particles, resulting in a QD-in-matrix structure. The photoluminescence emission spectra of the QD-in-matrix structure retains characteristic 0D electronic confinement. Importantly, annealing of the resulting structures removes inhomogeneities in the QD–QD inorganic bridges, which our atomistic electronic structure calculations demonstrate would otherwise lead to Anderson-type localization. The piecewise nature of this procedure allows one to independently tune the size and material of the QD core, shell, QD–QD distance, and the matrix material. These four choices can be tuned to control many properties (degree of quantum confinement, quantum coupling, band alignments, etc.) depending on the specific applications. Lastly, cation exchange reactions can be performed on the final QD-in-matrix, as demonstrated herein with a CdSe/CdS to HgSe/HgS conversion.},
doi = {10.1021/acsnano.0c07202},
journal = {ACS Nano},
number = 2,
volume = 15,
place = {United States},
year = {Wed Dec 30 00:00:00 EST 2020},
month = {Wed Dec 30 00:00:00 EST 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Quantum dot solids showing state-resolved band-like transport
journal, January 2020
- Lan, Xinzheng; Chen, Menglu; Hudson, Margaret H.
- Nature Materials, Vol. 19, Issue 3
Interfacial Self-Assembly and Oriented Attachment in the Family of PbX (X = S, Se, Te) Nanocrystals
journal, May 2018
- van Overbeek, Carlo; Peters, Joep L.; van Rossum, Susan A. P.
- The Journal of Physical Chemistry C, Vol. 122, Issue 23
Structural, Optical, and Electrical Properties of Self-Assembled Films of PbSe Nanocrystals Treated with 1,2-Ethanedithiol
journal, January 2008
- Luther, Joseph M.; Law, Matt; Song, Qing
- ACS Nano, Vol. 2, Issue 2
Self-Organization of CdSe Nanocrystallites into Three-Dimensional Quantum Dot Superlattices
journal, November 1995
- Murray, C. B.; Kagan, C. R.; Bawendi, M. G.
- Science, Vol. 270, Issue 5240
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking
journal, February 2013
- Chen, Ou; Zhao, Jing; Chauhan, Vikash P.
- Nature Materials, Vol. 12, Issue 5
Identification of atomic-like electronic states in indium arsenide nanocrystal quantum dots
journal, August 1999
- Banin, Uri; Cao, YunWei; Katz, David
- Nature, Vol. 400, Issue 6744
Effect of Thermal Fluctuations on the Radiative Rate in Core/Shell Quantum Dots
journal, February 2017
- Balan, Arunima D.; Eshet, Hagai; Olshansky, Jacob H.
- Nano Letters, Vol. 17, Issue 3
Absence of Diffusion in Certain Random Lattices
journal, March 1958
- Anderson, P. W.
- Physical Review, Vol. 109, Issue 5
Deposition of metal chalcogenide thin films by successive ionic layer adsorption and reaction (SILAR) method
journal, April 2004
- Pathan, H. M.; Lokhande, C. D.
- Bulletin of Materials Science, Vol. 27, Issue 2
DiffTools: Electron diffraction software tools for DigitalMicrograph™
journal, August 2008
- Mitchell, D. R. G.
- Microscopy Research and Technique, Vol. 71, Issue 8
Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995
- Plimpton, Steve
- Journal of Computational Physics, Vol. 117, Issue 1
High charge mobility in two-dimensional percolative networks of PbSe quantum dots connected by atomic bonds
journal, September 2015
- Evers, Wiel H.; Schins, Juleon M.; Aerts, Michiel
- Nature Communications, Vol. 6, Issue 1
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011
- Momma, Koichi; Izumi, Fujio
- Journal of Applied Crystallography, Vol. 44, Issue 6
Colloidal Nanocrystals with Molecular Metal Chalcogenide Surface Ligands
journal, June 2009
- Kovalenko, M. V.; Scheele, M.; Talapin, D. V.
- Science, Vol. 324, Issue 5933
Self-Assembly of Colloidal Hexagonal Bipyramid- and Bifrustum-Shaped ZnS Nanocrystals into Two-Dimensional Superstructures
journal, January 2014
- van der Stam, Ward; Gantapara, Anjan P.; Akkerman, Quinten A.
- Nano Letters, Vol. 14, Issue 2
Resilient Pathways to Atomic Attachment of Quantum Dot Dimers and Artificial Solids from Faceted CdSe Quantum Dot Building Blocks
journal, June 2019
- Ondry, Justin C.; Philbin, John P.; Lostica, Michael
- ACS Nano, Vol. 13, Issue 11
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
Successive Ionic Layer Absorption and Reaction for Postassembly Control over Inorganic Interdot Bonds in Long-Range Ordered Nanocrystal Films
journal, April 2017
- Treml, Benjamin E.; Savitzky, Benjamin H.; Tirmzi, Ali M.
- ACS Applied Materials & Interfaces, Vol. 9, Issue 15
Sequential Cation Exchange in Nanocrystals: Preservation of Crystal Phase and Formation of Metastable Phases
journal, November 2011
- Li, Hongbo; Zanella, Marco; Genovese, Alessandro
- Nano Letters, Vol. 11, Issue 11
The Electronic Structure of CdSe/CdS Core/Shell Seeded Nanorods: Type-I or Quasi-Type-II?
journal, November 2013
- Eshet, Hagai; Grünwald, Michael; Rabani, Eran
- Nano Letters, Vol. 13, Issue 12
CdSe@CdS Dot@Platelet Nanocrystals: Controlled Epitaxy, Monoexponential Decay of Two-Dimensional Exciton, and Nonblinking Photoluminescence of Single Nanocrystal
journal, October 2019
- Wang, Yonghong; Pu, Chaodan; Lei, Hairui
- Journal of the American Chemical Society, Vol. 141, Issue 44
Evaluation of Ordering in Single-Component and Binary Nanocrystal Superlattices by Analysis of Their Autocorrelation Functions
journal, February 2011
- Pichler, Stefan; Bodnarchuk, Maryna I.; Kovalenko, Maksym V.
- ACS Nano, Vol. 5, Issue 3
Structural Characterization of Self-Assembled Multifunctional Binary Nanoparticle Superlattices
journal, March 2006
- Shevchenko, Elena V.; Talapin, Dmitri V.; Murray, Christopher B.
- Journal of the American Chemical Society, Vol. 128, Issue 11
Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids
journal, June 2018
- Gilmore, Rachel H.; Winslow, Samuel W.; Lee, Elizabeth M. Y.
- ACS Nano, Vol. 12, Issue 8
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
Charge Carrier Hopping Dynamics in Homogeneously Broadened PbS Quantum Dot Solids
journal, January 2017
- Gilmore, Rachel H.; Lee, Elizabeth M. Y.; Weidman, Mark C.
- Nano Letters, Vol. 17, Issue 2
Ligand Exchange on Colloidal CdSe Nanocrystals Using Thermally Labile tert -Butylthiol for Improved Photocurrent in Nanocrystal Films
journal, December 2011
- Webber, David H.; Brutchey, Richard L.
- Journal of the American Chemical Society, Vol. 134, Issue 2
Propagation of Structural Disorder in Epitaxially Connected Quantum Dot Solids from Atomic to Micron Scale
journal, August 2016
- Savitzky, Benjamin H.; Hovden, Robert; Whitham, Kevin
- Nano Letters, Vol. 16, Issue 9
Effects of Disorder on Electronic Properties of Nanocrystal Assemblies
journal, January 2015
- Yang, Jun; Wise, Frank W.
- The Journal of Physical Chemistry C, Vol. 119, Issue 6
Evolution of Ordered Metal Chalcogenide Architectures through Chemical Transformations
journal, May 2013
- Rivest, Jessy B.; Buonsanti, Raffaella; Pick, Teresa E.
- Journal of the American Chemical Society, Vol. 135, Issue 20, p. 7446-7449
Exciton Transfer in Array of Epitaxially Connected Nanocrystals
journal, November 2016
- Reich, Konstantin V.; Shklovskii, Boris I.
- ACS Nano, Vol. 10, Issue 11
Collective topo-epitaxy in the self-assembly of a 3D quantum dot superlattice
journal, October 2019
- Abelson, Alex; Qian, Caroline; Salk, Trenton
- Nature Materials, Vol. 19, Issue 1
Colloidal CdSe/CdS Dot-in-Plate Nanocrystals with 2D-Polarized Emission
journal, July 2012
- Cassette, Elsa; Mahler, Benoît; Guigner, Jean-Michel
- ACS Nano, Vol. 6, Issue 8
Long-range orientation and atomic attachment of nanocrystals in 2D honeycomb superlattices
journal, May 2014
- Boneschanscher, M. P.; Evers, W. H.; Geuchies, J. J.
- Science, Vol. 344, Issue 6190
Charge transport in semiconductors assembled from nanocrystal quantum dots
journal, June 2020
- Yazdani, Nuri; Andermatt, Samuel; Yarema, Maksym
- Nature Communications, Vol. 11, Issue 1
Mechanistic Insights into Superlattice Transformation at a Single Nanocrystal Level Using Nanobeam Electron Diffraction
journal, June 2020
- daSilva, Jessica Cimada; Smeaton, Michelle A.; Dunbar, Tyler A.
- Nano Letters, Vol. 20, Issue 7
Forging Colloidal Nanostructures via Cation Exchange Reactions
journal, February 2016
- De Trizio, Luca; Manna, Liberato
- Chemical Reviews, Vol. 116, Issue 18
Superradiance of quantum dots
journal, January 2007
- Scheibner, Michael; Schmidt, Thomas; Worschech, Lukas
- Nature Physics, Vol. 3, Issue 2
Setting Carriers Free: Healing Faulty Interfaces Promotes Delocalization and Transport in Nanocrystal Solids
journal, November 2019
- Walravens, Willem; Solano, Eduardo; Geenen, Filip
- ACS Nano, Vol. 13, Issue 11
Stillinger-Weber potential for the II-VI elements Zn-Cd-Hg-S-Se-Te
journal, August 2013
- Zhou, X. W.; Ward, D. K.; Martin, J. E.
- Physical Review B, Vol. 88, Issue 8
Orientational Disorder in Epitaxially Connected Quantum Dot Solids
journal, September 2019
- McCray, Arthur R. C.; Savitzky, Benjamin H.; Whitham, Kevin
- ACS Nano, Vol. 13, Issue 10
Structural, Optical, and Electrical Properties of PbSe Nanocrystal Solids Treated Thermally or with Simple Amines
journal, May 2008
- Law, Matt; Luther, Joseph M.; Song, Qing
- Journal of the American Chemical Society, Vol. 130, Issue 18
Re-examination of the Size-Dependent Absorption Properties of CdSe Quantum Dots
journal, October 2009
- Jasieniak, Jacek; Smith, Lisa; van Embden, Joel
- The Journal of Physical Chemistry C, Vol. 113, Issue 45
Electronic structure of atomically coherent square semiconductor superlattices with dimensionality below two
journal, September 2013
- Kalesaki, E.; Evers, W. H.; Allan, G.
- Physical Review B, Vol. 88, Issue 11
Influence of the Ion Coordination Number on Cation Exchange Reactions with Copper Telluride Nanocrystals
journal, May 2016
- Tu, Renyong; Xie, Yi; Bertoni, Giovanni
- Journal of the American Chemical Society, Vol. 138, Issue 22
Mono- and Multilayer Silicene-Type Honeycomb Lattices by Oriented Attachment of PbSe Nanocrystals: Synthesis, Structural Characterization, and Analysis of the Disorder
journal, July 2018
- Peters, Joep L.; Altantzis, Thomas; Lobato, Ivan
- Chemistry of Materials, Vol. 30, Issue 14
Synthesis and Micrometer-Scale Assembly of Colloidal CdSe/CdS Nanorods Prepared by a Seeded Growth Approach
journal, October 2007
- Carbone, Luigi; Nobile, Concetta; De Giorgi, Milena
- Nano Letters, Vol. 7, Issue 10
Very Large Electronic Structure Calculations Using an Out-of-Core Filter-Diagonalization Method
journal, July 2002
- Toledo, Sivan; Rabani, Eran
- Journal of Computational Physics, Vol. 180, Issue 1
Size-Dependent Electrical Transport in CdSe Nanocrystal Thin Films
journal, September 2010
- Kang, Moon Sung; Sahu, Ayaskanta; Norris, David J.
- Nano Letters, Vol. 10, Issue 9
Local-density-derived semiempirical pseudopotentials
journal, June 1995
- Wang, Lin-Wang; Zunger, Alex
- Physical Review B, Vol. 51, Issue 24
Extraction, through filter‐diagonalization, of general quantum eigenvalues or classical normal mode frequencies from a small number of residues or a short‐time segment of a signal. I. Theory and application to a quantum‐dynamics model
journal, May 1995
- Wall, Michael R.; Neuhauser, Daniel
- The Journal of Chemical Physics, Vol. 102, Issue 20
Semiconductor Clusters, Nanocrystals, and Quantum Dots
journal, February 1996
- Alivisatos, A. P.
- Science, Vol. 271, Issue 5251, p. 933-937
Electronically Coupled Nanocrystal Superlattice Films by in Situ Ligand Exchange at the Liquid–Air Interface
journal, November 2013
- Dong, Angang; Jiao, Yucong; Milliron, Delia J.
- ACS Nano, Vol. 7, Issue 12
Binary nanocrystal superlattice membranes self-assembled at the liquid–air interface
journal, July 2010
- Dong, Angang; Chen, Jun; Vora, Patrick M.
- Nature, Vol. 466, Issue 7305
Superfluorescence from lead halide perovskite quantum dot superlattices
journal, November 2018
- Rainò, Gabriele; Becker, Michael A.; Bodnarchuk, Maryna I.
- Nature, Vol. 563, Issue 7733
Oleic Acid-Induced Atomic Alignment of ZnS Polyhedral Nanocrystals
journal, March 2016
- van der Stam, Ward; Rabouw, Freddy T.; Vonk, Sander J. W.
- Nano Letters, Vol. 16, Issue 4
Theory and practical recommendations for autocorrelation-based image correlation spectroscopy
journal, August 2012
- Robertson, Claire
- Journal of Biomedical Optics, Vol. 17, Issue 8
Course materials and datasets for the Alivisatos group-based undergraduate research program
other, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Zenodo
Course materials and datasets for the Alivisatos group-based undergraduate research program
dataset, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Dryad
Course materials and datasets for the Alivisatos group-based undergraduate research program
dataset, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Dryad
Works referencing / citing this record:
Course materials and datasets for the Alivisatos group-based undergraduate research program
other, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Zenodo
Course materials and datasets for the Alivisatos group-based undergraduate research program
dataset, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Dryad
Course materials and datasets for the Alivisatos group-based undergraduate research program
other, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Zenodo
Course materials and datasets for the Alivisatos group-based undergraduate research program
dataset, January 2021
- Calvin, Jason; Ondry, Justin; Dahl, Jakob
- Dryad