Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals
Abstract
Toward a truly photostable PbSe quantum dot (QD), we apply the thick-shell or “giant” QD structural motif to this notoriously environmentally sensitive nanocrystal system. Namely, using a sequential application of two shell-growth techniques—partial-cation exchange and successive ionic layer adsorption and reaction (SILAR)—we are able to overcoat the PbSe QDs with sufficiently thick CdSe shells to impart new single-QD-level photostability, as evidenced by suppression of both photobleaching and blinking behavior. Here, we further reveal that the crystal structure of the CdSe shell (cubic zinc-blende or hexagonal wurtzite) plays a key role in determining the photoluminescence properties of these giant QDs, with only cubic nanocrystals sufficiently bright and stable to be observed as single emitters. Moreover, we demonstrate that crystal structure and particle shape (cubic, spherical, or tetrapodal) and, thereby, emission properties can be synthetically tuned by either withholding or including the coordinating ligand, trioctylphosphine, in the SILAR component of the shell-growth process.
- Authors:
-
[1];
[1];
[1];
[4];
[1];
[1]
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Physics
- Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemistry
- Univ. of Texas at Dallas, Richardson, TX (United States). Dept. of Materials Science and Engineering
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1481991
- Report Number(s):
- LA-UR-18-21088
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 139; Journal Issue: 32; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 36 MATERIALS SCIENCE; Inorganic and Physical Chemistry; Material Science
Citation Formats
Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, and Hollingsworth, Jennifer A. Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals. United States: N. p., 2017.
Web. doi:10.1021/jacs.7b03705.
Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, & Hollingsworth, Jennifer A. Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals. United States. https://doi.org/10.1021/jacs.7b03705
Hanson, Christina J., Hartmann, Nicolai F., Singh, Ajay, Ma, Xuedan, DeBenedetti, William J. I., Casson, Joanna L., Grey, John K., Chabal, Yves J., Malko, Anton V., Sykora, Milan, Piryatinski, Andrei, Htoon, Han, and Hollingsworth, Jennifer A. Thu .
"Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals". United States. https://doi.org/10.1021/jacs.7b03705. https://www.osti.gov/servlets/purl/1481991.
@article{osti_1481991,
title = {Giant PbSe/CdSe/CdSe Quantum Dots: Crystal-Structure-Defined Ultrastable Near-Infrared Photoluminescence from Single Nanocrystals},
author = {Hanson, Christina J. and Hartmann, Nicolai F. and Singh, Ajay and Ma, Xuedan and DeBenedetti, William J. I. and Casson, Joanna L. and Grey, John K. and Chabal, Yves J. and Malko, Anton V. and Sykora, Milan and Piryatinski, Andrei and Htoon, Han and Hollingsworth, Jennifer A.},
abstractNote = {Toward a truly photostable PbSe quantum dot (QD), we apply the thick-shell or “giant” QD structural motif to this notoriously environmentally sensitive nanocrystal system. Namely, using a sequential application of two shell-growth techniques—partial-cation exchange and successive ionic layer adsorption and reaction (SILAR)—we are able to overcoat the PbSe QDs with sufficiently thick CdSe shells to impart new single-QD-level photostability, as evidenced by suppression of both photobleaching and blinking behavior. Here, we further reveal that the crystal structure of the CdSe shell (cubic zinc-blende or hexagonal wurtzite) plays a key role in determining the photoluminescence properties of these giant QDs, with only cubic nanocrystals sufficiently bright and stable to be observed as single emitters. Moreover, we demonstrate that crystal structure and particle shape (cubic, spherical, or tetrapodal) and, thereby, emission properties can be synthetically tuned by either withholding or including the coordinating ligand, trioctylphosphine, in the SILAR component of the shell-growth process.},
doi = {10.1021/jacs.7b03705},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 139,
place = {United States},
year = {Thu Aug 03 00:00:00 EDT 2017},
month = {Thu Aug 03 00:00:00 EDT 2017}
}
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Works referenced in this record:
PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors
journal, October 2005
- Talapin, D. V.
- Science, Vol. 310, Issue 5745, p. 86-89
Ultrasensitive solution-cast quantum dot photodetectors
journal, July 2006
- Konstantatos, Gerasimos; Howard, Ian; Fischer, Armin
- Nature, Vol. 442, Issue 7099
Infrared Colloidal Quantum Dots for Photovoltaics: Fundamentals and Recent Progress
journal, September 2010
- Tang, Jiang; Sargent, Edward H.
- Advanced Materials, Vol. 23, Issue 1
Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control
journal, May 2012
- Sun, Liangfeng; Choi, Joshua J.; Stachnik, David
- Nature Nanotechnology, Vol. 7, Issue 6
Tunable Near-Infrared Optical Gain and Amplified Spontaneous Emission Using PbSe Nanocrystals
journal, December 2003
- Schaller, R. D.; Petruska, M. A.; Klimov, V. I.
- The Journal of Physical Chemistry B, Vol. 107, Issue 50
Room-temperature amplified spontaneous emission at 1300 nm in solution-processed PbS quantum-dot films
journal, January 2005
- Sukhovatkin, V.; Musikhin, S.; Gorelikov, I.
- Optics Letters, Vol. 30, Issue 2
A solution-processed 1.53 μm quantum dot laser with temperature-invariant emission wavelength
journal, January 2006
- Hoogland, S.; Sukhovatkin, V.; Howard, I.
- Optics Express, Vol. 14, Issue 8
Optical Properties of Colloidal PbSe Nanocrystals
journal, November 2002
- Du, Hui; Chen, Chialing; Krishnan, Rishikesh
- Nano Letters, Vol. 2, Issue 11
Pushing the Band Gap Envelope: Mid-Infrared Emitting Colloidal PbSe Quantum Dots
journal, September 2004
- Pietryga, Jeffrey M.; Schaller, Richard D.; Werder, Donald
- Journal of the American Chemical Society, Vol. 126, Issue 38
Second window for in vivo imaging
journal, November 2009
- Smith, Andrew M.; Mancini, Michael C.; Nie, Shuming
- Nature Nanotechnology, Vol. 4, Issue 11
Photostability of Colloidal PbSe and PbSe/PbS Core/Shell Nanocrystals in Solution and in the Solid State
journal, December 2006
- Stouwdam, Jan W.; Shan, Jingning; van Veggel, Frank C. J. M.
- The Journal of Physical Chemistry C, Vol. 111, Issue 3
Unraveling Internal Structures of Highly Luminescent PbSe Nanocrystallites Using Variable-Energy Synchrotron Radiation Photoelectron Spectroscopy
journal, August 2006
- Sapra, Sameer; Nanda, J.; Pietryga, Jeffrey M.
- The Journal of Physical Chemistry B, Vol. 110, Issue 31
Effect of Air Exposure on Surface Properties, Electronic Structure, and Carrier Relaxation in PbSe Nanocrystals
journal, March 2010
- Sykora, Milan; Koposov, Alexey Y.; McGuire, John A.
- ACS Nano, Vol. 4, Issue 4
Utilizing the Lability of Lead Selenide to Produce Heterostructured Nanocrystals with Bright, Stable Infrared Emission
journal, April 2008
- Pietryga, Jeffrey M.; Werder, Donald J.; Williams, Darrick J.
- Journal of the American Chemical Society, Vol. 130, Issue 14
Highly Effective Surface Passivation of PbSe Quantum Dots through Reaction with Molecular Chlorine
journal, November 2012
- Bae, Wan Ki; Joo, Jin; Padilha, Lazaro A.
- Journal of the American Chemical Society, Vol. 134, Issue 49
Ultrastable PbSe Nanocrystal Quantum Dots via in Situ Formation of Atomically Thin Halide Adlayers on PbSe(100)
journal, June 2014
- Woo, Ju Young; Ko, Jae-Hyeon; Song, Jung Hoon
- Journal of the American Chemical Society, Vol. 136, Issue 25
Air-Stable PbSe Nanocrystals Passivated by Phosphonic Acids
journal, January 2016
- Woo, Ju Young; Lee, Sooho; Lee, Seokwon
- Journal of the American Chemical Society, Vol. 138, Issue 3
The Different Nature of Band Edge Absorption and Emission in Colloidal PbSe/CdSe Core/Shell Quantum Dots
journal, December 2010
- De Geyter, Bram; Justo, Yolanda; Moreels, Iwan
- ACS Nano, Vol. 5, Issue 1
Composition-Tunable Optical Properties of Colloidal IV−VI Quantum Dots, Composed of Core/Shell Heterostructures with Alloy Components
journal, October 2010
- Maikov, Georgy I.; Vaxenburg, Roman; Sashchiuk, Aldona
- ACS Nano, Vol. 4, Issue 11
Single Photon Counting from Individual Nanocrystals in the Infrared
journal, May 2012
- Correa, Raoul E.; Dauler, Eric A.; Nair, Gautham
- Nano Letters, Vol. 12, Issue 6
Fiber-based cryogenic and time-resolved spectroscopy of PbS quantum dots
journal, January 2011
- Rakher, Matthew T.; Bose, Ranojoy; Wong, Chee Wei
- Optics Express, Vol. 19, Issue 3
“Giant” Multishell CdSe Nanocrystal Quantum Dots with Suppressed Blinking
journal, April 2008
- Chen, Yongfen; Vela, Javier; Htoon, Han
- Journal of the American Chemical Society, Vol. 130, Issue 15
Towards non-blinking colloidal quantum dots
journal, June 2008
- Mahler, Benoit; Spinicelli, Piernicola; Buil, Stéphanie
- Nature Materials, Vol. 7, Issue 8
Effect of shell thickness and composition on blinking suppression and the blinking mechanism in ‘giant’ CdSe/CdS nanocrystal quantum dots
journal, July 2010
- Vela, Javier; Htoon, Han; Chen, Yongfen
- Journal of Biophotonics, Vol. 3, Issue 10-11
New Insights into the Complexities of Shell Growth and the Strong Influence of Particle Volume in Nonblinking “Giant” Core/Shell Nanocrystal Quantum Dots
journal, May 2012
- Ghosh, Yagnaseni; Mangum, Benjamin D.; Casson, Joanna L.
- Journal of the American Chemical Society, Vol. 134, Issue 23
Suppressed Blinking and Auger Recombination in Near-Infrared Type-II InP/CdS Nanocrystal Quantum Dots
journal, October 2012
- Dennis, Allison M.; Mangum, Benjamin D.; Piryatinski, Andrei
- Nano Letters, Vol. 12, Issue 11
Large-Scale Synthesis of Nearly Monodisperse CdSe/CdS Core/Shell Nanocrystals Using Air-Stable Reagents via Successive Ion Layer Adsorption and Reaction
journal, October 2003
- Li, J. Jack; Wang, Y. Andrew; Guo, Wenzhuo
- Journal of the American Chemical Society, Vol. 125, Issue 41, p. 12567-12575
Anisotropic Cation Exchange in PbSe/CdSe Core/Shell Nanocrystals of Different Geometry
journal, December 2011
- Casavola, Marianna; van Huis, Marijn A.; Bals, Sara
- Chemistry of Materials, Vol. 24, Issue 2
Ligand-Controlled Polytypism of Thick-Shell CdSe/CdS Nanocrystals
journal, January 2010
- Mahler, Benoît; Lequeux, Nicolas; Dubertret, Benoît
- Journal of the American Chemical Society, Vol. 132, Issue 3
Crystal Structure Control of Zinc-Blende CdSe/CdS Core/Shell Nanocrystals: Synthesis and Structure-Dependent Optical Properties
journal, November 2012
- Nan, Wennuan; Niu, Yuan; Qin, Haiyan
- Journal of the American Chemical Society, Vol. 134, Issue 48
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
Controlled growth of tetrapod-branched inorganic nanocrystals
journal, May 2003
- Manna, Liberato; Milliron, Delia J.; Meisel, Andreas
- Nature Materials, Vol. 2, Issue 6, p. 382-385
Zinc-blende–wurtzite polytypism in semiconductors
journal, October 1992
- Yeh, Chin-Yu; Lu, Z. W.; Froyen, S.
- Physical Review B, Vol. 46, Issue 16
Synthesis of CdSeS Nanocrystals in Coordinating and Noncoordinating Solvents: Solvent's Role in Evolution of the Optical and Structural Properties
journal, October 2007
- Al-Salim, Najeh; Young, Aidan G.; Tilley, Richard D.
- Chemistry of Materials, Vol. 19, Issue 21
Size control by rate control in colloidal PbSe quantum dot synthesis
journal, January 2015
- Čapek, Richard Karel; Yanover, Dianna; Lifshitz, Efrat
- Nanoscale, Vol. 7, Issue 12
Crystal Phase Transitions in the Shell of PbS/CdS Core/Shell Nanocrystals Influences Photoluminescence Intensity
journal, October 2014
- Lechner, Rainer T.; Fritz-Popovski, Gerhard; Yarema, Maksym
- Chemistry of Materials, Vol. 26, Issue 20
Seeded Growth of Highly Luminescent CdSe/CdS Nanoheterostructures with Rod and Tetrapod Morphologies
journal, October 2007
- Talapin, Dmitri V.; Nelson, James H.; Shevchenko, Elena V.
- Nano Letters, Vol. 7, Issue 10
Nearly Monodisperse and Shape-Controlled CdSe Nanocrystals via Alternative Routes: Nucleation and Growth
journal, April 2002
- Peng, Z. Adam; Peng, Xiaogang
- Journal of the American Chemical Society, Vol. 124, Issue 13, p. 3343-3353
Infrared-Active Heterostructured Nanocrystals with Ultralong Carrier Lifetimes
journal, July 2010
- Lee, Doh C.; Robel, István; Pietryga, Jeffrey M.
- Journal of the American Chemical Society, Vol. 132, Issue 29
Density Functional Theory Study of Ligand Binding on CdSe (0001), (0001̄), and (112̄0) Single Crystal Relaxed and Reconstructed Surfaces: Implications for Nanocrystalline Growth
journal, September 2006
- Rempel, Jane Y.; Trout, Bernhardt L.; Bawendi, Moungi G.
- The Journal of Physical Chemistry B, Vol. 110, Issue 36
The nature of quantum dot capping ligands
journal, January 2010
- Green, Mark
- Journal of Materials Chemistry, Vol. 20, Issue 28
Beyond Band Alignment: Hole Localization Driven Formation of Three Spatially Separated Long-Lived Exciton States in CdSe/CdS Nanorods
journal, July 2013
- Wu, Kaifeng; Rodríguez-Córdoba, William E.; Liu, Zheng
- ACS Nano, Vol. 7, Issue 8
Universal Length Dependence of Rod-to-Seed Exciton Localization Efficiency in Type I and Quasi-Type II CdSe@CdS Nanorods
journal, February 2015
- Wu, Kaifeng; Hill, Lawrence J.; Chen, Jinquan
- ACS Nano, Vol. 9, Issue 4
Using shape to turn off blinking for two-colour multiexciton emission in CdSe/CdS tetrapods
journal, May 2017
- Mishra, Nimai; Orfield, Noah J.; Wang, Feng
- Nature Communications, Vol. 8, Issue 1
Correlation of Atomic Structure and Photoluminescence of the Same Quantum Dot: Pinpointing Surface and Internal Defects That Inhibit Photoluminescence
journal, December 2014
- Orfield, Noah J.; McBride, James R.; Keene, Joseph D.
- ACS Nano, Vol. 9, Issue 1
Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation
journal, January 2016
- Orfield, Noah J.; McBride, James R.; Wang, Feng
- ACS Nano, Vol. 10, Issue 2
Hole-Induced Electron Transport through Core−Shell Quantum Dots: A Direct Measurement of the Electron−Hole Interaction
journal, May 2010
- Swart, Ingmar; Sun, Zhixiang; Vanmaekelbergh, Daniël
- Nano Letters, Vol. 10, Issue 5
Heterostructuring Nanocrystal Quantum Dots Toward Intentional Suppression of Blinking and Auger Recombination
journal, March 2013
- Hollingsworth, Jennifer A.
- Chemistry of Materials, Vol. 25, Issue 8
Works referencing / citing this record:
Role of Interface Chemistry in Opening New Radiative Pathways in InP/CdSe Giant Quantum Dots with Blinking‐Suppressed Two‐Color Emission
journal, June 2019
- Dennis, Allison M.; Buck, Matthew R.; Wang, Feng
- Advanced Functional Materials, Vol. 29, Issue 37
Tailoring the interfacial structure of colloidal “giant” quantum dots for optoelectronic applications
journal, January 2018
- Zhao, Haiguang; Liu, Jiabin; Vidal, François
- Nanoscale, Vol. 10, Issue 36
Real colloidal quantum dot structures revealed by high resolution analytical electron microscopy
journal, October 2019
- McBride, James R.; Rosenthal, Sandra J.
- The Journal of Chemical Physics, Vol. 151, Issue 16
Optoelectronic Properties in Near-Infrared Colloidal Heterostructured Pyramidal “Giant” Core/Shell Quantum Dots
journal, July 2018
- Tong, Xin; Kong, Xiang-Tian; Wang, Chao
- Advanced Science, Vol. 5, Issue 8