Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

Orfield, Noah J.; McBride, James R.; Wang, Feng; Buck, Matthew R.; Keene, Joseph D.; Reid, Kemar R.; Htoon, Han; Hollingsworth, Jennifer A.; Rosenthal, Sandra J.

doi:10.1021/acsnano.5b05876

Title: Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

Journal Article · Fri Feb 05 00:00:00 EST 2016 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b05876· OSTI ID:1393884

Orfield, Noah J. ^[1]; McBride, James R. ^[1]; Wang, Feng ^[2]; Buck, Matthew R. ^[2]; Keene, Joseph D. ^[1]; Reid, Kemar R. ^[1]; Htoon, Han ^[2]; Hollingsworth, Jennifer A. ^[2]; Rosenthal, Sandra J. ^[3]

Vanderbilt Univ., Nashville, TN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. Herein, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking "giant" CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging, rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive "dark" fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be "dark". Although, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 1393884

Journal Information:: ACS Nano, Vol. 10, Issue 2; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

References (47)

Hybrid passivated colloidal quantum dot solids Ip, Alexander H.; Thon, Susanna M.; Hoogland, Sjoerd Nature Nanotechnology, Vol. 7, Issue 9 https://doi.org/10.1038/nnano.2012.127	journal	July 2012
Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield Nasilowski, Michel; Spinicelli, Piernicola; Patriarche, Gilles Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.nanolett.5b00838	journal	May 2015
High-Efficiency All-Solution-Processed Light-Emitting Diodes Based on Anisotropic Colloidal Heterostructures with Polar Polymer Injecting Layers Castelli, Andrea; Meinardi, Francesco; Pasini, Mariacecilia Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b01849	journal	July 2015
Experimental Determination of the Extinction Coefficient of CdTe, CdSe, and CdS Nanocrystals Yu, W. William; Qu, Lianhua; Guo, Wenzhuo Chemistry of Materials, Vol. 15, Issue 14, p. 2854-2860 https://doi.org/10.1021/cm034081k	journal	July 2003
Structure Determines Function in Nanoparticles, Their Interfaces, and Their Assemblies Dickson, Robert M. The Journal of Physical Chemistry Letters, Vol. 2, Issue 16 https://doi.org/10.1021/jz200981k	journal	July 2011
Ligand-Controlled Polytypism of Thick-Shell CdSe/CdS Nanocrystals Mahler, Benoît; Lequeux, Nicolas; Dubertret, Benoît Journal of the American Chemical Society, Vol. 132, Issue 3 https://doi.org/10.1021/ja9034973	journal	January 2010
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking Chen, Ou; Zhao, Jing; Chauhan, Vikash P. Nature Materials, Vol. 12, Issue 5 https://doi.org/10.1038/nmat3539	journal	February 2013
A colloidal quantum dot spectrometer Bao, Jie; Bawendi, Moungi G. Nature, Vol. 523, Issue 7558 https://doi.org/10.1038/nature14576	journal	July 2015
On the Absorption Cross Section of CdSe Nanocrystal Quantum Dots Leatherdale, C. A.; Woo, W. -K.; Mikulec, F. V. The Journal of Physical Chemistry B, Vol. 106, Issue 31 https://doi.org/10.1021/jp025698c	journal	August 2002
Atomic-Scale Evolution of a Growing Core–Shell Nanoparticle Mangel, Shai; Aronovitch, Eran; Enyashin, Andrey N. Journal of the American Chemical Society, Vol. 136, Issue 36 https://doi.org/10.1021/ja506323s	journal	August 2014
Suppressed Auger Recombination in “Giant” Nanocrystals Boosts Optical Gain Performance García-Santamaría, Florencio; Chen, Yongfen; Vela, Javier Nano Letters, Vol. 9, Issue 10 https://doi.org/10.1021/nl901681d	journal	October 2009
“Giant” Multishell CdSe Nanocrystal Quantum Dots with Suppressed Blinking Chen, Yongfen; Vela, Javier; Htoon, Han Journal of the American Chemical Society, Vol. 130, Issue 15 https://doi.org/10.1021/ja711379k	journal	April 2008
Single-Molecule Colocalization Studies Shed Light on the Idea of Fully Emitting versus Dark Single Quantum Dots Pons, Thomas; Medintz, Igor L.; Farrell, Dorothy Small, Vol. 7, Issue 14 https://doi.org/10.1002/smll.201100802	journal	June 2011
Effect of shell thickness and composition on blinking suppression and the blinking mechanism in ‘giant’ CdSe/CdS nanocrystal quantum dots Vela, Javier; Htoon, Han; Chen, Yongfen Journal of Biophotonics, Vol. 3, Issue 10-11 https://doi.org/10.1002/jbio.201000058	journal	July 2010
Atomistic Model of Fluorescence Intermittency of Colloidal Quantum Dots Voznyy, O.; Sargent, E. H. Physical Review Letters, Vol. 112, Issue 15 https://doi.org/10.1103/PhysRevLett.112.157401	journal	April 2014
Evidence for the Role of Holes in Blinking: Negative and Oxidized CdSe/CdS Dots Qin, Wei; Guyot-Sionnest, Philippe ACS Nano, Vol. 6, Issue 10 https://doi.org/10.1021/nn303396c	journal	September 2012
Fluorescence quantum yield of CdSe/ZnS nanocrystals investigated by correlated atomic-force and single-particle fluorescence microscopy Ebenstein, Y.; Mokari, T.; Banin, U. Applied Physics Letters, Vol. 80, Issue 21 https://doi.org/10.1063/1.1482785	journal	May 2002
Near-Unity Quantum Yields of Biexciton Emission from $CdSe / CdS$ Nanocrystals Measured Using Single-Particle Spectroscopy Park, Y. -S.; Malko, A. V.; Vela, J. Physical Review Letters, Vol. 106, Issue 18 https://doi.org/10.1103/PhysRevLett.106.187401	journal	May 2011
Biexciton Quantum Yield of Single Semiconductor Nanocrystals from Photon Statistics Nair, Gautham; Zhao, Jing; Bawendi, Moungi G. Nano Letters, Vol. 11, Issue 3 https://doi.org/10.1021/nl104054t	journal	March 2011
Trion Decay in Colloidal Quantum Dots Jha, Praket P.; Guyot-Sionnest, Philippe ACS Nano, Vol. 3, Issue 4 https://doi.org/10.1021/nn9001177	journal	March 2009
Elimination of Hole–Surface Overlap in Graded CdS _x Se _{1– x} Nanocrystals Revealed by Ultrafast Fluorescence Upconversion Spectroscopy Keene, Joseph D.; McBride, James R.; Orfield, Noah J. ACS Nano, Vol. 8, Issue 10 https://doi.org/10.1021/nn504235w	journal	September 2014
Inverting Asymmetric Confinement Potentials in Core/Thick-Shell Nanocrystals Paulite, Melissa; Acharya, Krishna P.; Nguyen, Hue Minh The Journal of Physical Chemistry Letters, Vol. 6, Issue 4 https://doi.org/10.1021/jz5027163	journal	February 2015
Correlation of Atomic Structure and Photoluminescence of the Same Quantum Dot: Pinpointing Surface and Internal Defects That Inhibit Photoluminescence Orfield, Noah J.; McBride, James R.; Keene, Joseph D. ACS Nano, Vol. 9, Issue 1 https://doi.org/10.1021/nn506420w	journal	December 2014
Biocompatible Quantum Dots for Biological Applications Rosenthal, Sandra J.; Chang, Jerry C.; Kovtun, Oleg Chemistry & Biology, Vol. 18, Issue 1 https://doi.org/10.1016/j.chembiol.2010.11.013	journal	January 2011
Ultrafast Carrier Dynamics in CdSe Nanocrystals Determined by Femtosecond Fluorescence Upconversion Spectroscopy Underwood, David F.; Kippeny, Tadd; Rosenthal, Sandra J. The Journal of Physical Chemistry B, Vol. 105, Issue 2 https://doi.org/10.1021/jp003088b	journal	January 2001
Towards non-blinking colloidal quantum dots Mahler, Benoit; Spinicelli, Piernicola; Buil, Stéphanie Nature Materials, Vol. 7, Issue 8 https://doi.org/10.1038/nmat2222	journal	June 2008
Dynamic Fluctuations in Ultrasmall Nanocrystals Induce White Light Emission Pennycook, Timothy J.; McBride, James R.; Rosenthal, Sandra J. Nano Letters, Vol. 12, Issue 6 https://doi.org/10.1021/nl3008727	journal	May 2012
Lifetime blinking in nonblinking nanocrystal quantum dots Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1916	journal	January 2012
Full-colour quantum dot displays fabricated by transfer printing Kim, Tae-Ho; Cho, Kyung-Sang; Lee, Eun Kyung Nature Photonics, Vol. 5, Issue 3 https://doi.org/10.1038/nphoton.2011.12	journal	February 2011
Quantum correlation among photons from a single quantum dot at room temperature Michler, P.; Imamoğlu, A.; Mason, M. D. Nature, Vol. 406, Issue 6799 https://doi.org/10.1038/35023100	journal	August 2000
Aberration-Corrected Z-Contrast Scanning Transmission Electron Microscopy of CdSe Nanocrystals McBride, James R.; Kippeny, Tadd C.; Pennycook, Stephen J. Nano Letters, Vol. 4, Issue 7 https://doi.org/10.1021/nl049406q	journal	July 2004
Dynamic Trap Formation and Elimination in Colloidal Quantum Dots Voznyy, O.; Thon, S. M.; Ip, A. H. The Journal of Physical Chemistry Letters, Vol. 4, Issue 6 https://doi.org/10.1021/jz400125r	journal	March 2013
Quantitative Z-contrast imaging in the scanning transmission electron microscope with size-selected clusters Wang, Z. W.; Li, Z. Y.; Park, S. J. Physical Review B, Vol. 84, Issue 7 https://doi.org/10.1103/PhysRevB.84.073408	journal	August 2011
Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea Nature, Vol. 479, Issue 7372 https://doi.org/10.1038/nature10569	journal	November 2011
The Possibility and Implications of Dynamic Nanoparticle Surfaces McBride, James R.; Pennycook, Timothy J.; Pennycook, Stephen J. ACS Nano, Vol. 7, Issue 10 https://doi.org/10.1021/nn403478h	journal	September 2013
Effect of Surface Stoichiometry on Blinking and Hole Trapping Dynamics in CdSe Nanocrystals Busby, Erik; Anderson, Nicholas C.; Owen, Jonathan S. The Journal of Physical Chemistry C, Vol. 119, Issue 49 https://doi.org/10.1021/acs.jpcc.5b08243	journal	November 2015
Delayed Exciton Emission and Its Relation to Blinking in CdSe Quantum Dots Rabouw, Freddy T.; Kamp, Marko; van Dijk-Moes, Relinde J. A. Nano Letters, Vol. 15, Issue 11 https://doi.org/10.1021/acs.nanolett.5b03818	journal	October 2015
Biexciton Quantum Yield Heterogeneities in Single CdSe (CdS) Core (Shell) Nanocrystals and Its Correlation to Exciton Blinking Zhao, Jing; Chen, Ou; Strasfeld, David B. Nano Letters, Vol. 12, Issue 9 https://doi.org/10.1021/nl3013727	journal	January 2012
Quantitative Atomic Resolution Scanning Transmission Electron Microscopy LeBeau, James M.; Findlay, Scott D.; Allen, Leslie J. Physical Review Letters, Vol. 100, Issue 20 https://doi.org/10.1103/PhysRevLett.100.206101	journal	May 2008
Fluorescence spectroscopy and transmission electron microscopy of the same isolated semiconductor nanocrystals Koberling, Felix; Mews, Alf; Philipp, Günther Applied Physics Letters, Vol. 81, Issue 6 https://doi.org/10.1063/1.1499221	journal	August 2002
Wavelength-tunable colloidal quantum dot laser on ultra-thin flexible glass Foucher, C.; Guilhabert, B.; Laurand, N. Applied Physics Letters, Vol. 104, Issue 14 https://doi.org/10.1063/1.4871372	journal	April 2014
Fluorescence Anisotropy and Crystal Structure of Individual Semiconductor Nanocrystals ^† Koberling, Felix; Kolb, Ute; Philipp, Günther The Journal of Physical Chemistry B, Vol. 107, Issue 30 https://doi.org/10.1021/jp027800b	journal	July 2003
New Insights into the Complexities of Shell Growth and the Strong Influence of Particle Volume in Nonblinking “Giant” Core/Shell Nanocrystal Quantum Dots Ghosh, Yagnaseni; Mangum, Benjamin D.; Casson, Joanna L. Journal of the American Chemical Society, Vol. 134, Issue 23 https://doi.org/10.1021/ja212032q	journal	May 2012
Measurement of the Radiative and Nonradiative Decay Rates of Single CdSe Nanocrystals through a Controlled Modification of their Spontaneous Emission Brokmann, X.; Coolen, L.; Dahan, M. Physical Review Letters, Vol. 93, Issue 10 https://doi.org/10.1103/PhysRevLett.93.107403	journal	September 2004
Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals Javaux, C.; Mahler, B.; Dubertret, B. Nature Nanotechnology, Vol. 8, Issue 3 https://doi.org/10.1038/nnano.2012.260	journal	February 2013
CdSSe Nanocrystals with Induced Chemical Composition Gradients Harrison, Melissa A.; Ng, Amy; Hmelo, Anthony B. Israel Journal of Chemistry, Vol. 52, Issue 11-12 https://doi.org/10.1002/ijch.201200040	journal	December 2012
Non-blinking single-photon emitters in silica Rabouw, Freddy T.; Cogan, Nicole M. B.; Berends, Anne C. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep21187	journal	February 2016

Cited By (9)

Engineering Auger recombination in colloidal quantum dots via dielectric screening Hou, Xiaoqi; Kang, Jun; Qin, Haiyan Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09737-2	journal	April 2019
Correlating nano black spots and optical stability in mixed halide perovskite quantum dots Ko, Yun-Hyuk; Prabhakaran, Prem; Jalalah, Mohammed Journal of Materials Chemistry C, Vol. 6, Issue 29 https://doi.org/10.1039/c8tc01040d	journal	January 2018
Excited-State Dynamics in Colloidal Semiconductor Nanocrystals Rabouw, Freddy T.; de Mello Donega, Celso Topics in Current Chemistry, Vol. 374, Issue 5 https://doi.org/10.1007/s41061-016-0060-0	journal	August 2016
Determination of quantum yields of semiconductor nanocrystals at the single emitter level via fluorescence correlation spectroscopy Abbandonato, Gerardo; Hoffmann, Katrin; Resch-Genger, Ute Nanoscale, Vol. 10, Issue 15 https://doi.org/10.1039/c7nr09332b	journal	January 2018
Real colloidal quantum dot structures revealed by high resolution analytical electron microscopy McBride, James R.; Rosenthal, Sandra J. The Journal of Chemical Physics, Vol. 151, Issue 16 https://doi.org/10.1063/1.5128366	journal	October 2019
Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna Matsuzaki, Korenobu; Vassant, Simon; Liu, Hsuan-Wei arXiv https://doi.org/10.48550/arxiv.1608.07843	preprint	January 2016
Strong plasmonic enhancement of biexciton emission: controlled coupling of a single quantum dot to a gold nanocone antenna Matsuzaki, Korenobu; Vassant, Simon; Liu, Hsuan-Wei Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/srep42307	journal	February 2017
Excited-State Dynamics in Colloidal Semiconductor Nanocrystals Rabouw, Freddy T.; de Mello Donega, Celso Photoactive Semiconductor Nanocrystal Quantum Dots https://doi.org/10.1007/978-3-319-51192-4_1	book	August 2016
Effects of interface-potential smoothness and wavefunction delocalization on Auger recombination in colloidal CdSe-based core/shell quantum dots Hou, Xiaoqi; Li, Yang; Qin, Haiyan The Journal of Chemical Physics, Vol. 151, Issue 23 https://doi.org/10.1063/1.5125940	journal	December 2019

Similar Records

Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

Journal Article · Fri Feb 05 00:00:00 EST 2016 · ACS Nano · OSTI ID:1393884

Orfield, Noah J.; McBride, James R.; Wang, Feng; +6 more

Excitation wavelength dependent photon anti-bunching/bunching from single quantum dots near gold nanostructures

Journal Article · Mon Jan 01 00:00:00 EST 2018 · Nanoscale · OSTI ID:1393884

Dey, Swayandipta; Zhou, Yadong; Sun, Yonglei; +6 more

Photoluminescence Enhancement, Blinking Suppression, and Improved Biexciton Quantum Yield of Single Quantum Dots in Zero Mode Waveguides

Journal Article · Thu Mar 25 00:00:00 EDT 2021 · Journal of Physical Chemistry Letters · OSTI ID:1393884

Masud, Abdullah Al; Arefin, S. M. Nayeem; Fairooz, Fatema; +10 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
correlation
heterogeneity
nanocrystal atomic structure
nanocrystal quantum dot
quantum yield

Title: Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

Citation Formats

References (47)

Cited By (9)

Similar Records

Related Subjects