Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths

Park, Young -Shin; Lim, Jaehoon; Klimov, Victor I.

doi:10.1038/s41563-018-0254-7

Title: Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths

Journal Article · Mon Jan 07 00:00:00 EST 2019 · Nature Materials

DOI:https://doi.org/10.1038/s41563-018-0254-7· OSTI ID:1492545

^[1]; Lim, Jaehoon ^[2];

^[3]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Ajou Univ., Suwon (Korea, Republic of)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

The application of colloidal semiconductor quantum dots as single-dot light sources still requires overcoming several challenges. Recently, there has been considerable progress in suppressing intensity fluctuations (blinking) by encapsulating an emitting core into a thick protective shell. However, these nanostructures still show considerable fluctuations in both emission energy and linewidth. Here we demonstrate type-I core/shell heterostructures that overcome these deficiencies. They are made by combining wurtzite semiconductors with a large, directionally anisotropic lattice mismatch, which results in strong asymmetric compression of the emitting core. This modifies the structure of band-edge excitonic states and leads to accelerated radiative decay, reduced exciton-phonon interactions, and suppressed coupling to fluctuating electrostatic environment. As a result, individual asymmetrically strained dots exhibit highly stable emission energy (<1 meV standard deviation) and a subthermal room-temperature linewidth (~20 meV), concurrent with nearly nonblinking behaviour, high emission quantum yields, and a widely tunable emission colour.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1492545

Alternate ID(s):: OSTI ID: 1491837

Report Number(s):: LA-UR-19-20496

Journal Information:: Nature Materials, Vol. 18; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 61 works

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References (50)

Alternating layer addition approach to CdSe/CdS core/shell quantum dots with near-unity quantum yield and high on-time fractions Greytak, Andrew B.; Allen, Peter M.; Liu, Wenhao Chemical Science, Vol. 3, Issue 6 https://doi.org/10.1039/c2sc00561a	journal	January 2012
Colloidal Spherical Quantum Wells with Near-Unity Photoluminescence Quantum Yield and Suppressed Blinking Jeong, Byeong Guk; Park, Young-Shin; Chang, Jun Hyuk ACS Nano, Vol. 10, Issue 10 https://doi.org/10.1021/acsnano.6b03704	journal	October 2016
Near-Unity Quantum Yields from Chloride Treated CdTe Colloidal Quantum Dots Page, Robert C.; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A. Small, Vol. 11, Issue 13 https://doi.org/10.1002/smll.201402264	journal	October 2014
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
Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer Colvin, V. L.; Schlamp, M. C.; Alivisatos, A. P. Nature, Vol. 370, Issue 6488 https://doi.org/10.1038/370354a0	journal	August 1994
High-Power Genuine Ultraviolet Light-Emitting Diodes Based On Colloidal Nanocrystal Quantum Dots Kwak, Jeonghun; Lim, Jaehoon; Park, Myeongjin Nano Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.nanolett.5b00392	journal	May 2015
Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots Klimov, V. I.; Mikhailovsky, A. A.; Xu, Su Science, Vol. 290, Issue 5490, p. 314-317 https://doi.org/10.1126/science.290.5490.314	journal	October 2000
Optical gain in colloidal quantum dots achieved with direct-current electrical pumping Lim, Jaehoon; Park, Young-Shin; Klimov, Victor I. Nature Materials, Vol. 17, Issue 1 https://doi.org/10.1038/nmat5011	journal	November 2017
Tandem luminescent solar concentrators based on engineered quantum dots Wu, Kaifeng; Li, Hongbo; Klimov, Victor I. Nature Photonics, Vol. 12, Issue 2 https://doi.org/10.1038/s41566-017-0070-7	journal	January 2018
Quantum Dot Luminescent Concentrator Cavity Exhibiting 30-fold Concentration Bronstein, Noah D.; Yao, Yuan; Xu, Lu ACS Photonics, Vol. 2, Issue 11 https://doi.org/10.1021/acsphotonics.5b00334	journal	August 2015
Solid-state single-photon emitters Aharonovich, Igor; Englund, Dirk; Toth, Milos Nature Photonics, Vol. 10, Issue 10 https://doi.org/10.1038/nphoton.2016.186	journal	September 2016
Semiconductor Quantum Dots in Chemical Sensors and Biosensors Frasco, Manuela; Chaniotakis, Nikos Sensors, Vol. 9, Issue 9 https://doi.org/10.3390/s90907266	journal	September 2009
Quantum dot bioconjugates for imaging, labelling and sensing Medintz, Igor L.; Uyeda, H. Tetsuo; Goldman, Ellen R. Nature Materials, Vol. 4, Issue 6, p. 435-446 https://doi.org/10.1038/nmat1390	journal	June 2005
Semiconductor quantum dots for in vitro diagnostics and cellular imaging Jin, Zongwen; Hildebrandt, Niko Trends in Biotechnology, Vol. 30, Issue 7 https://doi.org/10.1016/j.tibtech.2012.04.005	journal	July 2012
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
“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
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
Single-Dot Spectroscopy of Zinc-Blende CdSe/CdS Core/Shell Nanocrystals: Nonblinking and Correlation with Ensemble Measurements Qin, Haiyan; Niu, Yuan; Meng, Renyang Journal of the American Chemical Society, Vol. 136, Issue 1 https://doi.org/10.1021/ja4078528	journal	December 2013
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
Fluorescence intermittency in single cadmium selenide nanocrystals Nirmal, M.; Dabbousi, B. O.; Bawendi, M. G. Nature, Vol. 383, Issue 6603 https://doi.org/10.1038/383802a0	journal	October 1996
“On”/“off” fluorescence intermittency of single semiconductor quantum dots Kuno, M.; Fromm, D. P.; Hamann, H. F. The Journal of Chemical Physics, Vol. 115, Issue 2 https://doi.org/10.1063/1.1377883	journal	July 2001
Random Telegraph Signal in the Photoluminescence Intensity of a Single Quantum Dot Efros, Al. L.; Rosen, M. Physical Review Letters, Vol. 78, Issue 6 https://doi.org/10.1103/PhysRevLett.78.1110	journal	February 1997
Nano-engineered electron–hole exchange interaction controls exciton dynamics in core–shell semiconductor nanocrystals Brovelli, S.; Schaller, R. D.; Crooker, S. A. Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1281	journal	April 2011
Quasiparticle band structures of six II-VI compounds: ZnS, ZnSe, ZnTe, CdS, CdSe, and CdTe Zakharov, Oleg; Rubio, Angel; Blase, X. Physical Review B, Vol. 50, Issue 15 https://doi.org/10.1103/PhysRevB.50.10780	journal	October 1994
(CdSe)ZnS Core−Shell Quantum Dots: Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites Dabbousi, B. O.; Rodriguez-Viejo, J.; Mikulec, F. V. The Journal of Physical Chemistry B, Vol. 101, Issue 46, p. 9463-9475 https://doi.org/10.1021/jp971091y	journal	November 1997
High-Pressure Structural Transformations in Semiconductor Nanocrystals Tolbert, Sarah H.; Alivisatos, A. P. Annual Review of Physical Chemistry, Vol. 46, Issue 1 https://doi.org/10.1146/annurev.pc.46.100195.003115	journal	October 1995
Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy Fan, Fengjia; Voznyy, Oleksandr; Sabatini, Randy P. Nature, Vol. 544, Issue 7648 https://doi.org/10.1038/nature21424	journal	March 2017
Size dependence of exciton fine structure in CdSe quantum dots Norris, D. J.; Efros, Al. L.; Rosen, M. Physical Review B, Vol. 53, Issue 24 https://doi.org/10.1103/PhysRevB.53.16347	journal	June 1996
Electronic structure and band parameters for Zn (, S, Se, Te) Karazhanov, S. Zh.; Ravindran, P.; Kjekhus, A. Journal of Crystal Growth, Vol. 287, Issue 1 https://doi.org/10.1016/j.jcrysgro.2005.10.061	journal	January 2006
Compressive strain induced heavy hole and light hole splitting of Zn1−xCdxSe epilayers grown by molecular beam epitaxy Yang, C. S.; Hsieh, Y. P.; Kuo, M. C. Materials Chemistry and Physics, Vol. 78, Issue 3 https://doi.org/10.1016/S0254-0584(01)00585-5	journal	February 2003
Strain-induced heavy-hole-to-light-hole energy splitting in (111) B pseudomorphic ${In}_{y}$ ${Ga}_{1 - y}$ As quantum wells Moise, T. S.; Guido, L. J.; Barker, R. C. Physical Review B, Vol. 47, Issue 11 https://doi.org/10.1103/PhysRevB.47.6758	journal	March 1993
Electronic structure and optical properties of [(ZnSe $)_{m}$ (CdSe $)_{n}$ $]_{N}$ -ZnSe multiple quantum wells Ren, Shang-Fen; Xia, Jian-Bai; Han, He-Xiang Physical Review B, Vol. 50, Issue 19 https://doi.org/10.1103/PhysRevB.50.14416	journal	November 1994
Bright and Grey States in CdSe-CdS Nanocrystals Exhibiting Strongly Reduced Blinking Spinicelli, P.; Buil, S.; Quélin, X. Physical Review Letters, Vol. 102, Issue 13 https://doi.org/10.1103/PhysRevLett.102.136801	journal	March 2009
Spectroscopy of single nanocrystals Fernée, Mark J.; Tamarat, Philippe; Lounis, Brahim Chemical Society Reviews, Vol. 43, Issue 4 https://doi.org/10.1039/c3cs60209e	journal	January 2014
Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime Crooker, S. A.; Barrick, T.; Hollingsworth, J. A. Applied Physics Letters, Vol. 82, Issue 17 https://doi.org/10.1063/1.1570923	journal	April 2003
Photogenerated Excitons in Plain Core CdSe Nanocrystals with Unity Radiative Decay in Single Channel: The Effects of Surface and Ligands Gao, Yuan; Peng, Xiaogang Journal of the American Chemical Society, Vol. 137, Issue 12 https://doi.org/10.1021/jacs.5b01314	journal	March 2015
Photoluminescence Spectroscopy of Single CdSe Nanocrystallite Quantum Dots Empedocles, S. A.; Norris, D. J.; Bawendi, M. G. Physical Review Letters, Vol. 77, Issue 18 https://doi.org/10.1103/PhysRevLett.77.3873	journal	October 1996
Spontaneous Spectral Diffusion in CdSe Quantum Dots Fernée, Mark J.; Plakhotnik, Taras; Louyer, Yann The Journal of Physical Chemistry Letters, Vol. 3, Issue 12 https://doi.org/10.1021/jz300456h	journal	June 2012
Electron−Phonon Coupling in CdSe Nanocrystals Kelley, Anne Myers The Journal of Physical Chemistry Letters, Vol. 1, Issue 9 https://doi.org/10.1021/jz100123b	journal	April 2010
Electron-phonon interactions and excitonic dephasing in semiconductor nanocrystals Takagahara, T. Physical Review Letters, Vol. 71, Issue 21 https://doi.org/10.1103/PhysRevLett.71.3577	journal	November 1993
Suppression of Auger Processes in Confined Structures Cragg, George E.; Efros, Alexander L. Nano Letters, Vol. 10, Issue 1 https://doi.org/10.1021/nl903592h	journal	January 2010
Spectroscopy of Colloidal Semiconductor Core/Shell Nanoplatelets with High Quantum Yield Tessier, M. D.; Mahler, B.; Nadal, B. Nano Letters, Vol. 13, Issue 7 https://doi.org/10.1021/nl401538n	journal	June 2013
Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure Rainò, Gabriele; Nedelcu, Georgian; Protesescu, Loredana ACS Nano, Vol. 10, Issue 2 https://doi.org/10.1021/acsnano.5b07328	journal	January 2016
Room‐temperature exciton luminescence in II‐VI quantum wells Stanley, R. P.; Hawdon, B. J.; Hegarty, J. Applied Physics Letters, Vol. 58, Issue 25 https://doi.org/10.1063/1.104712	journal	June 1991
Observation of free excitons in room‐temperature photoluminescence of GaAs/AlGaAs single quantum wells Fujiwara, K.; Tsukada, N.; Nakayama, T. Applied Physics Letters, Vol. 53, Issue 8 https://doi.org/10.1063/1.99847	journal	August 1988
Synthesis and Characterization of Strongly Luminescing ZnS-Capped CdSe Nanocrystals Hines, Margaret A.; Guyot-Sionnest, Philippe The Journal of Physical Chemistry, Vol. 100, Issue 2, p. 468-471 https://doi.org/10.1021/jp9530562	journal	January 1996
Raman-scattering study of exciton-phonon coupling in PbS nanocrystals Krauss, Todd D.; Wise, Frank W. Physical Review B, Vol. 55, Issue 15 https://doi.org/10.1103/PhysRevB.55.9860	journal	April 1997
Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths Cui, Jian; Beyler, Andrew P.; Coropceanu, Igor Nano Letters, Vol. 16, Issue 1 https://doi.org/10.1021/acs.nanolett.5b03790	journal	December 2015
Electron–Phonon Coupling in CdSe Nanocrystals from an Atomistic Phonon Model Kelley, Anne Myers ACS Nano, Vol. 5, Issue 6 https://doi.org/10.1021/nn201475d	journal	May 2011
Theory of the linear and nonlinear optical properties of semiconductor microcrystallites Schmitt-Rink, S.; Miller, D. A. B.; Chemla, D. S. Physical Review B, Vol. 35, Issue 15 https://doi.org/10.1103/PhysRevB.35.8113	journal	May 1987

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