Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths
Abstract
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.
- Authors:
-
[1];
[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)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1492545
- Alternate Identifier(s):
- OSTI ID: 1491837
- Report Number(s):
- LA-UR-19-20496
Journal ID: ISSN 1476-1122
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 18; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Material Science; quantum dots
Citation Formats
Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor I. Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths. United States: N. p., 2019.
Web. doi:10.1038/s41563-018-0254-7.
Park, Young -Shin, Lim, Jaehoon, & Klimov, Victor I. Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths. United States. https://doi.org/10.1038/s41563-018-0254-7
Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor I. Mon .
"Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths". United States. https://doi.org/10.1038/s41563-018-0254-7. https://www.osti.gov/servlets/purl/1492545.
@article{osti_1492545,
title = {Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths},
author = {Park, Young -Shin and Lim, Jaehoon and Klimov, Victor I.},
abstractNote = {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.},
doi = {10.1038/s41563-018-0254-7},
journal = {Nature Materials},
number = ,
volume = 18,
place = {United States},
year = {Mon Jan 07 00:00:00 EST 2019},
month = {Mon Jan 07 00:00:00 EST 2019}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 61 works
Citation information provided by
Web of Science
Web of Science
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:
Alternating layer addition approach to CdSe/CdS core/shell quantum dots with near-unity quantum yield and high on-time fractions
journal, January 2012
- Greytak, Andrew B.; Allen, Peter M.; Liu, Wenhao
- Chemical Science, Vol. 3, Issue 6
Colloidal Spherical Quantum Wells with Near-Unity Photoluminescence Quantum Yield and Suppressed Blinking
journal, October 2016
- Jeong, Byeong Guk; Park, Young-Shin; Chang, Jun Hyuk
- ACS Nano, Vol. 10, Issue 10
Near-Unity Quantum Yields from Chloride Treated CdTe Colloidal Quantum Dots
journal, October 2014
- Page, Robert C.; Espinobarro-Velazquez, Daniel; Leontiadou, Marina A.
- Small, Vol. 11, Issue 13
Full-colour quantum dot displays fabricated by transfer printing
journal, February 2011
- Kim, Tae-Ho; Cho, Kyung-Sang; Lee, Eun Kyung
- Nature Photonics, Vol. 5, Issue 3
Light-emitting diodes made from cadmium selenide nanocrystals and a semiconducting polymer
journal, August 1994
- Colvin, V. L.; Schlamp, M. C.; Alivisatos, A. P.
- Nature, Vol. 370, Issue 6488
High-Power Genuine Ultraviolet Light-Emitting Diodes Based On Colloidal Nanocrystal Quantum Dots
journal, May 2015
- Kwak, Jeonghun; Lim, Jaehoon; Park, Myeongjin
- Nano Letters, Vol. 15, Issue 6
Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000
- Klimov, V. I.; Mikhailovsky, A. A.; Xu, Su
- Science, Vol. 290, Issue 5490, p. 314-317
Optical gain in colloidal quantum dots achieved with direct-current electrical pumping
journal, November 2017
- Lim, Jaehoon; Park, Young-Shin; Klimov, Victor I.
- Nature Materials, Vol. 17, Issue 1
Tandem luminescent solar concentrators based on engineered quantum dots
journal, January 2018
- Wu, Kaifeng; Li, Hongbo; Klimov, Victor I.
- Nature Photonics, Vol. 12, Issue 2
Quantum Dot Luminescent Concentrator Cavity Exhibiting 30-fold Concentration
journal, August 2015
- Bronstein, Noah D.; Yao, Yuan; Xu, Lu
- ACS Photonics, Vol. 2, Issue 11
Solid-state single-photon emitters
journal, September 2016
- Aharonovich, Igor; Englund, Dirk; Toth, Milos
- Nature Photonics, Vol. 10, Issue 10
Semiconductor Quantum Dots in Chemical Sensors and Biosensors
journal, September 2009
- Frasco, Manuela; Chaniotakis, Nikos
- Sensors, Vol. 9, Issue 9
Quantum dot bioconjugates for imaging, labelling and sensing
journal, June 2005
- Medintz, Igor L.; Uyeda, H. Tetsuo; Goldman, Ellen R.
- Nature Materials, Vol. 4, Issue 6, p. 435-446
Semiconductor quantum dots for in vitro diagnostics and cellular imaging
journal, July 2012
- Jin, Zongwen; Hildebrandt, Niko
- Trends in Biotechnology, Vol. 30, Issue 7
Towards non-blinking colloidal quantum dots
journal, June 2008
- Mahler, Benoit; Spinicelli, Piernicola; Buil, Stéphanie
- Nature Materials, Vol. 7, Issue 8
“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
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
Single-Dot Spectroscopy of Zinc-Blende CdSe/CdS Core/Shell Nanocrystals: Nonblinking and Correlation with Ensemble Measurements
journal, December 2013
- Qin, Haiyan; Niu, Yuan; Meng, Renyang
- Journal of the American Chemical Society, Vol. 136, Issue 1
Suppressed Auger Recombination in “Giant” Nanocrystals Boosts Optical Gain Performance
journal, October 2009
- García-Santamaría, Florencio; Chen, Yongfen; Vela, Javier
- Nano Letters, Vol. 9, Issue 10
Fluorescence intermittency in single cadmium selenide nanocrystals
journal, October 1996
- Nirmal, M.; Dabbousi, B. O.; Bawendi, M. G.
- Nature, Vol. 383, Issue 6603
“On”/“off” fluorescence intermittency of single semiconductor quantum dots
journal, July 2001
- Kuno, M.; Fromm, D. P.; Hamann, H. F.
- The Journal of Chemical Physics, Vol. 115, Issue 2
Random Telegraph Signal in the Photoluminescence Intensity of a Single Quantum Dot
journal, February 1997
- Efros, Al. L.; Rosen, M.
- Physical Review Letters, Vol. 78, Issue 6
Nano-engineered electron–hole exchange interaction controls exciton dynamics in core–shell semiconductor nanocrystals
journal, April 2011
- Brovelli, S.; Schaller, R. D.; Crooker, S. A.
- Nature Communications, Vol. 2, Issue 1
Quasiparticle band structures of six II-VI compounds: ZnS, ZnSe, ZnTe, CdS, CdSe, and CdTe
journal, October 1994
- Zakharov, Oleg; Rubio, Angel; Blase, X.
- Physical Review B, Vol. 50, Issue 15
(CdSe)ZnS Core−Shell Quantum Dots: Synthesis and Characterization of a Size Series of Highly Luminescent Nanocrystallites
journal, November 1997
- Dabbousi, B. O.; Rodriguez-Viejo, J.; Mikulec, F. V.
- The Journal of Physical Chemistry B, Vol. 101, Issue 46, p. 9463-9475
High-Pressure Structural Transformations in Semiconductor Nanocrystals
journal, October 1995
- Tolbert, Sarah H.; Alivisatos, A. P.
- Annual Review of Physical Chemistry, Vol. 46, Issue 1
Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy
journal, March 2017
- Fan, Fengjia; Voznyy, Oleksandr; Sabatini, Randy P.
- Nature, Vol. 544, Issue 7648
Size dependence of exciton fine structure in CdSe quantum dots
journal, June 1996
- Norris, D. J.; Efros, Al. L.; Rosen, M.
- Physical Review B, Vol. 53, Issue 24
Electronic structure and band parameters for Zn (, S, Se, Te)
journal, January 2006
- Karazhanov, S. Zh.; Ravindran, P.; Kjekhus, A.
- Journal of Crystal Growth, Vol. 287, Issue 1
Compressive strain induced heavy hole and light hole splitting of Zn1−xCdxSe epilayers grown by molecular beam epitaxy
journal, February 2003
- Yang, C. S.; Hsieh, Y. P.; Kuo, M. C.
- Materials Chemistry and Physics, Vol. 78, Issue 3
Strain-induced heavy-hole-to-light-hole energy splitting in (111) B pseudomorphic As quantum wells
journal, March 1993
- Moise, T. S.; Guido, L. J.; Barker, R. C.
- Physical Review B, Vol. 47, Issue 11
Electronic structure and optical properties of [(ZnSe (CdSe -ZnSe multiple quantum wells
journal, November 1994
- Ren, Shang-Fen; Xia, Jian-Bai; Han, He-Xiang
- Physical Review B, Vol. 50, Issue 19
Bright and Grey States in CdSe-CdS Nanocrystals Exhibiting Strongly Reduced Blinking
journal, March 2009
- Spinicelli, P.; Buil, S.; Quélin, X.
- Physical Review Letters, Vol. 102, Issue 13
Spectroscopy of single nanocrystals
journal, January 2014
- Fernée, Mark J.; Tamarat, Philippe; Lounis, Brahim
- Chemical Society Reviews, Vol. 43, Issue 4
Multiple temperature regimes of radiative decay in CdSe nanocrystal quantum dots: Intrinsic limits to the dark-exciton lifetime
journal, April 2003
- Crooker, S. A.; Barrick, T.; Hollingsworth, J. A.
- Applied Physics Letters, Vol. 82, Issue 17
Photogenerated Excitons in Plain Core CdSe Nanocrystals with Unity Radiative Decay in Single Channel: The Effects of Surface and Ligands
journal, March 2015
- Gao, Yuan; Peng, Xiaogang
- Journal of the American Chemical Society, Vol. 137, Issue 12
Photoluminescence Spectroscopy of Single CdSe Nanocrystallite Quantum Dots
journal, October 1996
- Empedocles, S. A.; Norris, D. J.; Bawendi, M. G.
- Physical Review Letters, Vol. 77, Issue 18
Spontaneous Spectral Diffusion in CdSe Quantum Dots
journal, June 2012
- Fernée, Mark J.; Plakhotnik, Taras; Louyer, Yann
- The Journal of Physical Chemistry Letters, Vol. 3, Issue 12
Electron−Phonon Coupling in CdSe Nanocrystals
journal, April 2010
- Kelley, Anne Myers
- The Journal of Physical Chemistry Letters, Vol. 1, Issue 9
Electron-phonon interactions and excitonic dephasing in semiconductor nanocrystals
journal, November 1993
- Takagahara, T.
- Physical Review Letters, Vol. 71, Issue 21
Suppression of Auger Processes in Confined Structures
journal, January 2010
- Cragg, George E.; Efros, Alexander L.
- Nano Letters, Vol. 10, Issue 1
Spectroscopy of Colloidal Semiconductor Core/Shell Nanoplatelets with High Quantum Yield
journal, June 2013
- Tessier, M. D.; Mahler, B.; Nadal, B.
- Nano Letters, Vol. 13, Issue 7
Single Cesium Lead Halide Perovskite Nanocrystals at Low Temperature: Fast Single-Photon Emission, Reduced Blinking, and Exciton Fine Structure
journal, January 2016
- Rainò, Gabriele; Nedelcu, Georgian; Protesescu, Loredana
- ACS Nano, Vol. 10, Issue 2
Room‐temperature exciton luminescence in II‐VI quantum wells
journal, June 1991
- Stanley, R. P.; Hawdon, B. J.; Hegarty, J.
- Applied Physics Letters, Vol. 58, Issue 25
Observation of free excitons in room‐temperature photoluminescence of GaAs/AlGaAs single quantum wells
journal, August 1988
- Fujiwara, K.; Tsukada, N.; Nakayama, T.
- Applied Physics Letters, Vol. 53, Issue 8
Synthesis and Characterization of Strongly Luminescing ZnS-Capped CdSe Nanocrystals
journal, January 1996
- Hines, Margaret A.; Guyot-Sionnest, Philippe
- The Journal of Physical Chemistry, Vol. 100, Issue 2, p. 468-471
Raman-scattering study of exciton-phonon coupling in PbS nanocrystals
journal, April 1997
- Krauss, Todd D.; Wise, Frank W.
- Physical Review B, Vol. 55, Issue 15
Evolution of the Single-Nanocrystal Photoluminescence Linewidth with Size and Shell: Implications for Exciton–Phonon Coupling and the Optimization of Spectral Linewidths
journal, December 2015
- Cui, Jian; Beyler, Andrew P.; Coropceanu, Igor
- Nano Letters, Vol. 16, Issue 1
Electron–Phonon Coupling in CdSe Nanocrystals from an Atomistic Phonon Model
journal, May 2011
- Kelley, Anne Myers
- ACS Nano, Vol. 5, Issue 6
Theory of the linear and nonlinear optical properties of semiconductor microcrystallites
journal, May 1987
- Schmitt-Rink, S.; Miller, D. A. B.; Chemla, D. S.
- Physical Review B, Vol. 35, Issue 15
Works referencing / citing this record:
Exceptionally stable quantum dot/siloxane hybrid encapsulation material for white light-emitting diodes with a wide color gamut
journal, January 2019
- Jang, Junho; Yoon, Da-Eun; Kang, Seung-Mo
- Nanoscale, Vol. 11, Issue 31
III–V colloidal nanocrystals: control of covalent surfaces
journal, January 2020
- Kim, Youngsik; Chang, Jun Hyuk; Choi, Hyekyoung
- Chemical Science, Vol. 11, Issue 4
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
Black phosphorus @ molybdenum disulfide 2D nanocomposite with broad light absorption and high stability for methylene blue decomposition photocatalyst
journal, January 2020
- Jeong, Rak Hyun; Lee, Ji Won; Kim, Dong In
- Nanotechnology, Vol. 31, Issue 15
Electrochemically-stable ligands bridge photoluminescence-electroluminescence gap of quantum dots
text, January 2019
- Pu, Chaodan; Dai, Xingliang; Shu, Yufei
- arXiv