DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Towards zero-threshold optical gain using charged semiconductor quantum dots

Abstract

Colloidal semiconductor quantum dots are attractive materials for the realization of solution-processable lasers. However, their applications as optical-gain media are complicated by a non-unity degeneracy of band-edge states, because of which multiexcitons are required to achieve the lasing regime. This increases the lasing thresholds and leads to very short optical gain lifetimes limited by nonradiative Auger recombination. Here, we show that these problems can be at least partially resolved by employing not neutral but negatively charged quantum dots. By applying photodoping to specially engineered quantum dots with impeded Auger decay, we demonstrate a considerable reduction of the optical gain threshold due to suppression of ground-state absorption by pre-existing carriers. Moreover, by injecting approximately one electron per dot on average, we achieve a more than twofold reduction in the amplified spontaneous emission threshold, bringing it to the sub-single-exciton level. Furthermore, these measurements indicate the feasibility of ‘zero-threshold’ gain achievable by completely blocking the band-edge state with two electrons.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chinese Academy of Sciences, Dalian (China)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
  3. 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 Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1415416
Report Number(s):
LA-UR-17-26002
Journal ID: ISSN 1748-3387; TRN: US1800810
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Nature Nanotechnology
Additional Journal Information:
Journal Volume: 12; Journal Issue: 12; Journal ID: ISSN 1748-3387
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Material Science; Zero-threshold optical gain, colloidal quantum dot, lasing

Citation Formats

Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor Ivanovich. Towards zero-threshold optical gain using charged semiconductor quantum dots. United States: N. p., 2017. Web. doi:10.1038/nnano.2017.189.
Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, & Klimov, Victor Ivanovich. Towards zero-threshold optical gain using charged semiconductor quantum dots. United States. https://doi.org/10.1038/nnano.2017.189
Wu, Kaifeng, Park, Young -Shin, Lim, Jaehoon, and Klimov, Victor Ivanovich. Mon . "Towards zero-threshold optical gain using charged semiconductor quantum dots". United States. https://doi.org/10.1038/nnano.2017.189. https://www.osti.gov/servlets/purl/1415416.
@article{osti_1415416,
title = {Towards zero-threshold optical gain using charged semiconductor quantum dots},
author = {Wu, Kaifeng and Park, Young -Shin and Lim, Jaehoon and Klimov, Victor Ivanovich},
abstractNote = {Colloidal semiconductor quantum dots are attractive materials for the realization of solution-processable lasers. However, their applications as optical-gain media are complicated by a non-unity degeneracy of band-edge states, because of which multiexcitons are required to achieve the lasing regime. This increases the lasing thresholds and leads to very short optical gain lifetimes limited by nonradiative Auger recombination. Here, we show that these problems can be at least partially resolved by employing not neutral but negatively charged quantum dots. By applying photodoping to specially engineered quantum dots with impeded Auger decay, we demonstrate a considerable reduction of the optical gain threshold due to suppression of ground-state absorption by pre-existing carriers. Moreover, by injecting approximately one electron per dot on average, we achieve a more than twofold reduction in the amplified spontaneous emission threshold, bringing it to the sub-single-exciton level. Furthermore, these measurements indicate the feasibility of ‘zero-threshold’ gain achievable by completely blocking the band-edge state with two electrons.},
doi = {10.1038/nnano.2017.189},
journal = {Nature Nanotechnology},
number = 12,
volume = 12,
place = {United States},
year = {2017},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 90 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Continuous-wave biexciton lasing at room temperature using solution-processed quantum wells
journal, October 2014

  • Grim, Joel Q.; Christodoulou, Sotirios; Di Stasio, Francesco
  • Nature Nanotechnology, Vol. 9, Issue 11
  • DOI: 10.1038/nnano.2014.213

Electrochromic Nanocrystal Quantum Dots
journal, March 2001


Gradient CdSe/CdS Quantum Dots with Room Temperature Biexciton Unity Quantum Yield
journal, May 2015


Optical Gain and Stimulated Emission in Nanocrystal Quantum Dots
journal, October 2000


Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals
journal, May 2009


Heavily-doped semiconductor lasers
journal, November 1981


Gain and the threshold of three-dimensional quantum-box lasers
journal, September 1986

  • Asada, M.; Miyamoto, Y.; Suematsu, Y.
  • IEEE Journal of Quantum Electronics, Vol. 22, Issue 9
  • DOI: 10.1109/JQE.1986.1073149

Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Nanocrystals
journal, July 2000

  • Klimov, Victor I.
  • The Journal of Physical Chemistry B, Vol. 104, Issue 26
  • DOI: 10.1021/jp9944132

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
  • DOI: 10.1021/jp0311660

Controlling the Surface of Semiconductor Nanocrystals for Efficient Light Emission from Single Excitons to Multiexcitons
journal, June 2015

  • Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M.
  • The Journal of Physical Chemistry C, Vol. 119, Issue 28
  • DOI: 10.1021/acs.jpcc.5b03853

Interfacial Electronic Structure in Graded Shell Nanocrystals Dictates Their Performance for Optical Gain
journal, August 2016

  • Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M.
  • The Journal of Physical Chemistry C, Vol. 120, Issue 34
  • DOI: 10.1021/acs.jpcc.6b05836

Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots
journal, February 2000


Heavily doped n-type PbSe and PbS nanocrystals using ground-state charge transfer from cobaltocene
journal, June 2013

  • Koh, Weon-kyu; Koposov, Alexey Y.; Stewart, John T.
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02004

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
  • DOI: 10.1038/nature21424

Low-Threshold Stimulated Emission Using Colloidal Quantum Wells
journal, April 2014

  • She, Chunxing; Fedin, Igor; Dolzhnikov, Dmitriy S.
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500775p

Color-selective semiconductor nanocrystal laser
journal, June 2002

  • Eisler, Hans-Jürgen; Sundar, Vikram C.; Bawendi, Moungi G.
  • Applied Physics Letters, Vol. 80, Issue 24
  • DOI: 10.1063/1.1485125

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
  • DOI: 10.1021/nl901681d

Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors
journal, April 2015

  • Zhu, Haiming; Fu, Yongping; Meng, Fei
  • Nature Materials, Vol. 14, Issue 6
  • DOI: 10.1038/nmat4271

Spectroscopic and Device Aspects of Nanocrystal Quantum Dots
journal, September 2016


Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites
journal, August 2015

  • Yakunin, Sergii; Protesescu, Loredana; Krieg, Franziska
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9056

Synthesis of CdSe and CdTe Nanocrystals without Precursor Injection
journal, October 2005

  • Yang, Yongan Andrew; Wu, Huimeng; Williams, Kathryn R.
  • Angewandte Chemie International Edition, Vol. 44, Issue 41
  • DOI: 10.1002/anie.200502279

n-type colloidal semiconductor nanocrystals
journal, October 2000

  • Shim, Moonsub; Guyot-Sionnest, Philippe
  • Nature, Vol. 407, Issue 6807
  • DOI: 10.1038/35039577

Exciton-Exciton Interaction and Optical Gain in Colloidal CdSe/CdS Dot/Rod Nanocrystals
journal, August 2009

  • Saba, Michele; Minniberger, Stefan; Quochi, Francesco
  • Advanced Materials, Vol. 21, Issue 48, p. 4942-4946
  • DOI: 10.1002/adma.200901482

Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots
journal, November 2011

  • Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea
  • Nature, Vol. 479, Issue 7372
  • DOI: 10.1038/nature10569

Size Dependence of Negative Trion Auger Recombination in Photodoped CdSe Nanocrystals
journal, December 2013

  • Cohn, Alicia W.; Rinehart, Jeffrey D.; Schimpf, Alina M.
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl4041675

Enhancement of optical gain characteristics of quantum dot films by optimization of organic ligands
journal, January 2016

  • Malak, Sidney T.; Lafalce, Evan; Jung, Jaehan
  • Journal of Materials Chemistry C, Vol. 4, Issue 42
  • DOI: 10.1039/C6TC03148J

Single-exciton optical gain in semiconductor nanocrystals
journal, May 2007

  • Klimov, Victor I.; Ivanov, Sergei A.; Nanda, Jagjit
  • Nature, Vol. 447, Issue 7143
  • DOI: 10.1038/nature05839

Electron and hole relaxation pathways in semiconductor quantum dots
journal, November 1999


Light Emission and Amplification in Charged CdSe Quantum Dots
journal, July 2004

  • Wang, Congjun; Wehrenberg, Brian L.; Woo, Chui Y.
  • The Journal of Physical Chemistry B, Vol. 108, Issue 26
  • DOI: 10.1021/jp0489830

Room-Temperature, Tunable Gain Media from Novel II–VI Nanocrystal–Titania Composite Matrices
journal, May 2002


Evidence for the Role of Holes in Blinking: Negative and Oxidized CdSe/CdS Dots
journal, September 2012

  • Qin, Wei; Guyot-Sionnest, Philippe
  • ACS Nano, Vol. 6, Issue 10
  • DOI: 10.1021/nn303396c

What future for quantum dot-based light emitters?
journal, December 2015


High-Performance, Quantum Dot Nanocomposites for Nonlinear Optical and Optical Gain Applications
journal, April 2003

  • Petruska, M. A.; Malko, A. V.; Voyles, P. M.
  • Advanced Materials, Vol. 15, Issue 78, p. 610-613
  • DOI: 10.1002/adma.200304450

Auger Recombination of Biexcitons and Negative and Positive Trions in Individual Quantum Dots
journal, June 2014

  • Park, Young-Shin; Bae, Wan Ki; Pietryga, Jeffrey M.
  • ACS Nano, Vol. 8, Issue 7
  • DOI: 10.1021/nn5023473

Perovskite photonic sources
journal, April 2016


Suppression of Auger Processes in Confined Structures
journal, January 2010

  • Cragg, George E.; Efros, Alexander L.
  • Nano Letters, Vol. 10, Issue 1
  • DOI: 10.1021/nl903592h

Effect of the Core/Shell Interface on Auger Recombination Evaluated by Single-Quantum-Dot Spectroscopy
journal, January 2014

  • Park, Young-Shin; Bae, Wan Ki; Padilha, Lazaro A.
  • Nano Letters, Vol. 14, Issue 2
  • DOI: 10.1021/nl403289w

Effect of Auger Recombination on Lasing in Heterostructured Quantum Dots with Engineered Core/Shell Interfaces
journal, October 2015


Continuous-Wave Pumping of Multiexciton Bands in the Photoluminescence Spectrum of a Single CdTe-CdSe Core-Shell Colloidal Quantum Dot
journal, May 2009


From amplified spontaneous emission to microring lasing using nanocrystal quantum dot solids
journal, August 2002

  • Malko, A. V.; Mikhailovsky, A. A.; Petruska, M. A.
  • Applied Physics Letters, Vol. 81, Issue 7
  • DOI: 10.1063/1.1497708

Trion Decay in Colloidal Quantum Dots
journal, March 2009

  • Jha, Praket P.; Guyot-Sionnest, Philippe
  • ACS Nano, Vol. 3, Issue 4
  • DOI: 10.1021/nn9001177

Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals
journal, February 2013


Photochemical Electronic Doping of Colloidal CdSe Nanocrystals
journal, December 2013

  • Rinehart, Jeffrey D.; Schimpf, Alina M.; Weaver, Amanda L.
  • Journal of the American Chemical Society, Vol. 135, Issue 50
  • DOI: 10.1021/ja410825c

Controlled Alloying of the Core–Shell Interface in CdSe/CdS Quantum Dots for Suppression of Auger Recombination
journal, April 2013

  • Bae, Wan Ki; Padilha, Lazaro A.; Park, Young-Shin
  • ACS Nano, Vol. 7, Issue 4
  • DOI: 10.1021/nn4002825

Influence of doping on threshold current of semiconductor lasers
journal, January 1985


Measurement and assignment of the size-dependent optical spectrum in CdSe quantum dots
journal, June 1996


Synthesis of CdSe and CdTe Nanocrystals without Precursor Injection
journal, October 2005

  • Yang, Yongan Andrew; Wu, Huimeng; Williams, Kathryn R.
  • Angewandte Chemie, Vol. 117, Issue 41
  • DOI: 10.1002/ange.200502279

Near-Field Energy Transfer Using Nanoemitters For Optoelectronics
journal, October 2016

  • Guzelturk, Burak; Demir, Hilmi Volkan
  • Advanced Functional Materials, Vol. 26, Issue 45
  • DOI: 10.1002/adfm.201603311

All-Inorganic Colloidal Perovskite Quantum Dots: A New Class of Lasing Materials with Favorable Characteristics
journal, October 2015


Near-Unity Emitting Copper-Doped Colloidal Semiconductor Quantum Wells for Luminescent Solar Concentrators
journal, June 2017

  • Sharma, Manoj; Gungor, Kivanc; Yeltik, Aydan
  • Advanced Materials, Vol. 29, Issue 30
  • DOI: 10.1002/adma.201700821

Tunable Near-Infrared Optical Gain and Amplified Spontaneous Emission Using PbSe Nanocrystals.
journal, March 2004


Evidence for Fast Interlayer Energy Transfer in MoSe 2 /WS 2 Heterostructures
journal, June 2016


Unusual Exciton–Phonon Interactions at van der Waals Engineered Interfaces
journal, January 2017


Colloidal-Quantum-Dot Ring Lasers with Active Color Control
journal, January 2018


Giant Modal Gain Coefficients in Colloidal II–VI Nanoplatelets
journal, December 2018


Orientation-Controlled Nonradiative Energy Transfer to Colloidal Nanoplatelets: Engineering Dipole Orientation Factor
journal, June 2019


An All-Optical Excitonic Switch Operated in the Liquid and Solid Phases
journal, February 2019

  • Kellis, Donald L.; Sarter, Christopher; Cannon, Brittany L.
  • ACS Nano, Vol. 13, Issue 3
  • DOI: 10.1021/acsnano.8b07504

Core/Shell Colloidal Semiconductor Nanoplatelets
journal, November 2012

  • Mahler, Benoit; Nadal, Brice; Bouet, Cecile
  • Journal of the American Chemical Society, Vol. 134, Issue 45
  • DOI: 10.1021/ja307944d

DNA-Controlled Excitonic Switches
journal, January 2012

  • Graugnard, Elton; Kellis, Donald L.; Bui, Hieu
  • Nano Letters, Vol. 12, Issue 4
  • DOI: 10.1021/nl3004336

Electronic Structure and Exciton–Phonon Interaction in Two-Dimensional Colloidal CdSe Nanosheets
journal, May 2012

  • Achtstein, Alexander W.; Schliwa, Andrei; Prudnikau, Anatol
  • Nano Letters, Vol. 12, Issue 6
  • DOI: 10.1021/nl301071n

Amplified Spontaneous Emission and Lasing in Colloidal Nanoplatelets
journal, June 2014

  • Guzelturk, Burak; Kelestemur, Yusuf; Olutas, Murat
  • ACS Nano, Vol. 8, Issue 7
  • DOI: 10.1021/nn5022296

Low-temperature solution-processed wavelength-tunable perovskites for lasing
journal, March 2014

  • Xing, Guichuan; Mathews, Nripan; Lim, Swee Sien
  • Nature Materials, Vol. 13, Issue 5
  • DOI: 10.1038/nmat3911

Picosecond energy transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids
journal, March 2015

  • Rowland, Clare E.; Fedin, Igor; Zhang, Hui
  • Nature Materials, Vol. 14, Issue 5
  • DOI: 10.1038/nmat4231

Continuous-wave infrared optical gain and amplified spontaneous emission at ultralow threshold by colloidal HgTe quantum dots
journal, October 2017

  • Geiregat, Pieter; Houtepen, Arjan J.; Sagar, Laxmi Kishore
  • Nature Materials, Vol. 17, Issue 1
  • DOI: 10.1038/nmat5000

Red, green and blue lasing enabled by single-exciton gain in colloidal quantum dot films
journal, April 2012

  • Dang, Cuong; Lee, Joonhee; Breen, Craig
  • Nature Nanotechnology, Vol. 7, Issue 5
  • DOI: 10.1038/nnano.2012.61

Excitonic interconnects
journal, October 2009


Exciton–polariton spin switches
journal, April 2010


Room-temperature electrical control of exciton flux in a van der Waals heterostructure
journal, July 2018


Dynamic control of Förster energy transfer in a photonic environment
journal, January 2014

  • Schleifenbaum, Frank; Kern, Andreas M.; Konrad, Alexander
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 25
  • DOI: 10.1039/c4cp01306a

Nonradiative energy transfer in colloidal CdSe nanoplatelet films
journal, January 2015

  • Guzelturk, Burak; Olutas, Murat; Delikanli, Savas
  • Nanoscale, Vol. 7, Issue 6
  • DOI: 10.1039/c4nr06003b

Temperature-dependent optoelectronic properties of quasi-2D colloidal cadmium selenide nanoplatelets
journal, January 2017

  • Bose, Sumanta; Shendre, Sushant; Song, Zhigang
  • Nanoscale, Vol. 9, Issue 19
  • DOI: 10.1039/c7nr00163k

Low-threshold lasing from colloidal CdSe/CdSeTe core/alloyed-crown type-II heteronanoplatelets
journal, January 2018

  • Gao, Yuan; Li, Mingjie; Delikanli, Savas
  • Nanoscale, Vol. 10, Issue 20
  • DOI: 10.1039/c8nr01838c

Realization of a Double-Barrier Resonant Tunneling Diode for Cavity Polaritons
journal, June 2013


Electronic Energy Transfer in CdSe Quantum Dot Solids
journal, April 1996


Control of Exciton Fluxes in an Excitonic Integrated Circuit
journal, July 2008


Optically Controlled Excitonic Transistor
conference, January 2014


Excitonic Switches Operating at Around 100 K
conference, January 2010

  • Grosso, Gabriele; Graves, Joe C.; Hammack, Aaron T.
  • Quantum Electronics and Laser Science Conference, Conference on Lasers and Electro-Optics 2010
  • DOI: 10.1364/qels.2010.qfi5

Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites
text, January 2015


Low-threshold stimulated emission using colloidal quantum wells
text, January 2013


Works referencing / citing this record:

Coreless Fiber‐Based Whispering‐Gallery‐Mode Assisted Lasing from Colloidal Quantum Well Solids
journal, November 2019

  • Sak, Mustafa; Taghipour, Nima; Delikanli, Savas
  • Advanced Functional Materials, Vol. 30, Issue 1
  • DOI: 10.1002/adfm.201907417

Ultrafast Dynamics of Charge Transfer and Photochemical Reactions in Solar Energy Conversion
journal, October 2018


White Photoluminescent Ti 3 C 2 MXene Quantum Dots with Two‐Photon Fluorescence
journal, March 2019


Coherent Spectroscopy of Multiple Excitons in Colloidal Nanocrystal Quantum Dots
journal, June 2019


Acquisition of Hyperspectral Data with Colloidal Quantum Dots
journal, October 2019

  • Tang, Xin; Ackerman, Matthew M.; Guyot‐Sionnest, Philippe
  • Laser & Photonics Reviews, Vol. 13, Issue 11
  • DOI: 10.1002/lpor.201900165

All-optical control of exciton flow in a colloidal quantum well complex
journal, February 2020


A bright future for colloidal quantum dot lasers
journal, August 2019


Dual-band infrared imaging using stacked colloidal quantum dot photodiodes
journal, February 2019


Pattern-assisted stacking colloidal quantum dots for photonic integrated circuits
journal, January 2019


Near-infrared aggregation-induced enhanced electrochemiluminescence from tetraphenylethylene nanocrystals: a new generation of ECL emitters
journal, January 2019

  • Liu, Jia-Li; Zhang, Jia-Qi; Tang, Zhi-Ling
  • Chemical Science, Vol. 10, Issue 16
  • DOI: 10.1039/c9sc00084d

Trion dynamics in lead halide perovskite nanocrystals
journal, November 2019

  • Kanemitsu, Yoshihiko
  • The Journal of Chemical Physics, Vol. 151, Issue 17
  • DOI: 10.1063/1.5125628

Observation of positive and negative trions in organic-inorganic hybrid perovskite nanocrystals
journal, November 2018


Electrically control amplified spontaneous emission in colloidal quantum dots
journal, October 2019


Sub–single-exciton lasing using charged quantum dots coupled to a distributed feedback cavity
journal, August 2019


Spectroscopic Evidence for the Contribution of Holes to the Bleach of Cd-Chalcogenide Quantum Dots
journal, March 2019


Lasing Supraparticles Self-Assembled from Nanocrystals
journal, November 2018


All-optical control of exciton flow in a colloidal quantum well complex
journal, February 2020


Excitonic complexes and optical gain in two-dimensional molybdenum ditelluride well below the Mott transition
journal, March 2020


Electrically control amplified spontaneous emission in colloidal quantum dots
journal, October 2019