Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

Diroll, Benjamin T.; Cassidy, James P.; Harankahage, Dulanjan; Hua, Muchuan; Lin, Xiao-Min; Zamkov, Mikhail

doi:10.1039/d3nr04203k

Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

Journal Article · Wed Nov 08 00:00:00 EST 2023 · Nanoscale

DOI:https://doi.org/10.1039/d3nr04203k· OSTI ID:2569775

^[1]; Cassidy, James P. ^[2]; Harankahage, Dulanjan ^[2]; ^[1]; ^[1]; ^[2]

Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Bowling Green State Univ., OH (United States)

Colloidal quantum shells are spherical semiconductor quantum wells, which have shown strong promise as optical materials, particularly in classes of experiments requiring multiple excitons. The two-photon properties of CdS/CdSe/CdS quantum shell samples are studied here to demonstrate large non-linear absorption cross-sections while retaining advantageous multiexciton physics conferred by the geometrical structure. The quantum shells have large two-phonon cross sections (0.4–7.9 × 10⁶ GM), which highlights their potential use in upconversion imaging in which large per particle two-photon absorption is critical. Time-resolved measurements confirmed that the quantum shells have long biexciton lifetime (>10 ns in the largest core samples reported here) and large gain bandwidth (>300 meV). The combination of these attributes with large two-photon cross sections makes the CdS/CdSe/CdS quantum shells excellent gain media for two-photon excitation. With a broad gain bandwidth and long gain lifetime, quantum shell solids support multimodal amplified spontaneous emission from excitons, biexcitons, and higher excited states. In conclusion, thresholds for amplified spontaneous emission and lasing, which are as low as 1 mJ cm⁻², are comparable to, or lower than, the thresholds reported for other colloidal materials.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0016872

OSTI ID:: 2569775

Alternate ID(s):: OSTI ID: 2205242

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 45 Vol. 15; ISSN 2040-3364; ISSN 2040-3372

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

References (68)

Two-Photon Pumped Lasing from a Two-Dimensional Photonic Bandgap Structure with Polymeric Gain Material Bauer, C.; Schnabel, B.; Kley, E. -B. Advanced Materials, Vol. 14, Issue 9 https://doi.org/10.1002/1521-4095(20020503)14:9<673::AID-ADMA673>3.0.CO;2-F	journal	May 2002
Highly Efficient Amplified Stimulated Emission from CdSe-CdS-ZnS Quantum Dot Doped Waveguides with Two-Photon Infrared Optical Pumping Jasieniak, J. J.; Fortunati, I.; Gardin, S. Advanced Materials, Vol. 20, Issue 1 https://doi.org/10.1002/adma.200701582	journal	January 2008
Stimulated Emission and Lasing from CdSe/CdS/ZnS Core-Multi-Shell Quantum Dots by Simultaneous Three-Photon Absorption Wang, Yue; Ta, Van Duong; Gao, Yuan Advanced Materials, Vol. 26, Issue 18 https://doi.org/10.1002/adma.201305125	journal	February 2014
Stable and Low-Threshold Optical Gain in CdSe/CdS Quantum Dots: An All-Colloidal Frequency Up-Converted Laser Guzelturk, Burak; Kelestemur, Yusuf; Gungor, Kivanc Advanced Materials, Vol. 27, Issue 17 https://doi.org/10.1002/adma.201500418	journal	March 2015
Colloidal Two-Dimensional Systems: CdSe Quantum Shells and Wells Battaglia, David; Li, Jack J.; Wang, Yunjun Angewandte Chemie International Edition, Vol. 42, Issue 41, p. 5035-5039 https://doi.org/10.1002/anie.200352120	journal	October 2003
A quantum dot quantum well: CdS/HgS/CdS Eychmüller, A.; Mews, A.; Weller, H. Chemical Physics Letters, Vol. 208, Issue 1-2 https://doi.org/10.1016/0009-2614(93)80076-2	journal	June 1993
Dispersion of the two-photon cross section in rhodamine dyes Hermann, J. P.; Ducuing, J. Optics Communications, Vol. 6, Issue 2 https://doi.org/10.1016/0030-4018(72)90204-0	journal	October 1972
Transfer times of electrons and holes across the interface in CdS/HgS/CdS quantum dot quantum well nanoparticles Braun, Markus; Link, Stephan; Burda, Clemens Chemical Physics Letters, Vol. 361, Issue 5-6 https://doi.org/10.1016/S0009-2614(02)01001-1	journal	August 2002
Ligand-Dependent Tuning of Interband and Intersubband Transitions of Colloidal CdSe Nanoplatelets Diroll, Benjamin T. Chemistry of Materials, Vol. 32, Issue 13 https://doi.org/10.1021/acs.chemmater.0c02305	journal	June 2020
Statistical Description of CdSe/CdS Dot-in-Rod Heterostructures Using Scanning Transmission Electron Microscopy Diroll, Benjamin T.; Gogotsi, Natalie; Murray, Christopher B. Chemistry of Materials, Vol. 28, Issue 10 https://doi.org/10.1021/acs.chemmater.6b00376	journal	May 2016
Highly Stable Multicrown Heterostructures of Type-II Nanoplatelets for Ultralow Threshold Optical Gain Dede, Didem; Taghipour, Nima; Quliyeva, Ulviyya Chemistry of Materials, Vol. 31, Issue 5 https://doi.org/10.1021/acs.chemmater.9b00136	journal	February 2019
Multicarrier Dynamics in Quantum Dots Melnychuk, Christopher; Guyot-Sionnest, Philippe Chemical Reviews, Vol. 121, Issue 4 https://doi.org/10.1021/acs.chemrev.0c00931	journal	January 2021
Two-Photon Absorption and Photoluminescence of Individual CsPbBr₃ Nanocrystal Superlattices Ban, Jieting; Yu, Ying; Yue, Peng The Journal of Physical Chemistry C, Vol. 126, Issue 19 https://doi.org/10.1021/acs.jpcc.2c01693	journal	May 2022
Thermodynamic Equilibrium between Excitons and Excitonic Molecules Dictates Optical Gain in Colloidal CdSe Quantum Wells Geiregat, Pieter; Tomar, Renu; Chen, Kai The Journal of Physical Chemistry Letters, Vol. 10, Issue 13 https://doi.org/10.1021/acs.jpclett.9b01607	journal	June 2019
Frequency Stabilization and Optically Tunable Lasing in Colloidal Quantum Dot Superparticles Neuhaus, Steven J.; Marino, Emanuele; Murray, Christopher B. Nano Letters, Vol. 23, Issue 2 https://doi.org/10.1021/acs.nanolett.2c04498	journal	January 2023
Two Photon Absorption in II–VI Semiconductors: The Influence of Dimensionality and Size Scott, Riccardo; Achtstein, Alexander W.; Prudnikau, Anatol Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b00966	journal	July 2015
Colloidal Quantum Shells: An Emerging 2D Semiconductor for Energy Applications Cassidy, James; Harankahage, Dulanjan; Porotnikov, Dmitry ACS Energy Letters, Vol. 7, Issue 3 https://doi.org/10.1021/acsenergylett.2c00153	journal	March 2022
Quantum Shells Boost the Optical Gain of Lasing Media Cassidy, James; Diroll, Benjamin T.; Mondal, Navendu ACS Nano, Vol. 16, Issue 2 https://doi.org/10.1021/acsnano.1c10404	journal	February 2022
Lateral Size-Dependent Spontaneous and Stimulated Emission Properties in Colloidal CdSe Nanoplatelets Olutas, Murat; Guzelturk, Burak; Kelestemur, Yusuf ACS Nano, Vol. 9, Issue 5 https://doi.org/10.1021/acsnano.5b01927	journal	May 2015
Red, Yellow, Green, and Blue Amplified Spontaneous Emission and Lasing Using Colloidal CdSe Nanoplatelets She, Chunxing; Fedin, Igor; Dolzhnikov, Dmitriy S. ACS Nano, Vol. 9, Issue 10 https://doi.org/10.1021/acsnano.5b02509	journal	September 2015
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
Suppression of the Auger Recombination Process in CdSe/CdS Core/Shell Nanocrystals He, Yan; Hu, Sumei; Han, Taikun ACS Omega, Vol. 4, Issue 5 https://doi.org/10.1021/acsomega.9b00926	journal	May 2019
Efficient Optical Gain in Spherical Quantum Wells Enabled by Engineering Biexciton Interactions Nagamine, Gabriel; Jeong, Byeong Guk; Ferreira, Tomas A. C. ACS Photonics, Vol. 7, Issue 8 https://doi.org/10.1021/acsphotonics.0c00812	journal	July 2020
Sample Concentration Affects Optical Gain Results in Colloidal Nanomaterials: Circumventing the Distortions by Below Band Gap Excitation Nagamine, Gabriel; Ferreira, Tomas A. C.; Almeida, Diogo B. ACS Photonics, Vol. 9, Issue 1 https://doi.org/10.1021/acsphotonics.1c01293	journal	December 2021
Two-Photon Pumped Amplified Spontaneous Emission and Lasing from Formamidinium Lead Bromine Nanocrystals Liu, Zhengzheng; Hu, Zhiping; Zhang, Zeyu ACS Photonics, Vol. 6, Issue 12 https://doi.org/10.1021/acsphotonics.9b01226	journal	November 2019
Multiphoton Absorbing Materials: Molecular Designs, Characterizations, and Applications He, Guang S.; Tan, Loon-Seng; Zheng, Qingdong Chemical Reviews, Vol. 108, Issue 4 https://doi.org/10.1021/cr050054x	journal	April 2008
Chemistry and photophysics of mixed cadmium sulfide/mercury sulfide colloids Haesselbarth, A.; Eychmueller, A.; Eichberger, R. The Journal of Physical Chemistry, Vol. 97, Issue 20 https://doi.org/10.1021/j100122a026	journal	May 1993
Coupled and Decoupled Dual Quantum Systems in One Semiconductor Nanocrystal Battaglia, David; Blackman, Bridgette; Peng, Xiaogang Journal of the American Chemical Society, Vol. 127, Issue 31 https://doi.org/10.1021/ja0437297	journal	August 2005
Type-II Core/Shell CdS/ZnSe Nanocrystals: Synthesis, Electronic Structures, and Spectroscopic Properties Ivanov, Sergei A.; Piryatinski, Andrei; Nanda, Jagjit Journal of the American Chemical Society, Vol. 129, Issue 38 https://doi.org/10.1021/ja068351m	journal	September 2007
Two-Photon Pumped Lasing in Single-Crystal Organic Nanowire Exciton Polariton Resonators Zhang, Chuang; Zou, Chang-Ling; Yan, Yongli Journal of the American Chemical Society, Vol. 133, Issue 19 https://doi.org/10.1021/ja200549v	journal	April 2011
Two-Photon-Pumped Perovskite Semiconductor Nanocrystal Lasers Xu, Yanqing; Chen, Qi; Zhang, Chunfeng Journal of the American Chemical Society, Vol. 138, Issue 11 https://doi.org/10.1021/jacs.5b12662	journal	March 2016
One-Dimensional Carrier Confinement in “Giant” CdS/CdSe Excitonic Nanoshells Razgoniaeva, Natalia; Moroz, Pavel; Yang, Mingrui Journal of the American Chemical Society, Vol. 139, Issue 23 https://doi.org/10.1021/jacs.7b02054	journal	June 2017
Light Emission and Amplification in Charged CdSe Quantum Dots Wang, Congjun; Wehrenberg, Brian L.; Woo, Chui Y. The Journal of Physical Chemistry B, Vol. 108, Issue 26 https://doi.org/10.1021/jp0489830	journal	July 2004
Improving Optical Gain Performance in Semiconductor Quantum Dots via Coupled Quantum Shells Dias, Eva A.; Saari, Jonathan I.; Tyagi, Pooja The Journal of Physical Chemistry C, Vol. 116, Issue 9 https://doi.org/10.1021/jp211325x	journal	February 2012
One- and Two-Photon Absorption in CdS Nanodots and Wires: The Role of Dimensionality in the One- and Two-Photon Luminescence Excitation Spectrum Achtstein, Alexander W.; Ballester, Ana; Movilla, Jose L. The Journal of Physical Chemistry C, Vol. 119, Issue 2 https://doi.org/10.1021/jp511346w	journal	December 2014
Ultralow Threshold One-Photon- and Two-Photon-Pumped Optical Gain Media of Blue-Emitting Colloidal Quantum Dot Films Guzelturk, Burak; Kelestemur, Yusuf; Akgul, Mehmet Zafer The Journal of Physical Chemistry Letters, Vol. 5, Issue 13 https://doi.org/10.1021/jz500726h	journal	June 2014
Effect of the Core/Shell Interface on Auger Recombination Evaluated by Single-Quantum-Dot Spectroscopy Park, Young-Shin; Bae, Wan Ki; Padilha, Lazaro A. Nano Letters, Vol. 14, Issue 2 https://doi.org/10.1021/nl403289w	journal	January 2014
Multiexciton Engineering in Seeded Core/Shell Nanorods: Transfer from Type-I to Quasi-type-II Regimes Sitt, Amit; Sala, Fabio Della; Menagen, Gabi Nano Letters, Vol. 9, Issue 10 https://doi.org/10.1021/nl901679q	journal	October 2009
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
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
Ultralow-Threshold Two-Photon Pumped Amplified Spontaneous Emission and Lasing from Seeded CdSe/CdS Nanorod Heterostructures Xing, Guichuan; Liao, Yile; Wu, Xiangyang ACS Nano, Vol. 6, Issue 12 https://doi.org/10.1021/nn304200a	journal	November 2012
Two-Photon-Induced Blue Shift of Core and Shell Optical Transitions in Colloidal CdSe/CdS Quasi-Type II Quantum Rods Allione, Marco; Ballester, Ana; Li, Hongbo ACS Nano, Vol. 7, Issue 3 https://doi.org/10.1021/nn3057559	journal	March 2013
Amplified Spontaneous Emission and Lasing in Colloidal Nanoplatelets Guzelturk, Burak; Kelestemur, Yusuf; Olutas, Murat ACS Nano, Vol. 8, Issue 7 https://doi.org/10.1021/nn5022296	journal	June 2014
Observation of stimulated emission by direct three-photon excitation He, Guang S.; Markowicz, Przemyslaw P.; Lin, Tzu-Chau Nature, Vol. 415, Issue 6873 https://doi.org/10.1038/415767a	journal	February 2002
Deep tissue two-photon microscopy Helmchen, Fritjof; Denk, Winfried Nature Methods, Vol. 2, Issue 12 https://doi.org/10.1038/nmeth818	journal	November 2005
Towards zero-threshold optical gain using charged semiconductor quantum dots Wu, Kaifeng; Park, Young-Shin; Lim, Jaehoon Nature Nanotechnology, Vol. 12, Issue 12 https://doi.org/10.1038/nnano.2017.189	journal	October 2017
Frequency-upconverted stimulated emission by simultaneous five-photon absorption Zheng, Qingdong; Zhu, Haomiao; Chen, Shan-Ci Nature Photonics, Vol. 7, Issue 3 https://doi.org/10.1038/nphoton.2012.344	journal	January 2013
Colloidal quantum dot lasers Park, Young-Shin; Roh, Jeongkyun; Diroll, Benjamin T. Nature Reviews Materials, Vol. 6, Issue 5 https://doi.org/10.1038/s41578-020-00274-9	journal	February 2021
Gain roll-off in cadmium selenide colloidal quantum wells under intense optical excitation Diroll, Benjamin T.; Brumberg, Alexandra; Schaller, Richard D. Scientific Reports, Vol. 12, Issue 1 https://doi.org/10.1038/s41598-022-11882-6	journal	May 2022
A strain-induced exciton transition energy shift in CdSe nanoplatelets: the impact of an organic ligand shell Antanovich, A.; Achtstein, A. W.; Matsukovich, A. Nanoscale, Vol. 9, Issue 45 https://doi.org/10.1039/C7NR05065H	journal	January 2017
Room temperature two-photon-pumped random lasers in FAPbBr ₃ /polyethylene oxide (PEO) composite perovskite thin film Xu, Long; Meng, Yan; Xu, Caixia RSC Advances, Vol. 8, Issue 64 https://doi.org/10.1039/C8RA07452F	journal	January 2018
Low-threshold laser medium utilizing semiconductor nanoshell quantum dots Porotnikov, Dmitry; Diroll, Benjamin T.; Harankahage, Dulanjan Nanoscale, Vol. 12, Issue 33 https://doi.org/10.1039/D0NR03582C	journal	January 2020
Perspectives for CdSe/CdS spherical quantum wells as rapid-response nano-scintillators Meng, Zhu; Mahler, Benoit; Houel, Julien Nanoscale, Vol. 13, Issue 46 https://doi.org/10.1039/D1NR04781G	journal	January 2021
Lasing action in colloidal CdS∕CdSe∕CdS quantum wells Xu, Jianfeng; Xiao, Min Applied Physics Letters, Vol. 87, Issue 17 https://doi.org/10.1063/1.2119423	journal	October 2005
Nanoshell quantum dots: Quantum confinement beyond the exciton Bohr radius Cassidy, James; Zamkov, Mikhail The Journal of Chemical Physics, Vol. 152, Issue 11 https://doi.org/10.1063/1.5126423	journal	March 2020
Highly luminescent silica-coated CdS/CdSe/CdS nanoparticles with strong chemical robustness and excellent thermal stability Wang, Nianfang; Koh, Sungjun; Jeong, Byeong Guk Nanotechnology, Vol. 28, Issue 18 https://doi.org/10.1088/1361-6528/aa6828	journal	April 2017
Quantum-dot quantum well CdS/HgS/CdS: Theory and experiment Schooss, D.; Mews, A.; Eychmüller, A. Physical Review B, Vol. 49, Issue 24 https://doi.org/10.1103/PhysRevB.49.17072	journal	June 1994
Electron and hole states in quantum dot quantum wells within a spherical eight-band model Pokatilov, E. P.; Fonoberov, V. A.; Fomin, V. M. Physical Review B, Vol. 64, Issue 24 https://doi.org/10.1103/PhysRevB.64.245329	journal	December 2001
Multiexcitons in type-II colloidal semiconductor quantum dots Oron, Dan; Kazes, Miri; Banin, Uri Physical Review B, Vol. 75, Issue 3 https://doi.org/10.1103/PhysRevB.75.035330	journal	January 2007
Universal Size-Dependent Trend in Auger Recombination in Direct-Gap and Indirect-Gap Semiconductor Nanocrystals Robel, István; Gresback, Ryan; Kortshagen, Uwe Physical Review Letters, Vol. 102, Issue 17, Article No. 177404 https://doi.org/10.1103/PhysRevLett.102.177404	journal	May 2009
Two-photon laser scanning fluorescence microscopy Denk, W.; Strickler, J.; Webb, W. Science, Vol. 248, Issue 4951 https://doi.org/10.1126/science.2321027	journal	April 1990
Quantization of Multiparticle Auger Rates in Semiconductor Quantum Dots Klimov, V. I. Science, Vol. 287, Issue 5455 https://doi.org/10.1126/science.287.5455.1011	journal	February 2000
Sub–single-exciton lasing using charged quantum dots coupled to a distributed feedback cavity Kozlov, Oleg V.; Park, Young-Shin; Roh, Jeongkyun Science, Vol. 365, Issue 6454 https://doi.org/10.1126/science.aax3489	journal	August 2019
Multicarrier Interactions in Semiconductor Nanocrystals in Relation to the Phenomena of Auger Recombination and Carrier Multiplication Klimov, Victor I. Annual Review of Condensed Matter Physics, Vol. 5, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031113-133900	journal	March 2014
Two-photon fluorescence excitation cross sections of biomolecular probes from 690 to 960 nm Albota, Marius A.; Xu, Chris; Webb, Watt W. Applied Optics, Vol. 37, Issue 31 https://doi.org/10.1364/AO.37.007352	journal	January 1998
Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690 to 1050 nm Xu, Chris; Webb, Watt W. Journal of the Optical Society of America B, Vol. 13, Issue 3 https://doi.org/10.1364/JOSAB.13.000481	journal	January 1996
Multiphoton route to ZnO nanowire lasers Zhang, C. F.; Dong, Z. W.; You, G. J. Optics Letters, Vol. 31, Issue 22 https://doi.org/10.1364/OL.31.003345	journal	October 2006
Two-photon-pumped lasing from colloidal nanocrystal quantum dots Zhang, Chunfeng; Zhang, Fan; Zhu, Ting Optics Letters, Vol. 33, Issue 21 https://doi.org/10.1364/OL.33.002437	journal	January 2008

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Quantum shell
amplified spontaneous emission
laser
optical gain
two photon absorption

Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

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