PbS/CdS Core–Shell Quantum Dots Suppress Charge Transfer and Enhance Triplet Transfer

Huang, Zhiyuan; Xu, Zihao; Mahboub, Melika; Li, Xin; Taylor, Jordan W.; Harman, W. Hill; Lian, Tianquan; Tang, Ming Lee

doi:10.1002/anie.201710224

PbS/CdS Core–Shell Quantum Dots Suppress Charge Transfer and Enhance Triplet Transfer

Journal Article · Wed Nov 29 23:00:00 EST 2017 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201710224· OSTI ID:1410701

Huang, Zhiyuan ^[1]; Xu, Zihao ^[2]; Mahboub, Melika ^[1]; Li, Xin ^[1]; Taylor, Jordan W. ^[1]; Harman, W. Hill ^[1]; ^[2]; ^[1]

Department of Chemistry University of California, Riverside 900 University Ave. Riverside CA 92507 USA
Department of Chemistry Emory University Atlanta GA 30322 USA

Abstract

A sub‐monolayer CdS shell on PbS quantum dots (QDs) enhances triplet energy transfer (TET) by suppressing competitive charge transfer from QDs to molecules. The CdS shell increases the linear photon upconversion quantum yield (QY) from 3.5 % for PbS QDs to 5.0 % for PbS/CdS QDs when functionalized with a tetracene acceptor, 5‐CT . While transient absorption spectroscopy reveals that both PbS and PbS/CdS QDs show the formation of the 5‐CT triplet (with rates of 5.91±0.60 ns ⁻¹ and 1.03±0.09 ns ⁻¹ respectively), ultrafast hole transfer occurs only from PbS QDs to 5‐CT . Although the CdS shell decreases the TET rate, it enhances TET efficiency from 60.3±6.1 % to 71.8±6.2 % by suppressing hole transfer. Furthermore, the CdS shell prolongs the lifetime of the 5‐CT triplet and thus enhances TET from 5‐CT to the rubrene emitter, further bolstering the upconverison QY.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0008798

OSTI ID:: 1410701

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 52 Vol. 56; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (31)

Triplet Energy Transfer from PbS(Se) Nanocrystals to Rubrene: the Relationship between the Upconversion Quantum Yield and Size Mahboub, Melika; Maghsoudiganjeh, Hadi; Pham, Andrew Minh Advanced Functional Materials, Vol. 26, Issue 33 https://doi.org/10.1002/adfm.201505623	journal	June 2016
Colloidal PbS Nanocrystals with Size-Tunable Near-Infrared Emission: Observation of Post-Synthesis Self-Narrowing of the Particle Size Distribution Hines, M. A.; Scholes, G. D. Advanced Materials, Vol. 15, Issue 21, p. 1844-1849 https://doi.org/10.1002/adma.200305395	journal	November 2003
Complementary Lock-and-Key Ligand Binding of a Triplet Transmitter to a Nanocrystal Photosensitizer Li, Xin; Fast, Alexander; Huang, Zhiyuan Angewandte Chemie, Vol. 129, Issue 20 https://doi.org/10.1002/ange.201701929	journal	April 2017
Complementary Lock-and-Key Ligand Binding of a Triplet Transmitter to a Nanocrystal Photosensitizer Li, Xin; Fast, Alexander; Huang, Zhiyuan Angewandte Chemie International Edition, Vol. 56, Issue 20 https://doi.org/10.1002/anie.201701929	journal	April 2017
Nanocrystal Size and Quantum Yield in the Upconversion of Green to Violet Light with CdSe and Anthracene Derivatives Huang, Zhiyuan; Li, Xin; Yip, Benjamin D. Chemistry of Materials, Vol. 27, Issue 21 https://doi.org/10.1021/acs.chemmater.5b03731	journal	October 2015
Colloidal Quantum Dot Solar Cells Carey, Graham H.; Abdelhady, Ahmed L.; Ning, Zhijun Chemical Reviews, Vol. 115, Issue 23 https://doi.org/10.1021/acs.chemrev.5b00063	journal	June 2015
Delayed Molecular Triplet Generation from Energized Lead Sulfide Quantum Dots Garakyaraghi, Sofia; Mongin, Cédric; Granger, Devin B. The Journal of Physical Chemistry Letters, Vol. 8, Issue 7 https://doi.org/10.1021/acs.jpclett.7b00546	journal	March 2017
Hybrid Molecule–Nanocrystal Photon Upconversion Across the Visible and Near-Infrared Huang, Zhiyuan; Li, Xin; Mahboub, Melika Nano Letters, Vol. 15, Issue 8 https://doi.org/10.1021/acs.nanolett.5b02130	journal	July 2015
Efficient Infrared-to-Visible Upconversion with Subsolar Irradiance Mahboub, Melika; Huang, Zhiyuan; Tang, Ming Lee Nano Letters, Vol. 16, Issue 11 https://doi.org/10.1021/acs.nanolett.6b03503	journal	October 2016
Influence of Shell Thickness and Surface Passivation on PbS/CdS Core/Shell Colloidal Quantum Dot Solar Cells Neo, Darren C. J.; Cheng, Cheng; Stranks, Samuel D. Chemistry of Materials, Vol. 26, Issue 13 https://doi.org/10.1021/cm501595u	journal	June 2014
Prospects of Colloidal Nanocrystals for Electronic and Optoelectronic Applications Talapin, Dmitri V.; Lee, Jong-Soo; Kovalenko, Maksym V. Chemical Reviews, Vol. 110, Issue 1 https://doi.org/10.1021/cr900137k	journal	January 2010
Dimerization of the perylene and tetracene radical cations and electronic absorption spectra of their dimers Kimura, Katsumi; Yamazaki, Tomoko; Katsumata, Shunji The Journal of Physical Chemistry, Vol. 75, Issue 12 https://doi.org/10.1021/j100681a002	journal	June 1971
Electronic spectra of ion radicals and their molecular orbital interpretation. III. Aromatic hydrocarbons Shida, Tadamasa.; Iwata, Suehiro. Journal of the American Chemical Society, Vol. 95, Issue 11 https://doi.org/10.1021/ja00792a005	journal	May 1973
Ultrafast Charge Separation and Recombination Dynamics in Lead Sulfide Quantum Dot–Methylene Blue Complexes Probed by Electron and Hole Intraband Transitions Yang, Ye; Rodríguez-Córdoba, William; Lian, Tianquan Journal of the American Chemical Society, Vol. 133, Issue 24 https://doi.org/10.1021/ja2033348	journal	June 2011
Efficiency of Hole Transfer from Photoexcited Quantum Dots to Covalently Linked Molecular Species Ding, Tina X.; Olshansky, Jacob H.; Leone, Stephen R. Journal of the American Chemical Society, Vol. 137, Issue 5 https://doi.org/10.1021/ja512278a	journal	January 2015
Excited-State Dynamics of Organic Radical Ions in Liquids and in Low-Temperature Matrices Brodard, Pierre; Sarbach, Alexandre; Gumy, Jean-Claude The Journal of Physical Chemistry A, Vol. 105, Issue 27 https://doi.org/10.1021/jp010808l	journal	July 2001
Distribution of Multiexciton Generation Rates in CdSe and InAs Nanocrystals Rabani, Eran; Baer, Roi Nano Letters, Vol. 8, Issue 12 https://doi.org/10.1021/nl802443c	journal	December 2008
Size-Tunable, Bright, and Stable PbS Quantum Dots: A Surface Chemistry Study Moreels, Iwan; Justo, Yolanda; De Geyter, Bram ACS Nano, Vol. 5, Issue 3 https://doi.org/10.1021/nn103050w	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
Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals Thompson, Nicholas J.; Wilson, Mark W. B.; Congreve, Daniel N. Nature Materials, Vol. 13, Issue 11 https://doi.org/10.1038/nmat4097	journal	October 2014
Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals Wu, Mengfei; Congreve, Daniel N.; Wilson, Mark W. B. Nature Photonics, Vol. 10, Issue 1 https://doi.org/10.1038/nphoton.2015.226	journal	November 2015
Ligand enhanced upconversion of near-infrared photons with nanocrystal light absorbers Huang, Zhiyuan; Simpson, Duane E.; Mahboub, Melika Chemical Science, Vol. 7, Issue 7 https://doi.org/10.1039/C6SC00257A	journal	January 2016
CdS/ZnS core–shell nanocrystal photosensitizers for visible to UV upconversion Gray, Victor; Xia, Pan; Huang, Zhiyuan Chemical Science, Vol. 8, Issue 8 https://doi.org/10.1039/C7SC01610G	journal	January 2017
Synthesis, properties and perspectives of hybrid nanocrystal structures Cozzoli, Pantaleo Davide; Pellegrino, Teresa; Manna, Liberato Chemical Society Reviews, Vol. 35, Issue 11, p. 1195-1208 https://doi.org/10.1039/b517790c	journal	January 2006
Wavefunction engineering in quantum confined semiconductor nanoheterostructures for efficient charge separation and solar energy conversion Zhu, Haiming; Lian, Tianquan Energy & Environmental Science, Vol. 5, Issue 11 https://doi.org/10.1039/c2ee22679k	journal	January 2012
Band-edge exciton in quantum dots of semiconductors with a degenerate valence band: Dark and bright exciton states Efros, Al. L.; Rosen, M.; Kuno, M. Physical Review B, Vol. 54, Issue 7 https://doi.org/10.1103/PhysRevB.54.4843	journal	August 1996
Observation of the "Dark Exciton" in CdSe Quantum Dots Nirmal, M.; Norris, D. J.; Kuno, M. Physical Review Letters, Vol. 75, Issue 20 https://doi.org/10.1103/PhysRevLett.75.3728	journal	November 1995
Peak External Photocurrent Quantum Efficiency Exceeding 100% via MEG in a Quantum Dot Solar Cell Semonin, O. E.; Luther, J. M.; Choi, S. Science, Vol. 334, Issue 6062 https://doi.org/10.1126/science.1209845	journal	December 2011
Direct observation of triplet energy transfer from semiconductor nanocrystals Mongin, C.; Garakyaraghi, S.; Razgoniaeva, N. Science, Vol. 351, Issue 6271 https://doi.org/10.1126/science.aad6378	journal	January 2016
Semiconductor Quantum Dots for Bioimaging and Biodiagnostic Applications Kairdolf, Brad A.; Smith, Andrew M.; Stokes, Todd H. Annual Review of Analytical Chemistry, Vol. 6, Issue 1 https://doi.org/10.1146/annurev-anchem-060908-155136	journal	June 2013
Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals Klimov, Victor I. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.032806.104537	journal	May 2007

Similar Records

PbS/CdS Core–Shell Quantum Dots Suppress Charge Transfer and Enhance Triplet Transfer

Journal Article · Thu Dec 21 23:00:00 EST 2017 · Angewandte Chemie · OSTI ID:1410831

PbS/CdS Core–Shell Quantum Dots Suppress Charge Transfer and Enhance Triplet Transfer

Citation Formats

References (31)

Similar Records

Related Subjects