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Mechanisms Of Triplet Energy Transfer Across The Inorganic Nanocrystal/organic Molecule Interface
X. Luo, Y. Han, Zongwei Chen, Yu-lu Li, Gui-jie Liang, X. Liu, T. Ding, C. Nie, M. Wang, F. Castellano, Kaifeng Wu
Published 2020 · Materials Science, Medicine
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The mechanisms of triplet energy transfer across the inorganic nanocrystal/organic molecule interface remain poorly understood. Many seemingly contradictory results have been reported, mainly because of the complicated trap states characteristic of inorganic semiconductors and the ill-defined relative energetics between semiconductors and molecules used in these studies. Here we clarify the transfer mechanisms by performing combined transient absorption and photoluminescence measurements, both with sub-picosecond time resolution, on model systems comprising lead halide perovskite nanocrystals with very low surface trap densities as the triplet donor and polyacenes which either favour or prohibit charge transfer as the triplet acceptors. Hole transfer from nanocrystals to tetracene is energetically favoured, and hence triplet transfer proceeds via a charge separated state. In contrast, charge transfer to naphthalene is energetically unfavourable and spectroscopy shows direct triplet transfer from nanocrystals to naphthalene; nonetheless, this “direct” process could also be mediated by a high-energy, virtual charge-transfer state. Though literature reports models describing triplet energy transfer between inorganic semiconductors and organic molecules, a unified mechanism for this process is still lacking. Here, the authors report triplet energy transfer mechanism at lead halide perovskite nanocrystal/polyacene interfaces.
This paper references
Essentially Trap-Free CsPbBr3 Colloidal Nanocrystals by Postsynthetic Thiocyanate Surface Treatment.
Brent A Koscher (2017)
Kinetics of Fluorescence Quenching by Electron and H‐Atom Transfer
D. Rehm (1970)
Visible-Light-Driven Sensitization of Naphthalene Triplets Using Quantum-Confined CsPbBr3 Nanocrystals.
Y. Han (2019)
Diphenylisobenzofuran Bound to Nanocrystalline Metal Oxides: Excimer Formation, Singlet Fission, Electron Injection, and Low Energy Sensitization
Tanmay Banerjee (2018)
Band Edge Energies and Excitonic Transition Probabilities of Colloidal CsPbX3 (X = Cl, Br, I) Perovskite Nanocrystals
V. K. Ravi (2016)
Room temperature triplet state spectroscopy of organic semiconductors
S. Reineke (2014)
Photochemical upconversion: present status and prospects for its application to solar energy conversion
T. F. Schulze (2015)
Biexciton Auger recombination in mono-dispersed, quantum-confined CsPbBr3 perovskite nanocrystals obeys universal volume-scaling
Yu-lu Li (2018)
Rate expressions for excitation transfer. II. Electronic considerations of direct and through–configuration exciton resonance interactions
R. D. Harcourt (1994)
Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals
Q. Akkerman (2018)
Precise Control of Quantum Confinement in Cesium Lead Halide Perovskite Quantum Dots via Thermodynamic Equilibrium.
Y. Dong (2018)
Auger-assisted electron transfer from photoexcited semiconductor quantum dots.
Haiming Zhu (2014)
Visible-to-Ultraviolet Upconversion Efficiency above 10% Sensitized by Quantum-Confined Perovskite Nanocrystals.
S. He (2019)
Properties and potential optoelectronic applications of lead halide perovskite nanocrystals
M. Kovalenko (2017)
Microscopic theory of singlet exciton fission. II. Application to pentacene dimers and the role of superexchange.
Timothy C Berkelbach (2013)
Designing Transmitter Ligands That Mediate Energy Transfer between Semiconductor Nanocrystals and Molecules.
Zhiyuan Huang (2017)
Triplet sensitization by perovskite nanocrystals for photon upconversion.
K. Mase (2017)
Triplet-Sensitization by Lead Halide Perovskite Thin Films for Near-Infrared-to-Visible Upconversion
L. Nienhaus (2019)
Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage.
D. Kroupa (2018)
On the absence of a phonon bottleneck in strongly confined CsPbBr3 perovskite nanocrystals.
Yulu Li (2019)
Picosecond multi-hole transfer and microsecond charge-separated states at the perovskite nanocrystal/tetracene interface† †Electronic supplementary information (ESI) available: Fig. S1–S9, sample preparations, TA experiment set-ups, and other supplementary contents. See DOI: 10.1039/c8sc04408b
X. Luo (2019)
Light Absorption Coefficient of CsPbBr3 Perovskite Nanocrystals.
J. Maes (2018)
Dynamics of singlet fission and electron injection in self-assembled acene monolayers on titanium dioxide† †Electronic supplementary information (ESI) available: Steady-state UV-VIS and PL, solution transient absorption, X-ray diffraction, decay associated spectra, and TIPS Tc COOH/Al2O3/TiO2 film k
N. A. Pace (2018)
Surface States Mediate Triplet Energy Transfer in Nanocrystal-Acene Composite Systems.
Jon A Bender (2018)
Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals
M. Wu (2016)
"Intact" Carrier Doping by Pump-Pump-Probe Spectroscopy in Combination with Interfacial Charge Transfer: A Case Study of CsPbBr3 Nanocrystals.
J. Wang (2018)
PbS/CdS Core-Shell Quantum Dots Suppress Charge Transfer and Enhance Triplet Transfer.
Zhiyuan Huang (2017)
Electrochemistry of CdS nanoparticles: a correlation between optical and electrochemical band gaps.
S. Haram (2001)
Engineering Molecular Ligand Shells on Quantum Dots for Quantitative Harvesting of Triplet Excitons Generated by Singlet Fission
Jesse R Allardice (2019)
Sensitization-Initiated Electron Transfer for Photoredox Catalysis.
I. Ghosh (2017)
Light-Induced Activation of Forbidden Exciton Transition in Strongly Confined Perovskite Quantum Dots.
D. Rossi (2018)
Designed Long‐Lived Emission from CdSe Quantum Dots through Reversible Electronic Energy Transfer with a Surface‐Bound Chromophore
Marcello La Rosa (2018)
Electronic spectra of ion radicals and their molecular orbital interpretation. III. Aromatic hydrocarbons
T. Shida (1973)
Resonant energy transfer of triplet excitons from pentacene to PbSe nanocrystals.
Maxim Tabachnyk (2014)
Long-range electron transfer across Peptide bridges: the transition from electron superexchange to hopping.
Rouba Abdel Malak (2004)
New Triplet Sensitization Routes for Photon Upconversion: Thermally Activated Delayed Fluorescence Molecules, Inorganic Nanocrystals, and Singlet-to-Triplet Absorption.
N. Yanai (2017)
Photosensitized singlet oxygen and its applications
M. DeRosa (2002)
Maximizing singlet fission in organic dimers: theoretical investigation of triplet yield in the regime of localized excitation and fast coherent electron transfer.
E. Greyson (2010)
Sensitizing Singlet Fission with Perovskite Nanocrystals.
Haipeng Lu (2019)
Photosensitized, energy transfer-mediated organometallic catalysis through electronically excited nickel(II)
Eric R Welin (2017)
Direct observation of triplet energy transfer from semiconductor nanocrystals
Cédric Mongin (2016)
Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut
L. Protesescu (2015)
Handbook of photochemistry
Steven L. Murov (1973)
Evaluation of initiator systems for controlled and sequentially curable free‐radical/cationic hybrid photopolymerizations
J. D. Oxman (2005)
Charge transfer-mediated singlet fission.
N. Monahan (2015)
A Theory of Sensitized Luminescence in Solids
D. Dexter (1953)
Photoinduced electron transfer from semiconductor quantum dots to metal oxide nanoparticles
K. Tvrdy (2010)
Nanocrystals for Triplet Sensitization: Molecular Behavior from Quantum-Confined Materials.
Sofia Garakyaraghi (2018)
Determination of quantum confinement in CdSe nanocrystals by cyclic voltammetry
Erol Kuçur (2003)
Identification of a triplet pair intermediate in singlet exciton fission in solution
H. Stern (2015)
Harvesting singlet fission for solar energy conversion via triplet energy transfer.
John R. Tritsch (2013)
Crossover from superexchange to hopping as the mechanism for photoinduced charge transfer in DNA hairpin conjugates.
F. Lewis (2006)
Ultrafast Interfacial Electron and Hole Transfer from CsPbBr3 Perovskite Quantum Dots.
Kaifeng Wu (2015)
Sensitization of silicon by singlet exciton fission in tetracene
Markus Einzinger (2019)
Thermally activated delayed photoluminescence from pyrenyl-functionalized CdSe quantum dots.
Cédric Mongin (2018)
Lighting Up AIEgen Emission in Solution by Grafting onto Colloidal Nanocrystal Surfaces.
X. Luo (2018)
A transferable model for singlet-fission kinetics.
S. Yost (2014)
Delayed Molecular Triplet Generation from Energized Lead Sulfide Quantum Dots.
Sofia Garakyaraghi (2017)
Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals.
N. Thompson (2014)
Triplet Energy Transfer from CsPbBr3 Nanocrystals Enabled by Quantum Confinement.
X. Luo (2019)
Charge Transfer Dynamics from Photoexcited Semiconductor Quantum Dots.
Haiming Zhu (2016)
Electron transfers in chemistry and biology
R. Marcus (1985)
Triplet Sensitization by "Self-Trapped" Excitons of Nontoxic CuInS2 Nanocrystals for Efficient Photon Upconversion.
Y. Han (2019)
This paper is referenced by
Size and Halide Dependent Auger Recombination in Lead Halide Perovskite Nanocrystals.
Yu-lu Li (2020)
Trap state mediated triplet energy transfer from CdSe quantum dots to molecular acceptors.
Tao Jin (2020)
Triarylmethanolation as a versatile strategy for the conversion of PAHs into amorphization-induced emission luminogens for extremely sensitive explosive detection and fabrication of artificial light-harvesting systems
Min Su (2020)
Direct vs Delayed Triplet Energy Transfer from Organic Semiconductors to Quantum Dots and Implications for Luminescent Harvesting of Triplet Excitons
V. Gray (2020)
Engineering 3D perovskites for photon interconversion applications
S. Wieghold (2020)
Host-Guest Thin Films by Confining Ultrafine Pt/C QDs into Metal-Organic Frameworks for Highly Efficient Hydrogen Evolution.
Yihong Xiao (2020)
TIPS-pentacene triplet exciton generation on PbS quantum dots results from indirect sensitization† †Electronic supplementary information (ESI) available: Structural characterization of the PbS and PbS-TPn nanomaterials and additional transient absorption spectra and kinetic data and analyses. See DO
Christopher M. Papa (2020)
One‐Step Fabrication of Perovskite‐Based Upconversion Devices
Sarah Wieghold (2020)
Competition of Dexter, Förster, and charge transfer pathways for quantum dot sensitized triplet generation.
Tao Jin (2020)
Optical studies of semiconductor perovskite nanocrystals for classical optoelectronic applications and quantum information technologies: a review
Z. Cao (2020)
Sensitized Molecular Triplet and Triplet Excimer Emission in 2D Hybrid Perovskites.
Yuyang Tian (2020)
Impact of photosensitizer orientation on the distance dependent photocatalytic activity in zinc phthalocyanine–nanoporous gold hybrid systems
David Steinebrunner (2020)
High Photon Upconversion Efficiency with Hybrid Triplet Sensitizers by Ultrafast Hole-Routing in Electronic-Doped Nanocrystals.
A. Ronchi (2020)
Halide Perovskites: A Progress Report on Photon Interconversion
S. Wieghold (2020)
Engineering Sensitized Photon Upconversion Efficiency via Nanocrystal Wavefunction and Molecular Geometry.
S. He (2020)
Perovskite-sensitized upconversion bingo: Stoichiometry, composition, solvent, or temperature?
Alexander Bieber (2020)
Perovskite Nano Heterojunctions: Synthesis, Structures, Properties, Challenges and Prospects
X. Xu (2020)