Bidirectional triplet exciton transfer between silicon nanocrystals and perylene

Huang, Tingting; Koh, Timothy T.; Schwan, J.; Tran, Tiffany T.-T.; Wang, Kefu; Mangolini, Lorenzo; Tang, Ming Lee; Roberts, Sean T.

doi:10.1039/d1sc00311a

Cited by 21 publications

(25 citation statements)

References 67 publications

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“…4A , grey dashed line). 93 Indeed, a significant heterogeneous contribution to the linewidth could give rise to asymmetric quenching of the steady-state ensemble QD PL, 67,94 which we do not observe (Fig. S4 † ).…”

Section: Resultsmentioning

confidence: 48%

“…The microsecond-scale forward transfer and quasi-equilibrium dynamics are similar to a very recent report of Si QDs functionalized with a perylene derivative. 67 Additionally, while we discuss our results in the context of (correlated) excitonic energy transfer, we cannot rule out that transfer also occurs via a sequential mechanism following single-carrier trapping—a model that is consistent with experiments on larger QDs paired with triplet acceptors. 64,71,76,77 Exothermic carrier trapping on the QD would slow TET (relative to transfer from band-edge states) by increasing the effective endothermicity of the key QD → molecule transfer, but our experiments do not discern between these hypotheses.…”

Section: Resultsmentioning

confidence: 70%

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Ultra-small PbS nanocrystals as sensitizers for red-to-blue triplet-fusion upconversion

et al. 2021

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Section: Resultsmentioning

confidence: 48%

Section: Resultsmentioning

confidence: 70%

Ultra-small PbS nanocrystals as sensitizers for red-to-blue triplet-fusion upconversion

et al. 2021

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“…4,16,19,23,24 However, the presence of poisonous heavy metals often prohibits the use of these classes of QDs in consumer devices due to the potentially adverse effects on health and the environment. 25,26 Although Tang and Roberts recently demonstrated rTTET from perylene to environmentally friendly silicon nanocrystals, 10 the TADPL process was not observed in this indirect semiconductor nanomaterial. However, direct band gap InP QDs represent a promising lower toxicity alternative with respect to numerous toxic metal-containing QDs featuring high quantum yield (QY) photoluminescence.…”

Section: ■ Introductionmentioning

confidence: 95%

Engineering Long-Lived Blue Photoluminescence from InP Quantum Dots Using Isomers of Naphthoic Acid

2022

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Leveraging triplet excitons in semiconductor quantum dots (QDs) in concert with surface-anchored molecules to produce long-lifetime thermally activated delayed photoluminescence (TADPL) continues to emerge as a promising technology in diverse areas including photochemical catalysis and light generation. All QDs presently used to generate TADPL in QD/molecule constructs contain toxic metals including Cd(II) and Pb(II), ultimately limiting potential real-world applications. Here, we report newly conceived blue-emitting TADPL-producing nanomaterials featuring InP QDs interfaced with 1-and 2-naphthoic acid (1-NA and 2-NA) ligands. These constitutional isomers feature similar triplet energies but disparate triplet lifetimes, translating into InP-based TADPL processes displaying two distinct average lifetime ranges upon cooling from 293 to 193 K. The time constants fall between 4.4 and 59.2 μs in the 2-NA-decorated InP QDs while further expanding between 84.2 and 733.2 μs in the corresponding 1-NA-ligated InP materials, representing a 167-fold time window. The resulting long-lived excited states enabled facile bimolecular triplet sensitization of 1 O 2 phosphorescence in the near-IR and promoted sensitized triplet−triplet annihilation photochemistry in 2,5-diphenyloxazole. We speculate that the discovery of new nanomaterials exhibiting TADPL lies on the horizon as myriad QDs can be readily derivatized using isomers of numerous classes of surface-anchoring chromophores yielding precisely regulated photophysical properties.

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“…To strengthen the stability, polymer barriers on SiNCs' surfaces to retard the diffusion of oxygen has been demonstrated as a viable solution (Xia et al, 2021). Moreover, bidirectional triplet exciton transfer could also be realized by functionalizing SiNCs with perylene chromophores (Huang et al, 2021). Despite the fact that the SiNCs employed in these works were synthesized via nonthermal plasma, we are confident that SiNCs generated from thermal disproportionation should exhibit similar behaviors.…”

Section: Discussionmentioning

confidence: 97%

Thermal Disproportionation for the Synthesis of Silicon Nanocrystals and Their Photoluminescent Properties

Wang

Hong

et al. 2021

Front. Chem.

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In the past decades, silicon nanocrystals have received vast attention and have been widely studied owing to not only their advantages including nontoxicity, high availability, and abundance but also their unique luminescent properties distinct from bulk silicon. Among the various synthetic methods of silicon nanocrystals, thermal disproportionation of silicon suboxides (often with H as another major composing element) bears the superiorities of unsophisticated equipment requirements, feasible processing conditions, and precise control of nanocrystals size and structure, which guarantee a bright industrial application prospect. In this paper, we summarize the recent progress of thermal disproportionation chemistry for the synthesis of silicon nanocrystals, with the focus on the effects of temperature, Si/O ratio, and the surface groups on the resulting silicon nanocrystals’ structure and their corresponding photoluminescent properties. Moreover, the paradigmatic application scenarios of the photoluminescent silicon nanocrystals synthesized via this method are showcased or envisioned.

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Bidirectional triplet exciton transfer between silicon nanocrystals and perylene

Abstract: Hybrid materials comprised of inorganic quantum dots functionalized with small-molecule organic chromophores have emerged as promising materials for reshaping light’s energy content. Quantum dots in these structures can serve as...

Cited by 21 publications

References 67 publications

Ultra-small PbS nanocrystals as sensitizers for red-to-blue triplet-fusion upconversion

Ultra-small PbS nanocrystals as sensitizers for red-to-blue triplet-fusion upconversion

Engineering Long-Lived Blue Photoluminescence from InP Quantum Dots Using Isomers of Naphthoic Acid

Thermal Disproportionation for the Synthesis of Silicon Nanocrystals and Their Photoluminescent Properties

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