The Rise and Future of Discrete Organic–Inorganic Hybrid Nanomaterials

Brett, Matthew W.; Gordon, Calum K.; Hardy, Jake; Davis, Nathaniel J. L. K.

doi:10.1021/acsphyschemau.2c00018

Cited by 18 publications

(14 citation statements)

References 232 publications

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“…Organometallic chromophores such as metalloporphyrins have long been known as traditional sensitizers for TTA-UC . Recently, intensive research has been conducted on semiconductor nanocrystal (or quantum dot) sensitizers modified with triplet mediator ligands. , Although semiconductor nanocrystals exhibit excellent light-harvesting ability over a wide wavelength region, it is inevitable that they strongly reabsorb the generated UC photons. Additionally, they often contain toxic elements, such as Pb and Cd, which are problematic because they hinder the fabrication of ecofriendly materials.…”

Section: Introductionmentioning

confidence: 99%

Structurally Flexible Au–Cu Alloy Nanoclusters Enabling Efficient Triplet Sensitization and Photon Upconversion

Arima

Mitsui

2023

J. Am. Chem. Soc.

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Ligand-protected noble-metal nanoclusters exhibit an innately triplet nature and have been recently recognized as emerging platforms for triplet sensitizers of photon upconversion (UC) via triplet−triplet annihilation. Herein, we report that a structurally flexible Au−Cu alloy nanocluster, [Au 4 Cu 4 (S-Adm) 5 (DPPM) 2 ] + (Au 4 Cu 4 ; S-Adm = 1-adamantanethiolate, DPPM = bis(diphenylphosphino)methane), exhibited favorable sensitizer properties and superior UC performance. Contrary to the structurally rigid Au 2 Cu 6 (S-Adm) 6 (TPP) 2 (Au 2 Cu 6 , TPP = triphenylphosphine), Au 4 Cu 4 exhibited significantly better sensitizer characteristics, such as a near-unity quantum yield for intersystem crossing (ISC), long triplet lifetime (ca. 8 μs), and efficient triplet energy transfer (TET). The efficient ISC of Au 4 Cu 4 was attributed to the practically negligible activation barriers during the ISC process, which was caused by the spin−orbit interaction between the two isoenergetic isomers predicted by theoretical calculations. A series of aromatic molecules with different triplet energies were used as acceptors to reveal the driving force dependence of the TET rate constant (k TET ). This dependency was analyzed to evaluate the triplet energy and sensitization ability of the alloy nanoclusters. The results showed that the maximum value of k TET for Au 4 Cu 4 was seven times larger than that for Au 2 Cu 6 , which presumably reflects the structural/electronic fluctuations of Au 4 Cu 4 during the triplet state residence. The combination of the Au 4 Cu 4 sensitizer and the 9,10-diphenylanthracene (DPA) annihilator/emitter achieved UC with internal quantum yields of 14% (out of 50% maximum) and extremely low threshold intensities (2−26 mWcm −2 ). This performance far exceeds that of Au 2 Cu 6 and is also outstanding among the organic−inorganic hybrid nanomaterials reported so far.

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Section: Introductionmentioning

confidence: 99%

Structurally Flexible Au–Cu Alloy Nanoclusters Enabling Efficient Triplet Sensitization and Photon Upconversion

Arima

Mitsui

2023

J. Am. Chem. Soc.

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“…Discrete hybrid inorganic–organic luminophores are a modern avenue of research for LSC applications. ,, A discrete hybrid inorganic–organic luminophore is a combination of two or more luminophores covalently/noncovalently interactingconsisting of at least one organic and inorganic component that interact via energy transfer (Figure b).…”

Section: Introductionmentioning

confidence: 99%

Performance Evaluation of Solid State Luminescent Solar Concentrators Based on InP/ZnS-Rhodamine 101 Hybrid Inorganic–Organic Luminophores

et al. 2022

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Luminescent solar concentrators (LSCs) suffer greatly from reabsorption, where emitted light is parasitically reabsorbed by a luminophore. Specifically designed luminophores with inherently large Stokes shifts have been successfully synthesized in the literature; however, they introduce a new issue of poor absorption due to excessive blue shifting of the luminophores' absorption. Hybrid luminophores consisting of quantum dots (QDs) coupled to organic dyes offer a solution to this problem, by improving light sensitization and increasing the Stokes shift via energy transfer. We present a Cd/Pb-free InP/ZnS QD donor coupled to a rhodamine 101 acceptor hybrid luminophore LSC (10 × 10 × 0.3 cm, gain factor 8.33). The external quantum efficiency of the device under 405 nm illumination was 2.7 ± 0.6%, giving a mean 50% increase in external quantum efficiency relative to an InP/ZnS QD device. This study represents the first inorganic to organic hybrid nanomaterial system with attached luminophores in the solid state. We also perform an in-depth investigation by optical characterization of the different operational metrics of our novel LSCs.

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“…This is just the reason why big-data-driven Machine Learning [ 24 ] has been recently proposed as a powerful tool to suggest feasible ligands that can guide and accelerate the experimental work [ 6 , 23 , 25 , 26 ]. Because of all the aforementioned beneficial properties, CQDs are considered as the “building blocks” [ 27 , 28 ] for manufacturing an important variety of opto-electronics devices [ 1 , 29 , 30 , 31 ].…”

Section: Introductionmentioning

confidence: 99%

Carrier Transport in Colloidal Quantum Dot Intermediate Band Solar Cell Materials Using Network Science

Cuadra

Salcedo‐Sanz

Borge

2023

IJMS

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Colloidal quantum dots (CQDs) have been proposed to obtain intermediate band (IB) materials. The IB solar cell can absorb sub-band-gap photons via an isolated IB within the gap, generating extra electron-hole pairs that increase the current without degrading the voltage, as has been demonstrated experimentally for real cells. In this paper, we model the electron hopping transport (HT) as a network embedded in space and energy so that a node represents the first excited electron state localized in a CQD while a link encodes the Miller–Abrahams (MA) hopping rate for the electron to hop from one node (=state) to another, forming an “electron-HT network”. Similarly, we model the hole-HT system as a network so that a node encodes the first hole state localized in a CQD while a link represents the MA hopping rate for the hole to hop between nodes, leading to a “hole-HT network”. The associated network Laplacian matrices allow for studying carrier dynamics in both networks. Our simulations suggest that reducing both the carrier effective mass in the ligand and the inter-dot distance increases HT efficiency. We have found a design constraint: It is necessary for the average barrier height to be larger than the energetic disorder to not degrade intra-band absorption.

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The Rise and Future of Discrete Organic–Inorganic Hybrid Nanomaterials

Cited by 18 publications

References 232 publications

Structurally Flexible Au–Cu Alloy Nanoclusters Enabling Efficient Triplet Sensitization and Photon Upconversion

Structurally Flexible Au–Cu Alloy Nanoclusters Enabling Efficient Triplet Sensitization and Photon Upconversion

Performance Evaluation of Solid State Luminescent Solar Concentrators Based on InP/ZnS-Rhodamine 101 Hybrid Inorganic–Organic Luminophores

Carrier Transport in Colloidal Quantum Dot Intermediate Band Solar Cell Materials Using Network Science

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