Donor-acceptor bulk-heterojunction sensitizer for efficient solid-state infrared-to-visible photon up-conversion DOI Creative Commons
Pengqing Bi, Tao Zhang, Yuanyuan Guo

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 8, 2024

Solid-state infrared-to-visible photon up-conversion is important for spectral-tailoring applications. However, existing systems not only suffer from low efficiencies and a need high excitation intensity, but also exhibit limited selection of materials complex fabrication processes. Herein, we propose sensitizer with bulk-heterojunction structure, comprising both an energy donor acceptor, triplet-triplet annihilation devices. The occurs through charge separation at the donor-acceptor interface, followed by formation transfer state between annihilator following spin statistics. ensures efficient generation recombination. Hence, achieve highly solid-state device 2.20% efficiency intensity (10 mW cm

Language: Английский

Energy Versus Electron Transfer: Managing Excited-State Interactions in Perovskite Nanocrystal–Molecular Hybrids DOI
Jeffrey T. DuBose, Prashant V. Kamat

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(15), P. 12475 - 12494

Published: July 6, 2022

Energy and electron transfer processes in light harvesting assemblies dictate the outcome of overall energy conversion process. Halide perovskite nanocrystals such as CsPbBr3 with relatively high emission yield strong absorption can singlet triplet to surface-bound acceptor molecules. They also induce photocatalytic reduction oxidation by selectively transferring electrons holes across nanocrystal interface. This perspective discusses key factors dictating these excited-state pathways fundamental differences between processes. Spectroscopic methods decipher complex photoinduced are presented. A basic understanding two excited deactivation (charge transfer) ways modulate them should enable design more efficient semiconductor molecular systems.

Language: Английский

Citations

90
Near-infrared photon upconversion and solar synthesis using lead-free nanocrystals DOI
Wenfei Liang,

Chengming Nie,

Jun Du

et al.

Nature Photonics, Journal Year: 2023, Volume and Issue: 17(4), P. 346 - 353

Published: Feb. 6, 2023

Language: Английский

Citations

82
Triplet–triplet annihilation photon upconversion-mediated photochemical reactions DOI
Ling Huang, Gang Han

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(4), P. 238 - 255

Published: March 21, 2024

Language: Английский

Citations

30
Charge Transfer from Quantum-Confined 0D, 1D, and 2D Nanocrystals DOI Creative Commons
Qiuyang Li, Kaifeng Wu, Haiming Zhu

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(9), P. 5695 - 5763

Published: April 17, 2024

The properties of colloidal quantum-confined semiconductor nanocrystals (NCs), including zero-dimensional (0D) quantum dots, 1D nanorods, 2D nanoplatelets, and their heterostructures, can be tuned through size, dimensionality, material composition. In photovoltaic photocatalytic applications, a key step is to generate spatially separated long-lived electrons holes by interfacial charge transfer. These transfer have been extensively studied recently, which the subject this Review. Review starts with summary electronic structure optical 0D-2D nanocrystals, followed advances in wave function engineering, novel way control spatial distribution holes, dimension, It discusses dependence NC on various parameters development Auger-assisted model. Recent understanding multiple exciton generation, decay, dissociation are also discussed, an emphasis carrier Finally, applications nanocrystal-based systems for photocatalysis reviewed, focusing photodriven separation recombination processes that dictate performance these materials. ends outlook remaining challenges promising future directions field.

Language: Английский

Citations

26
Engineering Metal Halide Perovskite Nanocrystals with BODIPY Dyes for Photosensitization and Photocatalytic Applications DOI Creative Commons
Alejandro Cortés‐Villena, Delia Bellezza, Carla Cunha

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(21), P. 14479 - 14492

Published: April 4, 2024

The sensitization of surface-anchored organic dyes on semiconductor nanocrystals through energy transfer mechanisms has received increasing attention owing to their potential applications in photodynamic therapy, photocatalysis, and photon upconversion. Here, we investigate the visible-light excitation two nanohybrids based CsPbBr

Language: Английский

Citations

22
Energy‐Transfer Photocatalysis Using Lead Halide Perovskite Nanocrystals: Sensitizing Molecular Isomerization and Cycloaddition DOI
Meng Liu, Pan Xia, Guohui Zhao

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(35)

Published: July 7, 2022

Abstract A relatively new addition to the application portfolio of lead halide perovskites is photosensitize molecular triplets for a variety photochemical applications. Here we report visible‐light‐driven isomerization and cycloaddition organic molecules sensitized by spectrally‐tunable perovskite nanocrystals. We first demonstrate with stilbene as substrate molecule that photoisomerization can proceed efficiently rapidly either directly grafting carboxylated onto nanocrystal surfaces or using triplet–acceptor ligands energy relay. The relay approach more generally applicable it does not require anchoring‐group functionalization molecules, allowing us facilely extend series substituted ring‐closing diarylethene, well intermolecular [2+2] acenaphthylene. This study opens an avenue energy‐transfer photocatalysis

Language: Английский

Citations

45
Structurally Flexible Au–Cu Alloy Nanoclusters Enabling Efficient Triplet Sensitization and Photon Upconversion DOI

Daichi Arima,

Masaaki Mitsui

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(12), P. 6994 - 7004

Published: March 20, 2023

Ligand-protected noble-metal nanoclusters exhibit an innately triplet nature and have been recently recognized as emerging platforms for sensitizers of photon upconversion (UC) via triplet-triplet annihilation. Herein, we report that a structurally flexible Au-Cu alloy nanocluster, [Au4Cu4(S-Adm)5(DPPM)2]+ (Au4Cu4; S-Adm = 1-adamantanethiolate, DPPM bis(diphenylphosphino)methane), exhibited favorable sensitizer properties superior UC performance. Contrary to the rigid Au2Cu6(S-Adm)6(TPP)2 (Au2Cu6, TPP triphenylphosphine), Au4Cu4 significantly better characteristics, such near-unity quantum yield intersystem crossing (ISC), long lifetime (ca. 8 μs), efficient energy transfer (TET). The ISC was attributed practically negligible activation barriers during process, which caused by spin-orbit interaction between two isoenergetic isomers predicted theoretical calculations. A series aromatic molecules with different energies were used acceptors reveal driving force dependence TET rate constant (kTET). This dependency analyzed evaluate sensitization ability nanoclusters. results showed maximum value kTET seven times larger than Au2Cu6, presumably reflects structural/electronic fluctuations state residence. combination 9,10-diphenylanthracene (DPA) annihilator/emitter achieved internal yields 14% (out 50% maximum) extremely low threshold intensities (2-26 mWcm-2). performance far exceeds Au2Cu6 is also outstanding among organic-inorganic hybrid nanomaterials reported so far.

Language: Английский

Citations

31
Synthesis and hybridization of CuInS2 nanocrystals for emerging applications DOI
Bing Chen, Weilin Zheng, Fengjun Chun

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(23), P. 8374 - 8409

Published: Jan. 1, 2023

This review article focuses on the recent advances and emerging opportunities for CuInS 2 nanocrystals in luminescence opto-electric applications enabled by advanced synthetic methodologies hybridization techniques.

Language: Английский

Citations

29
Interfacial Charge Transfer Regulates Photoredox Catalysis DOI Creative Commons
Chen Ye, De-Shan Zhang, Bin Chen

et al.

ACS Central Science, Journal Year: 2024, Volume and Issue: 10(3), P. 529 - 542

Published: Feb. 26, 2024

Photoredox catalytic processes offer the potential for precise chemical reactions using light and materials. The central determinant is identified as interfacial charge transfer, which simultaneously engenders distinctive behavior in overall reaction. An in-depth elucidation of main mechanism highlighting complexity transfer can occur through both diffusive direct models, revealing its sophisticated design complex transformations. fundamental photophysics uncover these comprehensive applications a clue future development. This research contributes to growing body knowledge on photoredox catalysis sets stage further exploration this fascinating area research.

Language: Английский

Citations

12
Triplet-Mediator Ligand-Protected Metal Nanocluster Sensitizers for Photon Upconversion DOI

Daichi Arima,

Shion Hidaka,

So Yokomori

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(24), P. 16630 - 16638

Published: May 13, 2024

Triplet–triplet annihilation photon upconversion (TTA-UC) is attracting a great deal of attention as viable approach to exploit unutilized wavelengths light in solar-driven devices. Recently, ligand-protected metal nanoclusters have emerged compelling platform for serving triplet sensitizers TTA-UC. In this study, we developed an atomically precise, triplet-mediator ligand (TL)-protected nanocluster, Au2Cu6(S-Adm)6[P(DPA)3]2 (Au2Cu6DPA; S-Adm = 1-adamanthanethiolate, DPA 9,10-diphenylanthracene). Au2Cu6DPA, the excitation Au2Cu6 core rapidly generates metal-to-ligand charge transfer state, followed by formation long-lived state (approximately 150 μs) at site TL. By combining Au2Cu6DPA with annihilator, achieved red-to-blue quantum yield (ΦUCg) 20.7 ± 0.4% (50% max.) low threshold intensity 36 mW cm–2 640 nm. This almost reaches maximum limit achievable using annihilator and establishes record-setting value, outperforming previously reported nanocrystal nanocluster sensitizers. Furthermore, strong emission based on pseudo-first-order TTA process was observed under 1 sun illumination, indicating that sensitizer holds promise applications solar-energy-based systems.

Language: Английский

Citations

10