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1.
Small ; : e2310414, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38294968

RESUMO

As opposed to natural photosynthesis, a significant challenge in a semiconductor-based photocatalyst is the limited hole extraction efficiency, which adversely affects solar-to-fuel efficiency. Recent studies have demonstrated that photocatalysts featuring spatially isolated dual catalytic oxidation/reduction sites can yield enhanced hole extraction efficiencies. However, the decay dynamics of excited states in such photocatalysts have not been explored. Here a ternary barbell-shaped CdS/MoS2 /Cu2 S heterostructure is prepared, comprising CdS nanorods (NRs) interfaced with MoS2 nanosheets at both ends and Cu2 S nanoparticles on the sidewall. By using transient absorption (TA) spectra, highly efficient charge separation within the CdS/MoS2 /Cu2 S heterostructure are identified. This is achieved through directed electron transfer to the MoS2 tips at a rate constant of >8.3 × 109 s-1 and rapid hole transfer to the Cu2 S nanoparticles on the sidewall at a rate of >6.1 × 1010 s-1 , leading to an exceptional overall charge transfer constant of 2.3 × 1011 s-1 in CdS/MoS2 /Cu2 S. The enhanced hole transfer efficiency results in a remarkably prolonged charge-separated state, facilitating efficient electron accumulation within the MoS2 tips. Consequently, the ternary CdS/MoS2 /Cu2 S heterostructure demonstrates a 22-fold enhancement in visible-light-driven H2 generation compare to pure CdS nanorods. This work highlights the significance of efficient hole extraction in enhancing the solar-to-H2 performance of semiconductor-based heterostructure.

2.
Small ; 19(18): e2207173, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36740721

RESUMO

The relatively short-lived excited states, such as the nascent electron-hole pairs (excitons) and the shallow trapping states, in semiconductor-based photocatalysts produce an exceptionally high charge carrier recombination rate, dominating a low solar-to-fuel performance. Here, a π-conjugated in-plane heterostructure between graphitic carbon nitride (g-CN) and carbon rings (Crings ) (labeling g-CN/Crings ) is effectively synthesized from the thermolysis of melamine-citric acid aggregates via a microwave-assisted heating process. The g-CN/Crings in-plane heterostructure shows remarkably suppressed excited-state decay and increased charge carrier population in photocatalysis. Kinetics analysis from the femtosecond time-resolved transient absorption spectroscopy illustrates that the g-CN/Crings π-conjugated heterostructure produces slower exciton annihilation (τ1  = 7.9 ps) and longer shallow electron trapping (τ2  = 407.1 ps) than pristine g-CN (τ1  = 3.6 ps, τ2  = 264.1 ps) owing to Crings incorporation, both of which enable more photoinduced electrons to participate in the photocatalytic reactions, thereby realizing photoactivity enhancement. As a result, the photocatalytic activity exhibits an eightfold enhancement in visible-light-driven H2 generation. This work provides a viable route of constructing π-conjugated in-plane heterostructures to suppress the excited-state decay and improve the photocatalytic performance.

3.
eLight ; 3(1): 1, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36618904

RESUMO

Integrated silicon photonics has sparked a significant ramp-up of investment in both academia and industry as a scalable, power-efficient, and eco-friendly solution. At the heart of this platform is the light source, which in itself, has been the focus of research and development extensively. This paper sheds light and conveys our perspective on the current state-of-the-art in different aspects of application-driven on-chip silicon lasers. We tackle this from two perspectives: device-level and system-wide points of view. In the former, the different routes taken in integrating on-chip lasers are explored from different material systems to the chosen integration methodologies. Then, the discussion focus is shifted towards system-wide applications that show great prospects in incorporating photonic integrated circuits (PIC) with on-chip lasers and active devices, namely, optical communications and interconnects, optical phased array-based LiDAR, sensors for chemical and biological analysis, integrated quantum technologies, and finally, optical computing. By leveraging the myriad inherent attractive features of integrated silicon photonics, this paper aims to inspire further development in incorporating PICs with on-chip lasers in, but not limited to, these applications for substantial performance gains, green solutions, and mass production.

4.
ACS Appl Mater Interfaces ; 13(15): 17141-17157, 2021 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-33844908

RESUMO

Memristors have attracted considerable attention as one of the four basic circuit elements besides resistors, capacitors, and inductors. Especially, the nonvolatile memory devices have become a promising candidate for the new-generation information storage, due to their excellent write, read, and erase rates, in addition to the low-energy consumption, multistate storage, and high scalability. Among them, halide perovskite (HP) memristors have great potential to achieve low-cost practical information storage and computing. However, the usual lead-based HP memristors face serious problems of high toxicity and low stability. To alleviate the above issues, great effort has been devoted to develop lead-free HP memristors. Here, we have summarized and discussed the advances in HP memristors from lead-based to lead-free materials including memristive properties, stability, neural network applications, and memristive mechanism. Finally, the challenges and prospects of lead-free HP memristors have been discussed.

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