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Stepwise Two-Photon-Induced Electron Transfer from Higher Excited States of Noncovalently Bound Porphyrin-CdS/ZnS Core/Shell Nanocrystals
摘要： There has been an increasing amount of interest in stepwise two-photon absorption (2PA)-induced photochemical reactions because of their extremely lower power thresholds compared to that of the simultaneous process and drastic reaction enhancements in some cases. However, stepwise 2PA-induced photochemical reactions were reported only in single chromophores and covalently bound bi-chromophores and there are few reports on these reactions in noncovalently bound systems because of weak electronic interactions among chromophores. This study demonstrated the stepwise 2PA-induced electron transfer from higher excited states in noncovalently bound protoporphyrin IX·CdS/ZnS core/shell nanocrystals (NCs). The electron transfer from higher excited states of porphyrin to CdS NCs successfully overcomes the activation barrier associated with the wide bandgap ZnS shell, indicating that a high reduction potential can be obtained with the stepwise 2PA process. The concept presented in this study can be applied to various noncovalently bound multi-chromophore systems to explore nonlinear photoresponses.
关键词： Nonlinear,Anti-Kasha type,colloidal nanocrystals,hybrid nanomaterial,hot electron transfer
更新于2025-09-23 15:21:01
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Tailoring Carrier Dynamics in Perovskite Solar Cells via Precise Di-mension and Architecture Control and Interfacial Positioning of Plasmonic Nanoparticles
摘要： Placing plasmonic nanoparticles (NPs) in close proximity to semiconductor nanostructures renders effective tuning of the optoelectronic properties of semiconductors through the localized surface plasmon resonance (LSPR)-induced enhancement of light absorption and/or promotion of carrier transport. Herein, we report on, for the first time, the scrutiny of carrier dynamics of perovskite solar cells (PSCs) via sandwiching monodisperse plasmonic/dielectric core/shell NPs with systematically varied dielectric shell thickness yet fixed plasmonic core diameter within electron transport layer (ETL). Specifically, a set of Au NPs with precisely controlled dimensions (i.e., fixed Au core diameter and tunable SiO2 shell thickness) and architectures (plain Au NPs and plasmonic/dielectric Au/SiO2 core/shell NPs) are first crafted by capitalizing on the star-like block copolymer nanoreactor strategy. Subsequently, these monodisperse NPs are sandwiched between the two consecutive TiO2 ETLs. Intriguingly, there exists a critical dielectric SiO2 shell thickness, below which hot electrons from Au core are readily injected to TiO2 (i.e., hot electron transfer (HET)); this promotes local electron mobility in TiO2 ETL, leading to improved charge transport and increased short-circuit current density (Jsc). It is also notable that the HET effect moves up the Fermi level of TiO2, resulting in an enhanced built-in potential and open-circuit voltage (Voc). Taken together, the PSCs constructed by employing a sandwich-like TiO2/Au NPs/TiO2 ETL exhibit both greatly enhanced Jsc and Voc, delivering champion PCEs of 18.81% and 19.42% in planar and mesostructured PSCs, respectively. As such, the judicious positioning of rationally designed monodisperse plasmonic NPs in ETL affords effective tailoring of carrier dynamics, thereby providing a unique platform for developing high-performance PSCs.
关键词： hot electron transfer,perovskite solar cells,plasmonic nanoparticles,carrier dynamics,localized surface plasmon resonance
更新于2025-09-23 15:19:57
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Plasmonic hot electron transfer in anisotropic Pt–Au nanodisks boosts electrochemical reactions in the visible-NIR region
摘要： Plasmonic hot electron transfer in anisotropic Pt–Au nanodisks boosts electrochemical reactions in the visible-NIR region. Anisotropic plasmonic metals have attracted significant attention in enhancing the catalytic performance of catalysts due to their broad light-harnessing capabilities and active hot electrons; however, limited investigations have been dedicated towards improving their electrochemical reaction performance in the visible and near infrared (NIR) regions. Herein, anisotropic Pt-edged Au nanodisks (NDs) were synthesized by controlling the preferential loading of Pt and used as catalysts for plasmon-enhanced electrochemical methanol oxidation reactions (MORs) under visible-NIR light irradiation by, and the light-enhanced electric current over the Pt-edged Au NDs was found to be 3-fold higher than that under dark conditions. Wavelength-dependent electric current over the Pt-edged Au NDs for the MOR in the visible-NIR light region demonstrates that the light-induced enhancement of the electric current is due to surface plasmon resonance (SPR) of the Au NDs. Furthermore, plasmonic hot electron transfer was studied by the single-particle photoluminescence images and spectra of Au NDs and Pt–Au NDs, and the dipole surface plasmon resonance (DSPR) mode was proved to be the main channel for hot electron transfer. During the electrochemical reaction under visible-NIR light irradiation, a plasmonic hot electron is transferred to the electrode, and a 'hot hole' is left on the surface, boosting the MOR.
关键词： Pt–Au nanodisks,Plasmonic hot electron transfer,electrochemical reactions,visible-NIR region
更新于2025-09-16 10:30:52
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Fast Photoelectric Conversion in the Near‐Infrared Enabled by Plasmon‐Induced Hot‐Electron Transfer
摘要： Interfacial charge transfer is a fundamental and crucial process in photoelectric conversion. If charge transfer is not fast enough, carrier harvesting can compromise with competitive relaxation pathways, e.g., cooling, trapping, and recombination. Some of these processes can strongly affect the speed and efficiency of photoelectric conversion. In this work, it is elaborated that plasmon-induced hot-electron transfer (HET) from tungsten suboxide to graphene is a sufficiently fast process to prevent carrier cooling and trapping processes. A fast near-infrared detector empowered by HET is demonstrated, and the response time is three orders of magnitude faster than that based on common band-edge electron transfer. Moreover, HET can overcome the spectral limit of the bandgap of tungsten suboxide (≈2.8 eV) to extent the photo-response to the communication band of 1550 nm (≈0.8 eV). These results indicate that plasmon-induced HET is a new strategy for implementation of efficient and high-speed photoelectric devices.
关键词： localized surface plasmon resonance,infrared photodetection,photoelectric conversion,hot-electron transfer,graphene
更新于2025-09-11 14:15:04
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Overall water splitting and hydrogen peroxide synthesis by gold nanoparticle-based plasmonic photocatalysts
摘要： Gold nanoparticle-based plasmonic photocatalysts can be driven by excitation of the localized surface plasmon resonance. Among them, hot-electron transfer-type photocatalysts have recently attracted interest as promising solar-to-chemical converters owing to the wide spectral response from visible-to-infrared light. This Minireview highlights recent studies on two kinds of artificial photosynthesis - water splitting and H2O2 synthesis from water and oxygen - using hot-electron transfer-type plasmonic photocatalysts with particular emphasis placed on the electrocatalysis of Au nanoparticles.
关键词： water splitting,gold nanoparticle,hot-electron transfer,hydrogen peroxide synthesis,plasmonic photocatalysts
更新于2025-09-11 14:15:04
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Disentangling the Electron and Hole Dynamics in Janus CdSe/PbSe Nanocrystals through Variable Pump Transient Absorption Spectroscopy
摘要： CdSe/PbSe Janus hetero-nanocrystals (HNCs) represent an interesting system where structurally immiscible CdSe and PbSe co-exist in a single structure with intermixed electronic states. Here, we have investigated the carrier dynamics in Janus CdSe/PbSe HNCs through ultrafast transient absorption spectroscopy by selectively exciting either the CdSe or the PbSe domains. Upon excitation of the CdSe domain sub-picosecond hole transfer to the hybrid interfacial PbSe states were identified. On the other hand, the transfer of hot electron from PbSe to CdSe was evident upon creation of hot electrons in PbSe domain without exciting the CdSe domain. The photo-excited hot hole also gets transferred to the hybrid interfacial states in sub-ps time (~1ps) bleaching the corresponding transition. The decay of the localized hole was found to be much slower compared to the electron which can be beneficial for carrier extraction and multiexciton generation. The finding of hot electron transfer in a single structure and slow decay of holes can thus prove to be advantageous for future design of photovoltaic devices.
关键词： carrier dynamics,ultrafast transient absorption spectroscopy,CdSe/PbSe Janus hetero-nanocrystals,photovoltaic devices,hot electron transfer
更新于2025-09-10 09:29:36