Journal
NANO LETTERS
Volume 21, Issue 3, Pages 1461-1468Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c04614
Keywords
hot-electron transfer; localized surface plasmon resonances; photocatalysis; semiconductor nanoparticles; ultrafast optical spectroscopy
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Funding
- Israel Science Foundation [1363/18]
- PRIN 2017 Project [201795SBA3]
- Horizon 2020 [654148]
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Recent research has shown that charge separation in hybrid metal-semiconductor nanoparticles can be achieved through photoexcitation, offering intriguing possibilities for photocatalytic systems. By studying CdSe-Au HNPs, the complete pathways of electron transfer for semiconductor and localized surface plasmon resonance excitation were described, revealing the potential for diverse photocatalytic applications utilizing the combined effects of excitonic and plasmonic contributions.
Recently, it was demonstrated that charge separation in hybrid metal-semiconductor nanoparticles (HNPs) can be obtained following photoexcitation of either the semiconductor or of the localized surface plasmon resonance (LSPR) of the metal. This suggests the intriguing possibility of photocatalytic systems benefiting from both plasmon and exciton excitation, the main challenge being to outcompete other ultrafast relaxation processes. Here we study CdSe-Au HNPs using ultrafast spectroscopy with high temporal resolution. We describe the complete pathways of electron transfer for both semiconductor and LSPR excitation. In the former, we distinguish hot and band gap electron transfer processes in the first few hundred fs. Excitation of the LSPR reveals an ultrafast (<30 fs) electron transfer to CdSe, followed by back-transfer from the semiconductor to the metal within 210 fs. This study establishes the requirements for utilization of the combined excitonic-plasmonic contribution in HNPs for diverse photocatalytic applications.
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