4.8 Article

Fermi Level Equilibration at the Metal-Molecule Interface in Plasmonic Systems

期刊

NANO LETTERS
卷 21, 期 15, 页码 6592-6599

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02003

关键词

Photocatalysis; catalysis; Fermi level; charge transfer; SERS

资金

  1. Romanian Ministry of Research and Innovation, CCCDI-UEFISCDI within PNCDI III [PN-III-P1-1.2-PCCDI-2017-0056, PN-III-P22.1-PED-2019-3268, PN-III-P4-ID-PCCF-2016-0112]
  2. Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under Germany's Excellence Strategy [EXC 2089/1-390776260]
  3. Bavarian program Solar Energies Go Hybrid (SolTech)
  4. Center for NanoScience (CeNS)
  5. European Commission through the ERC [802989]

向作者/读者索取更多资源

This study highlights a new metal-molecule charge transfer process by tuning the Fermi energy of plasmonic silver nanoparticles (AgNPs) in situ. The strong adsorption of halide ions upshifts the Fermi level of AgNPs, promoting spontaneous charge transfer to molecular acceptor orbitals. The catalytic role of halide ions in plasmonic nanostructures depends on their surface affinity compared to the target molecule, providing new insights into the interaction mechanisms.
We highlight a new metal-molecule charge transfer process by tuning the Fermi energy of plasmonic silver nanoparticles (AgNPs) in situ. The strong adsorption of halide ions upshifts the Fermi level of AgNPs by up to similar to 0.3 eV in the order Cl- < Br- < I-, favoring the spontaneous charge transfer to aligned molecular acceptor orbitals until charge neutrality across the interface is achieved. By carefully quantifying, experimentally and theoretically, the Fermi level upshift, we show for the first time that this effect is comparable in energy to different plasmonic effects such as the plasmoelectric effect or hot-carriers production. Moreover, by monitoring in situ the adsorption dynamic of halide ions in different AgNP-molecule systems, we show for the first time that the catalytic role of halide ions in plasmonic nanostructures depends on the surface affinity of halide ions compared to that of the target molecule.

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