High spatial resolution ambient tip-enhanced (multipolar) Raman scattering

El‐Khoury, Patrick Z.

doi:10.1039/d3cc00434a

Chem. Commun.

2023

DOI: 10.1039/d3cc00434a

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High spatial resolution ambient tip-enhanced (multipolar) Raman scattering

Patrick Z. El‐Khoury

Abstract: This article summarizes lessons learnt from ambient tip-enhanced Raman (TER) mapping of molecules interacting with plasmonic nanostructures. It is shown that numerous physical and chemical phenomena contribute to high-resolution TER...

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2024

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Classical vs. quantum plasmon-induced molecular transformations at metallic nanojunctions

Mantilla,

Wang,

Krayev

et al. 2024

Proc. Natl. Acad. Sci. U.S.A.

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Chemical transformations near plasmonic metals have attracted increasing attention in the past few years. Specifically, reactions occurring within plasmonic nanojunctions that can be detected via surface and tip-enhanced Raman (SER and TER) scattering were the focus of numerous reports. In this context, even though the transition between localized and nonlocal (quantum) plasmons at nanojunctions is documented, its implications on plasmonic chemistry remain poorly understood. We explore the latter through AFM-TER-current measurements. We use two molecules: i) 4-mercaptobenzonitrile (MBN) that reports on the (non)local fields and ii) 4-nitrothiophenol (NTP) that features defined signatures of its neutral/anionic forms and dimer product, 4,4′-dimercaptoazobenzene (DMAB). The transition from classical to quantum plasmons is established through our optical measurements: It is marked by molecular charging and optical rectification. Simultaneously recorded force and current measurements support our assignments. In the case of NTP, we observe the parent and DMAB product beneath the probe in the classical regime. Further reducing the gap leads to the collapse of DMAB to form NTP anions. The process is reversible: Anions subsequently recombine into DMAB. Our results have significant implications for AFM-based TER measurements and their analysis, beyond the scope of this work. In effect, when precise control over the junction is not possible (e.g., in SER and ambient TER), both classical and quantum plasmons need to be considered in the analysis of plasmonic reactions

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Classical vs. quantum plasmon-induced molecular transformations at metallic nanojunctions

Mantilla,

Wang,

Krayev

et al. 2024

Proc. Natl. Acad. Sci. U.S.A.

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show abstract

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High spatial resolution ambient tip-enhanced (multipolar) Raman scattering

Abstract: This article summarizes lessons learnt from ambient tip-enhanced Raman (TER) mapping of molecules interacting with plasmonic nanostructures. It is shown that numerous physical and chemical phenomena contribute to high-resolution TER...

Cited by 1 publication

References 35 publications

Classical vs. quantum plasmon-induced molecular transformations at metallic nanojunctions

Classical vs. quantum plasmon-induced molecular transformations at metallic nanojunctions

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