Observation of inhomogeneous plasmonic field distribution in a nanocavity

Li, Chaoyu; Duan, Sai; Wen, Bo; Li, Songbo; Kathiresan, Murugavel; Xie, Liqiang; Chen, Shu; Anema, Jason R.; Mao, Bing‐Wei; Luo, Yi; Zhang, Tian; Li, Jianfeng

doi:10.1038/s41565-020-0753-y

Cited by 78 publications

(75 citation statements)

References 51 publications

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“…TEFE measures the fluorescence cross section in the far field with different incident wavelengths at a specific tip position. In other words, both the spectral resonance and different enhancement for different vibrational modes that can be experimentally calibrated by dark-field scattering spectra 46 have been neglected in the practical simulations. Owing to the constant quantum efficiency as we assumed above, the observed cross section (the downward red-solid arrows in Figure 1 b) is proportional to the absorbance of incident light.…”

Section: Methodsmentioning

confidence: 99%

Optical Images of Molecular Vibronic Couplings from Tip-Enhanced Fluorescence Excitation Spectroscopy

Qiu

Gong

Cao

et al. 2021

JACS Au

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Tip-based photoemission spectroscopic techniques have now achieved subnanometer resolution that allows visualization of the chemical structure and even the ground-state vibrational modes of a single molecule. However, the ability to visualize the interplay between electronic and nuclear motions of excited states, i.e., vibronic couplings, is yet to be explored. Herein, we theoretically propose a new technique, namely, tip-enhanced fluorescence excitation (TEFE). TEFE takes advantage of the highly confined plasmonic field and thus can offer a possibility to directly visualize the vibronic effect of a single molecule in real space for arbitrary excited states in a given energy window. Numerical simulations for a single porphine molecule confirm that vibronic couplings originating from Herzberg–Teller (HT) active modes can be visually identified. TEFE further enables high-order vibrational transitions that are normally suppressed in the other plasmon-based processes. Images of the combination vibrational transitions have the same pattern as that of their parental HT active mode’s fundamental transition, providing a direct protocol for measurements of the activity of Franck–Condon modes of selected excited states. These findings strongly suggest that TEFE is a powerful strategy to identify the involvement of molecular moieties in the complicated electron–nuclear interactions of the excited states at the single-molecule level.

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Section: Methodsmentioning

confidence: 99%

Optical Images of Molecular Vibronic Couplings from Tip-Enhanced Fluorescence Excitation Spectroscopy

Qiu

Gong

Cao

et al. 2021

JACS Au

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“…For the first time, we measured plasmon field distributions in the nanocavity gap perpendicular to the surface by appropriately designing a molecular ruler-based system (Figure 2b). [22] A [22] Copyright 2020, Springer Nature. e) SEM and TEM images of Ag nanocubes.…”

Section: Plasmon-enhanced Raman Spectroscopymentioning

confidence: 99%

“…c) SERS spectra of viologen molecules in the nanogap, at distances away from the surface determined by the alkyl chain length n, where n = 4, 6, 8, 10, 12, and 14. d) Normalized Raman intensities for viologen molecules in the nanogap. Reproduced with permission [22]. Copyright 2020, Springer Nature.…”

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confidence: 99%

Plasmonic Core–Shell Nanomaterials and their Applications in Spectroscopies

et al. 2021

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“…For the first time, we measured the distribution of the plasmonic field inside the nanocavity with ~2 Å spatial resolution by the elaborate design of a molecular ruler (Figure 3D). [ 17 ] The atomically smooth single‐crystal surface of Au(111) was combined with the self‐assembled monolayers (SAMs) of viologen molecules. The single‐crystal surface was linked with the ending of the thiol group, and the signals of the detect molecular were provided by the bipyridinium group.…”

Section: Applications Of Core‐shell Nanostructuresmentioning

confidence: 99%

Plasmonic Core‐Shell Nanostructures Enhanced Spectroscopies

et al. 2021

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Comprehensive Summary Core‐shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies, catalysis, energy, and other fields because of their splendid properties such as multifunctionality, stability, and adjustability. In this article, we summarized the endeavors made by our group in the past decade about the core‐shell nanostructures in the shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) and plasmon‐enhanced spectroscopies. Meanwhile, the potential challenges and perspectives about core‐shell nanostructures in spectroscopies have also been proposed. Thus, we believe this article would provide an avenue for a comprehensive understanding of enhanced spectroscopies with core‐shell nanostructures. What is the most favorite and original chemistry developed in your research group?? Core‐shell nanostructure enhanced Raman spectroscopy for surface analysis. How do you get into this specific field? Could you please share some experiences with our readers?? I started the studies on Raman spectroscopy since I was a Ph.D. candidate. I think most researchers should concentrate on specific fields, especially those that can hardly be solved by others, and make constant research on them. How do you supervise your students?? First, give highly challenging or unique topics to students. Then, make detailed plans for them and supervise them to execute the plans. What is the most important personality for scientific research?? Insistence and diligence. What are your hobbies? What's your favorite book(s)? Playing computer games. My favorite book is State of Divinity (笑傲江湖), by Louis Cha. What is your favorite journal(s)? The journals report systematic and pioneer works on chemistry, materials, or energy, etc.

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Observation of inhomogeneous plasmonic field distribution in a nanocavity

Cited by 78 publications

References 51 publications

Optical Images of Molecular Vibronic Couplings from Tip-Enhanced Fluorescence Excitation Spectroscopy

Optical Images of Molecular Vibronic Couplings from Tip-Enhanced Fluorescence Excitation Spectroscopy

Plasmonic Core–Shell Nanomaterials and their Applications in Spectroscopies

Plasmonic Core‐Shell Nanostructures Enhanced Spectroscopies

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