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  • Review Article
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From plasmon-enhanced molecular spectroscopy to plasmon-mediated chemical reactions

Nature Reviews Chemistry volume 2, pages 216–230 (2018)Cite this article

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Abstract

The excitation of surface plasmons (SPs) — collective oscillation of conduction-band electrons in nanostructures — can afford photon, electron and heat energy redistribution over time and space. Making use of this ability, plasmon-enhanced molecular spectroscopy (PEMS) techniques with ultra-high sensitivity and surface selectivity have attracted much attention and have undergone considerable development over the past four decades. Recently, the development of plasmon-mediated chemical reactions (PMCRs) has shown the potential to have a large impact on the practice of chemistry. PMCRs exhibit some obvious differences from and potential advantages over traditional thermochemistry, photochemistry and photocatalysis. However, our physicochemical understanding of PMCRs is still far from complete. In this Review, we analyse the similarities and distinctive features of PEMS and PMCRs and compare PMCRs with traditional photochemical and thermochemical reactions. We then discuss how PMCRs can be improved by rationally designing and fabricating plasmonic nanostructures, selecting suitable surface and interface mediators and teaming them synergistically.

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Fig. 1: Surface plasmon excitation, optical confinement and spectral features of some typical nanostructures.
Fig. 2: Three main effects induced by the excitation and relaxation of surface plasmons.
Fig. 3: The plasmon-enhanced Raman scattering process.
Fig. 4: A microscopic view of plasmon-mediated chemical reactions.
Fig. 5: The three key components of plasmon-mediated chemical reactions.
Fig. 6: A graphical summary of novel mechanisms of SP-mediated energy and/or charge transfer processes.
Fig. 7: Comparison of plasmon-enhanced molecular spectroscopy and plasmon-mediated chemical reactions.

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Acknowledgements

The authors are deeply grateful to M. Moskovits for his very helpful suggestions and careful academic and English editing of the manuscript. This work is financially supported by the National Natural Science Foundation of China (21533006, 21621091, 91427304 and 21403180) and the Ministry of Science and Technology of China (2015CB932300).

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Nature Reviews Chemistry thanks R. Aroca, S. Schlücker and the other anonymous reviewer(s) for their contribution to the peer review of this work.

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Authors and Affiliations

  1. State Key Laboratory for Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials, Xiamen University, Xiamen, China

    Chao Zhan, Xue-Jiao Chen, Jun Yi, Jian-Feng Li, De-Yin Wu & Zhong-Qun Tian

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  1. Chao Zhan
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  2. Xue-Jiao Chen
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  3. Jun Yi
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Contributions

Z-Q.T. conceived the outline. C.Z., X-J.C. and Z-Q.T. wrote the manuscript. J.Y. supplied the calculation in Figure 1. All authors contributed to discussions, editing and corrections. C.Z. and Z-Q.T. revised the manuscript before the final submission.

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Correspondence to Zhong-Qun Tian.

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Glossary

Optical diffraction limit

The fundamental maximum of the spatial resolution of an optical system that is due to diffraction.

Landau damping

The damping effect of longitudinal space charge waves in plasma or a similar environment. Landau damping occurs because of the energy exchange between an electromagnetic wave and particles (for example, electrons) in the plasma, which can interact strongly with the wave. In a surface plasmon system, the Landau damping process represents the direct absorption of a photon assisted by the surface plasmon momentum, creating a hot hole and a hot electron.

Fermi–Dirac distribution

The distribution of particles over energy states in systems consisting of many identical particles that obey the Pauli exclusion principle.

Electrostatic approximation

The assumption that the phase of the harmonically oscillating electromagnetic field is practically constant over the particle volume, so that one can calculate the spatial field distribution by assuming the simplified problem of a particle in an electrostatic field.

Drude model

A model used to explain the transport properties of electrons in materials in which the microscopic behaviour of electrons in a solid is treated classically. It is the basic model used in the study of optical properties of different materials and is commonly used to explain the dielectric function of plasmonic nanostructures.

Fermi level

The highest energy level that an electron can fill in the solid state at absolute zero temperature.

Förster resonance energy transfer

(FRET). A mechanism describing the energy transfer between two light-sensitive dipoles, in which energy non-radiatively transfers from a blueshifted emitter to a redshifted absorber through dipole–dipole coupling.

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Zhan, C., Chen, XJ., Yi, J. et al. From plasmon-enhanced molecular spectroscopy to plasmon-mediated chemical reactions. Nat Rev Chem 2, 216–230 (2018). https://doi.org/10.1038/s41570-018-0031-9

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