The discovery in 1974 of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is considered a landmark in the history of spectroscopic and analytical techniques. Much experimental and theoretical effort has been spent toward understanding the surface enhanced Raman scattering (SERS) effect, and demonstrating its potential toward various types of ultrasensitive sensing applications in a wide variety of fields. Forty five years later, SERS has blossomed as an extremely rich area of research and technology, but additional efforts are still needed before it can be routinely used as a commercial product. In this Review, prominent authors from all over the world joined efforts to summarize the current state-of-the-art in understanding and using SERS, as well as to propose what can be expected in the near future, in terms of research, applications, and technological development.

Placing a light emitter in an ultra-small optical cavity results in coupling between matter and light, generating new forms of emission that can be exploited in practical or fundamental applications; here, a system is described in which strong light–matter coupling occurs at room temperature and in ambient conditions by aligning single dye molecules in the optical cavities between gold nanoparticles and surfaces. When a light-emitter is placed in a high-quality optical cavity, where light remains confined for a long time, coupling between matter and light occurs. This coupling produces new forms of light that can be exploited in practical or fundamental applications such as low-power switches or quantum information networks. Jeremy Baumberg and colleagues demonstrate an unusual system, of interest for photochemistry studies, where the fully mixed, strong-coupling regime is reached for single dye molecules at room temperature and in ambient conditions. The system is assembled by aligning dye molecules using a host–guest chemistry approach in plasmonic gaps (the optical cavities) between gold nanoparticles and surfaces. The authors demonstrate strong statistical evidence for single-molecule strong coupling. This opens up the possibility of exploring the chemical structure of molecules with light-dressed states. Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extraction of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter1,2, forming building blocks for quantum information systems and for ultralow-power switches and lasers3,4,5,6. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complicated fabrication methods, compromising its use5,7,8. Here, by scaling the cavity volume to less than 40 cubic nanometres and using host–guest chemistry to align one to ten protectively isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light–matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue molecules, decreasing to 90 millielectronvolts for single molecules—matching quantitative models. Statistical analysis of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis9 and the possibility of manipulating chemical bonds10.

A cool route to nanospectroscopy: Confining light to a cavity is often used to enhance the interaction between the light and a particle stored within the cavity. Benz et al. worked with a self-assembled monolayer of biphenyl-4-thiol molecules sandwiched between a gold film and a gold nanoparticle. They used laser irradiation to move atoms in the nanoparticle and produced a “picocavity” that was stable at cryogenic temperatures. The authors were then able to obtain time-dependent Raman spectra from individual molecules. Such subwavelength cavities that can localize light to volumes well below 1 nm ³ will enable optical experiments on the atomic scale. Science , this issue p. 726

Metallic structures with nanogap features have proven highly effective as building blocks for plasmonic systems, as they can provide a wide tuning range of operating frequencies and large near-field enhancements. Recent work has shown that quantum mechanical effects such as electron tunnelling and nonlocal screening become important as the gap distances approach the subnanometre length-scale. Such quantum effects challenge the classical picture of nanogap plasmons and have stimulated a number of theoretical and experimental studies. This review outlines the findings of many groups into quantum mechanical effects in nanogap plasmons, and discusses outstanding challenges and future directions.

Strong coupling of monolayer metal dichalcogenide semiconductors with light offers encouraging prospects for realistic exciton devices at room temperature. However, the nature of this coupling depends extremely sensitively on the optical confinement and the orientation of electronic dipoles and fields. Here, we show how plasmon strong coupling can be achieved in compact, robust, and easily assembled gold nano-gap resonators at room temperature. We prove that strong-coupling is impossible with monolayers due to the large exciton coherence size, but resolve clear anti-crossings for greater than 7 layer devices with Rabi splittings exceeding 135 meV. We show that such structures improve on prospects for nonlinear exciton functionalities by at least 10⁴, while retaining quantum efficiencies above 50%, and demonstrate evidence for superlinear light emission.