Emitters placed in an optical cavity experience an environment that changes their coupling to light. In the weak-coupling regime light extraction is enhanced, but more profound effects emerge in the single-molecule strong-coupling regime where mixed light-matter states form1,2. Individual two-level emitters in such cavities become non-linear for single photons, forming key building blocks for quantum information systems as well as ultra-low power switches and lasers3–6. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complex fabrication, severely compromising their use5,7,8. Here, by scaling the cavity volume below 40 nm3 and using host-guest chemistry to align 1-10 protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from >50 plasmonic nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10 molecules decreasing to 90 meV for single molecules, matching quantitative models. Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra provide 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 pathways towards manipulation of chemical bonds10.
Optical metamaterials and nanoplasmonics bridge the gap between conventional optics and the nanoworld. Exciting and technologically important capabilities range from subwavelength focusing and stopped light to invisibility cloaking, with applications across science and engineering from biophotonics to nanocircuitry. A problem that has hampered practical implementations have been dissipative metal losses, but the efficient use of optical gain has been shown to compensate these and to allow for loss-free operation, amplification and nanoscopic lasing. Here, we review recent and ongoing progress in the realm of active, gain-enhanced nanoplasmonic metamaterials. On introducing and expounding the underlying theoretical concepts of the complex interaction between plasmons and gain media, we examine the experimental efforts in areas such as nanoplasmonic and metamaterial lasers. We underscore important current trends that may lead to improved active imaging, ultrafast nonlinearities on the nanoscale or cavity-free lasing in the stopped-light regime.
Light usually propagates inside transparent materials in well known ways. However, recent research has examined the possibility of modifying the way the light travels by taking a normal transparent dielectric and inserting tiny metallic inclusions of various shapes and arrangements. As light passes through these structures, oscillating electric currents are set up that generate electromagnetic field moments; these can lead to dramatic effects on the light propagation, such as negative refraction. Possible applications include lenses that break traditional diffraction limits and 'invisibility cloaks' (refs 5, 6). Significantly less research has focused on the potential of such structures for slowing, trapping and releasing light signals. Here we demonstrate theoretically that an axially varying heterostructure with a metamaterial core of negative refractive index can be used to efficiently and coherently bring light to a complete standstill. In contrast to previous approaches for decelerating and storing light, the present scheme simultaneously allows for high in-coupling efficiencies and broadband, room-temperature operation. Surprisingly, our analysis reveals a critical point at which the effective thickness of the waveguide is reduced to zero, preventing the light wave from propagating further. At this point, the light ray is permanently trapped, its trajectory forming a double light-cone that we call an 'optical clepsydra'. Each frequency component of the wave packet is stopped at a different guide thickness, leading to the spatial separation of its spectrum and the formation of a 'trapped rainbow'. Our results bridge the gap between two important contemporary realms of science-metamaterials and slow light. Combined investigations may lead to applications in optical data processing and storage or the realization of quantum optical memories.
Lasers that use metallic cavities have emerged recently as a new class of light source [1][2][3] . Plasmonic lasers achieve optical confinement and feedback using surface plasmon polaritons (SPPs), quasiparticles of photons and electrons at metal-dielectric interfaces, which can be amplified by suitable optical gain media 4 . The high gain of inorganic crystalline semiconductors is typically necessary to overcome fast electron scattering in metals (~10 fs), which leaves plasmonic lasers with high parasitic cavity loss. Nevertheless, SPPs offer the capability to reduce optical mode sizes far below the scale of the vacuum wavelength 3,5-8 leading to compact lasers that can generate extremely focussed optical excitations on potentially ultrafast time scales 1,9 with applications in Raman sensing
On the basis of a full-vectorial three-dimensional Maxwell-Bloch approach we investigate the possibility of using gain to overcome losses in a negative refractive index fishnet metamaterial. We show that appropriate placing of optically pumped laser dyes (gain) into the metamaterial structure results in a frequency band where the nonbianisotropic metamaterial becomes amplifying. In that region both the real and the imaginary part of the effective refractive index become simultaneously negative and the figure of merit diverges at two distinct frequency points.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
customersupport@researchsolutions.com
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
This site is protected by reCAPTCHA and the Google Privacy Policy and Terms of Service apply.
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.