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      A Single-Emitter Gain Medium for Bright Coherent Radiation from a Plasmonic Nanoresonator

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          Abstract

          We theoretically demonstrate the generation and radiation of coherent nanoplasmons powered by a single three-level quantum emitter on a plasmonic nanoresonator. By pumping the three-level emitter in a Raman configuration, we show a pathway to achieve macroscopic accumulation of nanoplasmons due to stimulated emission in the nanoresonator despite their fast relaxation. Thanks to the antenna effect of the nanoresonator, the system acts as an efficient and bright nanoscopic coherent light source with a photon emission rate of hundreds of Terahertz and could be realized with solid-state emitters at room temperatures in pulse mode. We provide physical interpretations of the results and discuss their realization and implications for ultra-compact integration of optoelectronics.

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          Most cited references34

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          Plasmon lasers at deep subwavelength scale.

          Laser science has been successful in producing increasingly high-powered, faster and smaller coherent light sources. Examples of recent advances are microscopic lasers that can reach the diffraction limit, based on photonic crystals, metal-clad cavities and nanowires. However, such lasers are restricted, both in optical mode size and physical device dimension, to being larger than half the wavelength of the optical field, and it remains a key fundamental challenge to realize ultracompact lasers that can directly generate coherent optical fields at the nanometre scale, far beyond the diffraction limit. A way of addressing this issue is to make use of surface plasmons, which are capable of tightly localizing light, but so far ohmic losses at optical frequencies have inhibited the realization of truly nanometre-scale lasers based on such approaches. A recent theoretical work predicted that such losses could be significantly reduced while maintaining ultrasmall modes in a hybrid plasmonic waveguide. Here we report the experimental demonstration of nanometre-scale plasmonic lasers, generating optical modes a hundred times smaller than the diffraction limit. We realize such lasers using a hybrid plasmonic waveguide consisting of a high-gain cadmium sulphide semiconductor nanowire, separated from a silver surface by a 5-nm-thick insulating gap. Direct measurements of the emission lifetime reveal a broad-band enhancement of the nanowire's exciton spontaneous emission rate by up to six times owing to the strong mode confinement and the signature of apparently threshold-less lasing. Because plasmonic modes have no cutoff, we are able to demonstrate downscaling of the lateral dimensions of both the device and the optical mode. Plasmonic lasers thus offer the possibility of exploring extreme interactions between light and matter, opening up new avenues in the fields of active photonic circuits, bio-sensing and quantum information technology.
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            Single-molecule strong coupling at room temperature in plasmonic nanocavities

            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.
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              Demonstration of a spaser-based nanolaser.

              One of the most rapidly growing areas of physics and nanotechnology focuses on plasmonic effects on the nanometre scale, with possible applications ranging from sensing and biomedicine to imaging and information technology. However, the full development of nanoplasmonics is hindered by the lack of devices that can generate coherent plasmonic fields. It has been proposed that in the same way as a laser generates stimulated emission of coherent photons, a 'spaser' could generate stimulated emission of surface plasmons (oscillations of free electrons in metallic nanostructures) in resonating metallic nanostructures adjacent to a gain medium. But attempts to realize a spaser face the challenge of absorption loss in metal, which is particularly strong at optical frequencies. The suggestion to compensate loss by optical gain in localized and propagating surface plasmons has been implemented recently and even allowed the amplification of propagating surface plasmons in open paths. Still, these experiments and the reported enhancement of the stimulated emission of dye molecules in the presence of metallic nanoparticles lack the feedback mechanism present in a spaser. Here we show that 44-nm-diameter nanoparticles with a gold core and dye-doped silica shell allow us to completely overcome the loss of localized surface plasmons by gain and realize a spaser. And in accord with the notion that only surface plasmon resonances are capable of squeezing optical frequency oscillations into a nanoscopic cavity to enable a true nanolaser, we show that outcoupling of surface plasmon oscillations to photonic modes at a wavelength of 531 nm makes our system the smallest nanolaser reported to date-and to our knowledge the first operating at visible wavelengths. We anticipate that now it has been realized experimentally, the spaser will advance our fundamental understanding of nanoplasmonics and the development of practical applications.
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                Author and article information

                Journal
                2017-01-02
                Article
                1701.00386
                0f132f49-018a-450c-b8ba-1bafac779d20

                http://arxiv.org/licenses/nonexclusive-distrib/1.0/

                History
                Custom metadata
                15 pages, 7 figures
                physics.optics cond-mat.mes-hall quant-ph

                Quantum physics & Field theory,Nanophysics,Optical materials & Optics
                Quantum physics & Field theory, Nanophysics, Optical materials & Optics

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