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Plasmonic control: enter the spaser Nanoplasmonics — the nanoscale manipulation of surface plasmons (fluctuations in the electron density at a metallic surface) — could revolutionize applications ranging from sensing and biomedicine to imaging and information technology. But first, we need a simple and efficient method for actively generating coherent plasmonic fields. This is in theory possible with the spaser, first proposed in 2003 as a device that generates and amplifies surface plasmons in the same way that a laser generates and amplifies photons. Now Noginov et al . present the first unambiguous experimental demonstration of spasing, using 44-nm diameter nanoparticles with a gold core and dye-doped silica shell. The system generates stimulated emission of surface plasmons in the same way as a laser generates stimulated emission of coherent photons, and has been used to implement the smallest nanolaser reported to date, and the first operating at visible wavelengths. Nanoplasmonics promises to revolutionize applications ranging from sensing and biomedicine to imaging and information technology, but its full development is hindered by the lack of devices that can generate coherent plasmonic fields. In theory, this is possible with a so-called 'spaser' — analogous to a laser — which would generate stimulated emission of surface plasmons. This is now realized experimentally, and should enable many new technological developments. 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 1 , 2 . However, the full development of nanoplasmonics is hindered by the lack of devices that can generate coherent plasmonic fields. It has been proposed 3 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 4 , 5 , 6 to compensate loss by optical gain in localized and propagating surface plasmons has been implemented recently 7 , 8 , 9 , 10 and even allowed the amplification of propagating surface plasmons in open paths 11 . Still, these experiments and the reported enhancement of the stimulated emission of dye molecules in the presence of metallic nanoparticles 12 , 13 , 14 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 15 , 16 , 17 , 18 , 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.

We have studied effects of metal–dielectric substrates on photopolymerization of [2,2ʹ-Bi-1H-indene]-1,1ʹ-dione-3,3ʹ-diyl diheptanoate (BITh) monomer. We synthetized BITh and spin-coated it onto a variety of dielectric, metallic, and metal–dielectric substrates. The films were exposed to radiation of a UV–Visible Xe lamp, causing photo-polymerization of monomer molecules. The magnitude and the rate of the photo-polymerization were monitored by measuring the strength of the ~ 480 nm absorption band, which existed in the monomer but not in the polymer. Expectedly, the rate of photo-polymerization changed nearly linearly with the change of the pumping intensity. In contrast with our early study of photo-degradation of semiconducting polymer P3HT, the rate of photo-polymerization of BITh is getting modestly higher if the monomer film is deposited on top of silver separated from the monomer by a thin insulating MgF 2 layer preventing a charge transfer. This effect is partly due to a constructive interference of the incident and reflected light waves, as well as known in the literature effects of metal/dielectric substrates on a variety of spectroscopic and energy transfer parameters. At the same time, the rate of photopolymerization is getting threefold larger if monomer is deposited on Ag film directly and charge transfer is allowed. Finally, Au substrates cause modest (~ 50%) enhancement of both monomer film absorption and the rate of photo-polymerization.

Spontaneous emission is one of the most fundamental quantum phenomena in optics. Following the seminal work of Purcell and in agreement with the Fermi's Golden Rule, its rate can be controlled with the photonic density of states (PDOS). In recent years, this effect has been demonstrated in metamaterials with hyperbolic dispersion – highly anisotropic composite materials, which have a broad-band singularity of the density of photonic states. At this time, we show that hyperbolic metamaterials can control spontaneous emission spectra as well. Experimentally, DCM laser dye has been embedded into lamellar metal/dielectric metamaterial. The observed 18 nm blue shift of emission is explained by strong dispersion of the density of photonic states. On the other hand, practically no spectral shift has been observed in the excitation spectra of the same dye. This suggests that the effect of PDOS on spontaneous emission is very different from its effect on excitation and absorption.

Kirchhoff’s law of thermal radiation, relating emissivity and absorptance is commonly formulated for opaque bodies in thermodynamic equilibrium with the environment. However, in many systems of practical importance, both assumptions are often not satisfied. We revisit the century-old law and examine the limits of its applicability in an example of Er:YAG and Er:YLF dielectric crystals–potential radiation converters for thermophotovoltaic applications. The (80 at.%) Er:YAG crystal is opaque between 1.45 μm and 1.64 μm. In this spectral range, its absorptance α(λ) is spectrally flat and differentiates from unity only by a small amount of reflection. The shape of the emissivity spectrum ɛ(λ) closely matches that of absorptance α(λ), implying that the Kirchhoff’s law can adequately describe thermal radiation of opaque bodies, even if thermodynamic equilibrium is not satisfied. The (20 at.%) Er:YLF crystal had smaller size, lower concentration of Er ions, and it was not opaque. Nevertheless, its spectrum of emissivity had almost the same shape (between 1.45 μm and 1.62 μm) as the absorptance derived from the transmission measurements. Our results are consistent with the conclusion that the Kirchhoff’s law of thermal radiation can be extended (with caution) to not-opaque bodies away from the thermodynamic equilibrium.

Proximity to metallic surfaces, plasmonic structures, cavities and other inhomogeneous dielectric environments is known to control spontaneous emission, energy transfer, scattering and many other phenomena of practical importance. The aim of the present study was to demonstrate that, in spirit of the Marcus theory, the rates of chemical reactions can, too, be influenced by nonlocal dielectric environments, such as metallic films and metal/dielectric bilayer or multilayer structures. We have experimentally shown that metallic, composite metal/dielectric substrates can, indeed, control ordering as well as photodegradation of thin poly-3-hexylthiophene (p3ht) films. In many particular experiments, p3ht films were separated from metal by a dielectric spacer, excluding conventional catalysis facilitated by metals and making modification of the nonlocal dielectric environment a plausible explanation for the observed phenomena. This first step toward understanding of a complex relationship between chemical reactions and nonlocal dielectric environments is to be followed by the theory development and a broader scope of thorough experimental studies.

It has been recently shown that scores of physical and chemical phenomena (including spontaneous emission, scattering and Förster energy transfer) can be controlled by nonlocal dielectric environments provided by metamaterials with hyperbolic dispersion and simpler metal/dielectric structures. At this time, we have researched van der Waals interactions and experimentally studied wetting of several metallic, dielectric and composite multilayered substrates. We have found that the wetting angle of water on top of MgF 2 is highly sensitive to the thickness of the MgF 2 layer and the nature of the underlying substrate that could be positioned as far as ~100 nm beneath the water/MgF 2 interface. We refer to this phenomenon as long range wetting transparency. The latter effect cannot be described in terms of the most basic model of dispersion van der Waals-London forces based on pair-wise summation of dipole-dipole interactions across an interface or a gap separating the two media. We infer that the experimentally observed gradual change of the wetting angle with increase of the thickness of the MgF 2 layer can possibly be explained by the distance dependence of the Hamaker function (describing the strength of interaction), which originates from retardation of electromagnetic waves at the distances comparable to a wavelength.

We have studied photoinduced reduction of absorption and emission in p3ht, a semiconducting polymer, and found that the rate of photodegradation (destruction of the constituent thiophene rings) does not correlate with the luminescence intensity and, correspondingly, does not depend on the excited state concentration. This conclusion rules out Purcell enhancement of radiative decay rate as a possible explanation of the recently discovered reduction of the p3ht photodegradation rate in the vicinity of metallic substrates and lamellar metal-dielectric metamaterials.

We have studied angular distribution of emission of dye molecules deposited on lamellar metal/dielectric and Si/Ag nanowire based metamaterials with hyperbolic dispersion. In agreement with the theoretical prediction, the emission pattern of dye on top of lamellar metamaterial is similar to that on top of metal. At the same time, the effective medium model predicts the emission patterns of the nanowire array and the dye film deposited on glass to be nearly identical to each other. This is not the case of our experiment. We tentatively explain the nearly Lambertian (∝cosθ) angular distribution of emission of the nanowire based sample by a surface roughness.

Abstract We have studied effects of metal–dielectric substrates on photopolymerization of [2,2ʹ-Bi-1H-indene]-1,1ʹ-dione-3,3ʹ-diyl diheptanoate (BITh) monomer. We synthetized BITh and spin-coated it onto a variety of dielectric, metallic, and metal–dielectric substrates. The films were exposed to radiation of a UV–Visible Xe lamp, causing photo-polymerization of monomer molecules. The magnitude and the rate of the photo-polymerization were monitored by measuring the strength of the ~ 480 nm absorption band, which existed in the monomer but not in the polymer. Expectedly, the rate of photo-polymerization changed nearly linearly with the change of the pumping intensity. In contrast with our early study of photo-degradation of semiconducting polymer P3HT, the rate of photo-polymerization of BITh is getting modestly higher if the monomer film is deposited on top of silver separated from the monomer by a thin insulating MgF2layer preventing a charge transfer. This effect is partly due to a constructive interference of the incident and reflected light waves, as well as known in the literature effects of metal/dielectric substrates on a variety of spectroscopic and energy transfer parameters. At the same time, the rate of photopolymerization is getting threefold larger if monomer is deposited on Ag film directly and charge transfer is allowed. Finally, Au substrates cause modest (~ 50%) enhancement of both monomer film absorption and the rate of photo-polymerization.