The physics of electrons, photons, and their plasmonic interactions changes greatly when one or more dimensions are reduced down to the nanometer scale 1 . For example, graphene shows unique electrical, optical, and plasmonic properties, which are tunable through gating or chemical doping 2-5 . Similarly, ultrathin metal films (UTMFs) down to atomic thickness can possess new quantum optical effects 6,7 , peculiar dielectric properties 8 , and predicted strong plasmons 9,10 . However, truly two-dimensional plasmonics in metals has so far elusive because of the difficulty in producing large areas of sufficiently thin continuous films. Thanks to a deposition technique that allows percolation even at 1 nm thickness, we demonstrate plasmons in few-nanometer gold UTMFs, with clear evidence of new dispersion regimes and large electrical tunability. Resonance peaks at 1.5-5 m wavelengths are shifted by hundreds of nanometers and amplitude-modulated by tens of per cent through gating using relatively low voltages. The results suggest ways to use metals in plasmonic applications, such as electrooptic modulation, bio-sensing, and smart windows. Main text:Since ancient times, plasmons in nanoparticles of noble metals such as silver and gold have been used to color glass, culminating during the last two decades with a remarkable broadening of the use of plasmon excitations triggered by an improved understanding of their origin and behaviour, as well as by the availability of more sophisticated means to synthesize and pattern the metals [11][12][13] . New applications promise to have an impact on the optical industry: for example, super lenses allowing unprecedented sub-diffraction-limited optical imaging 14 , metasurfaces providing on-chip functionality in ultrathin form factor 15 , light modulation 16 , compact biosensors 17 and electrochemical effects that can be used in smart windows 18 . All
Ultrathin metal films (UTMFs) are widely used in optoelectronic applications, from transparent conductors to photovoltaic cells, low emissivity windows, and plasmonic metasurfaces. During the initial deposition phase, many metals tend to form islands on the receiving substrate rather than a physically connected (percolated) network, which eventually evolves into continuous films as the thickness increases. For example, in the case of Ag and Au on dielectric surfaces, percolation begins when the thickness of the metal film is at least about 5 nm. It is known that the type of growth can be changed when a proper seed layer is used. Here, we show that a CuO layer directly deposited on a substrate can dramatically influence surface wetting and promote early percolation of polycrystalline Ag and Au UTMFs. We demonstrate that the proposed seed is effective even when its thickness is sub-nanometric, in this way maintaining the full transparency of the receiving substrate. The Ag and Au films seeded with CuO showed a percolation thickness close to 1 nm and were morphologically and optically characterized from an ultraviolet (λ = 300 nm) to a midinfrared (λ = 15 μm) wavelength. Infrared reflectors, a mirror and a resonant plasmonic structure, were also demonstrated and uniquely tuned by electrical gating, this being possible owing to the small thickness of the constituting Au UTMF.
We compare experimental fluctuation electron microscopy (FEM) speckle data with electron diffraction simulations for thin amorphous carbon and silicon samples. We find that the experimental speckle intensity variance is generally more than an order of magnitude lower than kinematical scattering theory predicts for spatially coherent illumination. We hypothesize that decoherence, which randomizes the phase relationship between scattered waves, is responsible for the anomaly. Specifically, displacement decoherence can contribute strongly to speckle suppression, particularly at higher beam energies. Displacement decoherence arises when the local structure is rearranged significantly by interactions with the beam during the exposure. Such motions cause diffraction speckle to twinkle, some of it at observable time scales. We also find that the continuous random network model of amorphous silicon can explain the experimental variance data if displacement decoherence and multiple scattering is included in the modeling. This may resolve the longstanding discrepancy between X-ray and electron diffraction studies of radial distribution functions, and conclusions reached from previous FEM studies. Decoherence likely affects all quantitative electron imaging and diffraction studies. It likely contributes to the so-called Stobbs factor, where high-resolution atomic-column image intensities are anomalously lower than predicted by a similar factor to that observed here.
This work presents a spectroscopic study of the thermally enhanced photoinduced electron emission from nitrogen-doped diamond films prepared on p-type silicon substrates. It has been shown that photonenhanced thermionic emission (PETE) can substantially enhance thermionic emission intensity from a p-type semiconductor. An n-type diamond/p-type silicon structure was illuminated with 400-450 nm light, and the spectra of the emitted electrons showed a work function less than 2 eV and nearly an order of magnitude increase in emission intensity as the temperature was increased from ambient to ß400°C. Thermionic emission was negligible in this temperature range. The results are modeled in terms of contributions from PETE and direct photoelectron emission, and the large increase is consistent with a PETE component. The results indicate possible application in combined solar/thermal energy conversion devices.
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