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The study of the non-linear response of matter to high electric fields has recently encompassed harmonic generation in solids at near-infrared (NIR) driving wavelengths. Interest has been driven by the prospect of ultrafast signal processing and all-optical mapping of electron wave-functions in solids. Engineering solid-state band structures to control the non-linear process has already been highlighted theoretically. Here, we show experimentally for the first time that second harmonic generation (SHG) can be enhanced by doping crystals of magnesium oxide (MgO) with chromium (Cr) atoms. We show that the degree of enhancement depends non-linearly on dopant concentration. The SHG efficiency is shown to increase when Cr dopants are introduced into pure MgO. A physical picture of the effect of Cr dopants is aided by density functional theory (DFT) calculations of the electronic structure for pure and doped samples. This work shows an unambiguous enhancement of the SHG efficiency by modifying the electronic structure. The observed effects are consistent with an electronic structure that facilitates the surface induced SHG and demonstrates a minimal angular dependence. This work highlights the potential of manipulating the electronic structure of solids to control or test theories of their non-linear optical response., Comment: We have some technical and scientific issues in this article which need to be corrected

The enhancement and control of non-linear phenomena at a nanometer scale has a wide range of applications in science and in industry. Among these phenomena, high-harmonic generation in solids is a recent focus of research to realize next generation petahertz optoelectronic devices or compact all solid state EUV sources. Here, we report on the realization of the first nanoscale high harmonic source. The strong field regime is reached by confining the electric field from a few nanojoules femtosecond laser in a single 3D semiconductor waveguide. We reveal a strong competition between enhancement of coherent harmonics and incoherent fluorescence favored by excitonic processes. However, far from the band edge, clear enhancement of the harmonic emission is reported with a robust sustainability offering a compact nanosource for applications. We illustrate the potential of our harmonic nano-device by performing a coherent diffractive imaging experiment. Ultra-compact UV/X-ray nanoprobes are foreseen to have other potential applications such as petahertz electronics, nano-tomography or nano-medicine.

Light beams carrying orbital angular momentum (OAM) have led to stunning applications in various fields from quantum information to microscopy. In this letter, we examine OAM from the recently discovered high-harmonic generation (HHG) in semiconductor crystals. HHG from solids could be a valuable approach for integrated high-flux short-wavelength coherent light sources. The solid state nature of the generation medium allows the possibility to tailor directly the radiation at the source of the emission and offers a substantial degree of freedom for spatial beam shaping. First, we verify the fundamental principle of the transfer and conservation of the OAM from the generation laser to the harmonics. Second, we create OAM beams by etching a spiral zone structure directly at the surface of a zinc oxide crystal. Such diffractive optics act on the generated harmonics and produces focused optical vortices with nanometer scale sizes that may have potential applications in nanoscale optical trapping and quantum manipulation.

Nanoscale amplification of non-linear processes in solid-state devices opens novel applications in nano-electronics, nano-medicine or high energy conversion for example. Coupling few nano-joules laser energy at a nanometer scale for strong field physics is demonstrated. We report enhancement of high harmonic generation in nano-structured semiconductors using nanoscale amplification of a mid-infrared laser in the sample rather than using large laser amplifier systems. Field amplification is achieved through light confinement in nano-structured semiconductor 3D waveguides. The high harmonic nano-converter consists of an array of zinc-oxide nanocones. They exhibit a large amplification volume, 6 orders of magnitude larger than previously reported and avoid melting observed in metallic plasmonic structures. The amplification of high harmonics is observed by coupling only 5-10 nano-joules of a 3.2 {\mu}m high repetition-rate OPCPA laser at the entrance of each nanocone. Harmonic amplification (factor 30) depends on the laser energy input, wavelength and nanocone geometry.

We experimentally demonstrate the use of subwavelength optical nanoantennae to assist the gentle ablation of nanostructures directly using ultralow fluence from a Ti: sapphire oscillator through the excitation of surface plasmon waves. We show that this ablation mechanism is the same for metal and dielectric. The analytical solutions of ablation threshold are in excellent agreement with the experiment estimations. Surface plasmon assisted locally enhanced ablation at nanoscale provides a method for nanomachining, manipulation and modification the nanostructures without collateral thermal damage to the materials. It is also shown that this ablation can deposit low-density high quality thin nano film., Comment: 4 pages, 4 figures

We investigate theoretically and numerically the coupling between elastic and localized surface plasmon modes in a system of gold nanocylinders separated from a thin gold film by a dielectric spacer of few nanometers thickness. That system supports plasmon modes confined in between the bottom of the nanocylinder and the top of the gold film, which arise from the formation of interference patterns by short-wavelength metal-insulator-metal propagating plasmon. First we present the plasmonic properties of the system though computer-simulated extinction spectra and field maps associated to the different optical modes. Next a simple analytical model is introduced, which allows to correctly reproduce the shape and wavelengths of the plasmon modes. This model is used to investigate the efficiency of the coupling between an elastic deformation and the plasmonic modes. In the last part of the paper, we present the full numerical simulations of the phononic properties of the system, and then compute the acousto-plasmonic coupling between the different plasmon modes and five acoustic modes of very different shape. The efficiency of the coupling is assessed first by evaluating the modulation of the resonance wavelength, which allows comparison with the analytical model, and finally in term of time-modulation of the transmission spectra on the full visible range, computed for realistic values of the deformation of the nanoparticle., Comment: 12 pages, 9 figures