Heavily doped semiconductors have emerged as tunable low-loss plasmonic materials at mid-infrared frequencies. In this article we investigate nonlinear optical phenomena associated with high concentration of free electrons. We use a hydrodynamic description to study free electron dynamics in heavily doped semiconductors up to third-order terms, which are usually negligible for noble metals. We find that cascaded third-harmonic generation due to second-harmonic signals can be as strong as direct third-harmonic generation contributions even when the second-harmonic generation efficiency is zero. Moreover, we show that when coupled with plasmonic enhancement free electron nonlinearities could be up to two orders of magnitude larger than conventional semiconductor nonlinearities. Our study might open a new route for nonlinear optical integrated devices at mid-infrared frequencies.
Plasmonic waveguides provide an integrated platform to develop efficient nanoscale ultrafast photonic devices. Theoretical models that describe nonlinear optical phenomena in plasmonic waveguides, usually, only incorporate bulk nonlinearities, while nonlinearities that arise from metallic constituents remained unexplored. In this work, we present a method that enables a generalized treatment of the nonlinearities present in plasmonic waveguides and use it to calculate second-harmonic generation from free electrons through a hydrodynamic nonlocal description. As a general application of our met…
Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanopartic…
Realizing strong coupling between a single quantum emitter (QE) and an optical cavity is of crucial importance in the context of various quantum optical applications. While Rabi splitting of single quantum emitters coupled to high-Q diffraction limited cavities have been reported in numerous configurations, attaining single emitter Rabi splitting with a plasmonic nanostructure is still elusive. Here, we establish the analytical condition for strong coupling between a single QE and a plasmonic nanocavity and apply it to study various plasmonic arrangements that were shown to enable Rabi splitti…
The n-type Ge-on-Si epitaxial material platform enables a novel paradigm for plasmonics in the mid-infrared, prompting the future development of lab-on-a-chip and subwavelength vibrational spectroscopic sensors. In order to exploit this material, through proper electrodynamic design, it is mandatory to retrieve the dielectric constants of the thin Ge epilayers with high precision due to the difference from bulk Ge crystals. Here we discuss the procedure we have employed to extract the real and imaginary part of the dielectric constants from normal incidence reflectance measurements, by combini…
From the demonstration of saturable absorption by Vavilow and Levshin in 1926, and with invention of the laser, unavailability of strongly nonlinear materials was a key obstacle for developing optical signal processing, in particular in transparent telecommunication networks. Today, most advanced photonic switching materials exploit gain dynamics and near-band and excitonic effects in semiconductors, nonlinearities in organic media with weakly-localized electrons and nonlinearities enhanced by hybridization with metamaterials. Here we report on a new type of artificial nonlinearity that is nan…
Plasmonic-cavity Modulator for the Mid-IR with a Semi-transparent and Nonlinear Heavily-doped Semiconductor Mirror
Istituto Italiano di Tecnologia（意大利理工学院）；Istituto di Fotonica e Nanotecnologie, Consiglio Nazionale delle Ricerche（国家研究委员会光子和纳米技术研究所）；University of Luxembourg（卢森堡大学）；Institute for Advanced Studies, University of Luxembourg Campus Belval（卢森堡大学贝尔瓦尔校区高等研究院）；Centre de Nanosciences et de Nanotechnologies (C2N), CNRS UMR 9001, Universit´e Paris-Saclay（巴黎萨克雷大学CNRS 9001联合实验室纳米科学与纳米技术中心）
Nanophotonic devices offer an unprecedented ability to concentrate light into small volumes which can greatly increase nonlinear effects. However, traditional plasmonic materials suffer from low damage thresholds and are not compatible with standard semiconductor technology. Here we study the nonlinear optical properties in the novel refractory plasmonic material titanium nitride using the Z scan method at 1550 nm and 780 nm. We compare the extracted nonlinear parameters for TiN with previous works on noble metals and note a similarly large nonlinear optical response. However, TiN films have b…
The spectral response of a plasmonic nanostructure may heavily depend on the refractive index of its surroundings. The key idea of this paper is to control this response by coherent optical means, i.e. with an optically controlled electromagnetically-induced-transparency medium. In such environment, an external laser provides a knob to shift the position of plasmonic resonances without the need to change the geometry of the nanostructure. Additionally, the setup can be exploited to excite narrow-band surface plasmon polaritons.
Recent metamaterial (MM) research faces several problems when using metal-based plasmonic components as building blocks for MMs. The use of conventional metals for MMs is limited by several factors: metals such as gold and silver have high losses in the visible and near-infrared (NIR) ranges and very large negative real permittivity values, and in addition, their optical properties cannot be tuned. These issues that put severe constraints on the device applications of MMs could be overcome if semiconductors are used as plasmonic materials instead of metals. Heavily doped, wide bandgap oxide se…
Tunable light filters are critical components for many optical applications in which light in-coupling, out-coupling or rejection is crucial, such as lasing, sensing, photovoltaics and information and communication technology. For this purpose, Bragg mirrors, band-pass filters with high reflectivity represent good candidates. However, their optical characteristics are determined at the stage of fabrication. Heavily doped semiconductor nanocrystals (NCs) on the other hand deliver a high degree of optical tunability through the active modulation of their carrier density ultimately influencing th…
We investigate enhanced harmonic generation processes in gain-assisted, near-zero permittivity metamaterials composed of spherical plasmonic nanoshells. We report the presence of narrow-band features in transmission, reflection and absorption induced by the presence of an active material inside the core of the nanoshells. The damping-compensation mechanism used to achieve the near-zero effective permittivity condition also induces a significant increase in field localization and strength and, consequently, enhancement of linear absorption. When only metal nonlinearities are considered, second …
Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light-matter interactions. These systems are expected to have nonlinear optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe2 monolayer strongly coupled to a single gold nano…
There is an active demand to develop efficient nanoscale nonlinear sources for applications in photonic circuitry, quantum optics and biosensing. To this end, plasmonic systems have been utilized to boost the nonlinear signal generation, however high efficiencies of frequency conversion for realistic applications remain a challenge. Metal-insulator-metal (MIM) nanocavities are good candidates for strongly concentrating the fields at the nanoscale to enhance the optical nonlinearities, however they typically suffer from the requirement to have a quadrupolar resonance at the emission wavelength.…
Plasmonic nanostructures and devices are rapidly transforming light manipulation technology by allowing to modify and enhance optical fields on sub-wavelength scales. Advances in this field rely heavily on the development of new characterization methods for the fundamental nanoscale interactions. However, the direct and quantitative mapping of transient electric and magnetic fields characterizing the plasmonic coupling has been proven elusive to date. Here we demonstrate how to directly measure the inelastic momentum transfer of surface plasmon modes via the energy-loss filtered deflection of …
Fully reconfigurable metasurfaces would enable new classes of optical devices that provide unprecedented control of electromagnetic beamforms. The principal challenge for achieving reconfigurability is the need to generate large tunability of subwavelength, low-Q metasurface resonators. Here, we demonstrate large refractive index tuning can be efficiently facilitated at mid-infrared wavelengths using novel temperature-dependent control over free-carrier refraction. In doped InSb we demonstrate nearly two-fold increase in the electron effective mass leading to a positive refractive index shift …
Understanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different, or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental differ…
Frequency conversion processes, such as second- and third-harmonic generation, are one of the most common effects in nonlinear optics which offer many opportunities for photonics, chemistry, material science, characterization, and biosensing. Given the inherently weak nonlinear response of natural materials, one typically relies on optically large samples and complex phase-matching techniques to achieve nonlinear effects. A direct translation of these approaches to small dimensions, however, is extremely challenging, because nonlinear effects locally comparable to the linear response cannot be…
We demonstrate heavy and hyper doping of ZnO by a combination of gallium (Ga) ion implantation using a focused ion beam (FIB) system and post-implantation laser annealing. Ion implantation allows for the incorporation of impurities with nearly arbitrary concentrations, and the laser-annealing process enables dopant activation close to or beyond the solid-solubility limit of Ga in ZnO. We achieved heavily doped ZnO:Ga with free-carrier concentrations of ~10^21 cm^(-3), resulting in a plasma wavelength of 1.02 um, which is substantially shorter than the telecommunication wavelength of 1.55 um. T…
Plasmon-Enhanced Second-Harmonic Generation in Atomically Thin Crystalline Silver Nanostructures
ICFO–Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology（ICFO-光子科学研究所，巴塞罗那科学技术研究院）；University of Vienna, Faculty of Physics, Vienna Center for Quantum Science and Technology (VCQ)（维也纳大学物理学院，维也纳量子科学与技术中心）；Center for Nanophotonics, NWO Institute AMOLF（纳米光子学中心，NWO AMOLF研究所）；Department of Physics, Dokuz Eylül University（德古兹埃勒大学物理系）；Centro de Física de Materiales CSIC-UPV/EHU and Materials Physics Center（CSIC-巴斯克国立大学物质物理学中心和材料物理中心）
Nonlinear optical phenomena in nanostructured materials have been challenging our perceptions of nonlinear optical processes that have been explored since the invention of lasers. For example, the ability to control optical field confinement, enhancement, and scattering almost independently, allows nonlinear frequency conversion efficiencies to be enhanced by many orders of magnitude compared to bulk materials. Also, the subwavelength length scale renders phase matching issues irrelevant. Compared with plasmonic nanostructures, dielectric resonator metamaterials show great promise for enhanced…
Dielectric metasurfaces have shown prominent applications in nonlinear optics due to strong field enhancement and low dissipation losses at the nanoscale. Chalcogenide glasses are one of the promising materials for the observation of nonlinear effects due to their high intrinsic nonlinearities. Here, we demonstrate, experimentally and theoretically, that significant second harmonic generation can be obtained within amorphous chalcogenide based metasurfaces by relying on the coupling between lattice and particle resonances. We further show that the high quality factor resonance at the origin of…
