We experimentally demonstrate enhanced third-harmonic generation from indium tin oxide nanolayers at telecommunication wavelengths with an efficiency that is approximately 600 times larger than crystalline silicon (Si). The increased optical nonlinearity of the fabricated nanolayers is driven by their epsilon-near-zero response, which can be tailored on-demand in the near-infrared region. The present material platform is obtained without any specialized nanofabrication process and is fully compatible with the standard Si-planar technology. The proposed approach can lead to largely scalable and highly integrated optical nonlinearities in Si-integrated devices for information processing and optical sensing applications.

We perform a comparative study of second-harmonic generation (SHG) from indium tin oxide (ITO) and from titanium nitride (TiN) nanolayers excited in the near-infrared spectrum. Both materials are compatible with Si technology and are candidate platforms for integrated nonlinear optics. In this work, we fabricate ITO samples with an ε-near-zero (ENZ) condition, which can be continuously tailored in the 1150−1670 nm spectral range, and TiN samples with a metallic behavior in the same spectral range. For the ITO nanolayers, we observe tunability and enhancement of the SHG intensity when the samples are excited at their respective ENZ condition, in agreement with the electromagnetic modeling and analogous to its third-harmonic generation studied earlier. On the other hand, we show that the SHG efficiency of TiN nanolayers is lower by a factor of 50. We determine experimentally that the dominant component of the second-order susceptibility for our best ITO nanolayer is χ zzz (2ω) = 0.18 pm V −1 , and we theoretically predict that the SHG process is enhanced up to 4 orders of magnitude when resonantly pumping the nanolayer at the ENZ wavelength with respect to a wavelength at 2000 nm. Remarkably, the resulting SHG efficiency is comparable with a crystalline quartz plate with thickness 0.5 mm used as a reference in our experiments in reflection configuration. Our study clearly indicates that ITO nanolayers with engineered ENZ conditions are a promising material platform for surface nonlinearities, with possible applications to nonlinear metasurfaces, Si-based flat optics, and sensing.

No abstract

The all-inorganic perovskite nanocrystals are currently in the research spotlight owing to their physical stability and superior optical properties—these features make them interesting for optoelectronic and photovoltaic applications. Here, we report on the observation of highly efficient carrier multiplication in colloidal CsPbI3 nanocrystals prepared by a hot-injection method. The carrier multiplication process counteracts thermalization of hot carriers and as such provides the potential to increase the conversion efficiency of solar cells. We demonstrate that carrier multiplication commences at the threshold excitation energy near the energy conservation limit of twice the band gap, and has step-like characteristics with an extremely high quantum yield of up to 98%. Using ultrahigh temporal resolution, we show that carrier multiplication induces a longer build-up of the free carrier concentration, thus providing important insights into the physical mechanism responsible for this phenomenon. The evidence is obtained using three independent experimental approaches, and is conclusive.

In the present Letter, we demonstrate how the design of metallic nanoparticle arrays with large electric field enhancement can be performed using the basic paradigm of engineering, namely the optimization of a well-defined objective function. Such optimization is carried out by coupling a genetic algorithm with the analytical multiparticle Mie theory. General design criteria for best enhancement of electric fields are obtained, unveiling the fundamental interplay between the near-field plasmonic and radiative photonic coupling. Our optimization approach is experimentally validated by surface-enhanced Raman scattering measurements, which demonstrate how genetically optimized arrays, fabricated using electron beam lithography, lead to order of ten improvement of Raman enhancement over nanoparticle dimer antennas, and order of one hundred improvement over optimal nanoparticle gratings. A rigorous design of nanoparticle arrays with optimal field enhancement is essential to the engineering of numerous nanoscale optical devices such as plasmon-enhanced biosensors, photodetectors, light sources and more efficient nonlinear optical elements for on chip integration.

We propose a numerical method, based on surface integral equations (SIE), for evaluating the second harmonic (SH) scattering by metal nanoparticles (NPs) of arbitrary shape, considering both nonlocal-bulk and local-surface SH sources, induced by the electromagnetic field at the fundamental frequency. We demonstrate that the contribution of the nonlocal-bulk sources can be taken into account through equivalent surface electric and magnetic currents. We numerically solve the SIE problem by using the Galerkin method and the Rao-Wilton-Glisson basis functions in the framework of the distribution theory. The accuracy of the proposed method is verified by comparing with the SH-Mie analytical solution. As an example of a complex-shaped particle, we investigate the SH scattering by a triangular nanoprism. This method paves the way for a better understanding of the SH generation process in arbitrarily shaped NPs and can also have a high impact on the design of novel nanoplasmonic devices with enhanced SH emission

We present a full-wave analytical solution for the problem of second-harmonic generation from spherical nanoparticles. The sources of the second-harmonic radiation are represented through an effective nonlinear polarization. The solution is derived in the framework of the Mie theory by expanding the pump field, the nonlinear sources, and the second-harmonic fields in series of spherical vector wave functions. We use the proposed solution for studying the second-harmonic radiation generated from gold nanospheres as a function of the pump wavelength and the particle size, in the framework of the Rudnick–Stern model. We demonstrate the importance of high-order multipolar contributions to the second-harmonic radiated power. Moreover, we investigate the dependence of the p- and s-components of the second-harmonic radiation on the Rudnick–Stern parameters. This approach provides a rigorous methodology to understand second-order optical processes in nanostructured metals and to design novel nanoplasmonic devices in the nonlinear regime

We demonstrate optical Second Harmonic Generation (SHG) in planar arrays of cylindrical Au nanoparticles arranged in periodic and deterministic aperiodic geometries. In order to understand the respective roles of near-field plasmonic coupling and long-range photonic interactions on the SHG signal, we systematically vary the interparticle separation from 60 nm to distances comparable to the incident pump wavelength. Using polarization-resolved measurements under femtosecond pumping, we demonstrate multipolar SHG signal largely tunable by the array geometry. Moreover, we show that the SHG signal intensity is maximized by arranging Au nanoparticles in aperiodic spiral arrays. The possibility to engineer multipolar SHG in planar arrays of metallic nanoparticles paves the way to the development of novel optical elements for nanophotonics, such as nonlinear optical sensors, compact frequency converters, optical mixers, and broadband harmonic generators on a chip.