We present a multipolar tensor analysis of second-harmonic generation from arrays of noncentrosymmetric gold nanoparticles. In contrast to earlier results, where higher multipoles and symmetry-forbidden signals arising from sample defects play a significant role, the present results are completely dominated by symmetry-allowed electric-dipole tensor components. The result arises from significant improvement in sample quality, which suppresses the higher-multipole effects and enhances the overall response by an order of magnitude. The results are a prerequisite for metamaterials with controllable nonlinear properties.
We present a comprehensive tensorial characterization of second-harmonic generation from silicon nitride films with varying compositions. The samples were fabricated using plasma-enhanced chemical vapor deposition, and the material composition was varied by the reactive gas mixture in the process. We found a six-fold enhancement between the lowest and highest second-order susceptibility, with the highest value of approximately 5 pm/V from the most silicon-rich sample. Moreover, the optical losses were found to be sufficiently small (below 6 dB/cm) for applications. The tensorial results show that all samples retain in-plane isotropy independent of the silicon content, highlighting the controllability of the fabrication process. High-performance complementary metal oxide semiconductor (CMOS) compatible materials are essential elements for advanced on-chip photonic devices to realize the future progress in all-optical processing. The ultra-fast speed and high bandwidth of integrated photonic networks continuously require new materials possessing excellent linear and nonlinear optical properties [1,2]. Although silicon (Si) is still the most commonly used CMOS material, the intrinsic drawbacks of Si, such as its narrow bandgap and centrosymmetric structure, highly limit its future applications especially in the visible and ultraviolet spectral regimes [2,3]. Thus, exploring novel CMOScompatible materials with wide bandgap and strong optical nonlinearities is very important for future integrated devices.Many photonic applications rely on nonlinear optical effects. One of the limitations of many nonlinear materials for CMOS-compatible platforms is the lack of second-order nonlinearity due to centrosymmetry. The problem can be overcome by poling [4,5], straining the material [3] or by using multilayer composites [6][7][8]. Unexpectedly, CMOS-compatible amorphous silicon nitride films (SiN) have been shown to possess a bulk second-order nonlinearity by measuring strong second-harmonic generation (SHG) from thin films [9][10][11]. Although the exact reason for this strong SHG response remains unclear, it is believed that the complicated composition, crystalline phase, and defects in the film during the deposition may be responsible [10,[12][13][14][15][16].In this Letter, we show that the strong second-harmonic signal from SiN films can be further enhanced by varying the composition of the films prepared with plasma-enhanced chemical vapor deposition (PECVD). Furthermore, we demonstrate that such composition tuning does not compromise the linear optical properties or optical losses of the material for applications. Our results are crucial for the comprehensive understanding of the linear and nonlinear optical properties in SiN films with different structures, opening the path for further optimization of SiN for on-chip devices.We recognize that there have been previous studies yielding different values for the SHG susceptibility of SiN [9,10,11,17,18]. Samples prepared by sputtering can yield very high values of the su...
We report the fabrication of artificial unidimensional crystals exhibiting an effective bulk second-order nonlinearity. The crystals are created by cycling atomic layer deposition of three dielectric materials such that the resulting metamaterial is noncentrosymmetric in the direction of the deposition. Characterization of the structures by second-harmonic generation Maker-fringe measurements shows that the main component of their nonlinear susceptibility tensor is about 5 pm/V, which is comparable to well-established materials and more than an order of magnitude greater than reported for a similar crystal [Appl. Phys. Lett.107, 121903 (2015)APPLAB0003-695110.1063/1.4931492]. Our demonstration opens new possibilities for second-order nonlinear effects on CMOS-compatible nanophotonic platforms.
We study second-harmonic generation from gold nanoislands covered with amorphous titanium oxide (TiO_{2}) films. As the TiO_{2} thickness increases, the plasmon resonance of the nanoislands shifts away from the second-harmonic wavelength of 532 nm, diminishing the resonant enhancement of the process at this wavelength. Nevertheless, the second-harmonic signal is enhanced by up to a factor of 45 with increasing TiO_{2} thickness. This unexpected effect arises from the scaling of local fields at the fundamental wavelength of 1064 nm-which is at the far tail of the resonance-due to a change in the dielectric environment of the nanoislands.
The determination of the second-order susceptibility (χ(2)) of thin film samples can be a delicate matter since well-established χ(2) measurement methodologies such as the Maker fringe technique are best suited for nonlinear materials with large thicknesses typically ranging from tens of microns to several millimeters. Here we compare two different second-harmonic generation setups and the corresponding measurement methodologies that are especially advantageous for thin film χ(2) characterization. This exercise allows for cross-checking the χ(2) obtained for identical samples and identifying the main sources of error for the respective techniques. The development of photonic integrated circuits makes nonlinear thin films of particular interest, since they can be processed into long waveguides to create efficient nonlinear devices. The investigated samples are ABC-type nanolaminates, which were reported recently by two different research groups. However, the subsequent analysis can be useful for all researchers active in the field of thin film χ(2) characterization.
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