Unpatterned Silicon Research Articles

Second harmonic generation and third harmonic enhancement in silicon by a composite metasurface and intense terahertz.

The compression and integration of nonlinear optical processes to the nanoscale are expected to have significant implications for quantum optics, biology, and medicine. In this work, a composite metasurface consisting of a hollow-bow-tie-shaped metal metasurface and a patterned amorphous silicon metasurface is proposed. An external terahertz (THz) electric field enhanced by the hollow-bow-tie structure is employed to break the centrosymmetry, which allows the generation of optical second harmonic. Meanwhile, the amorphous silicon nanocolumns inside the hollow-bow-tie-shaped structure enhance the optical laser field and improve the conversion efficiency of second and third harmonics. The numerical results indicate that at an incident optical laser intensity of 1.20 GW/cm2 and a y-component of the incident THz electric field of 10 kV/cm, the powers of the generated second and third harmonics are 3.96 × 10-6 W and 7.42 × 10-6 W, respectively, with conversion efficiencies of 3.93 × 10-7 and 7.18 × 10-7. The conversion efficiency of the third harmonic is increased by a factor of 700 compared to that of unpatterned silicon. The configuration proposed in this paper offers a solution for applications that need to take into account both high nonlinear efficiency and ultra-fast tunability.

Si metasurface supporting multiple quasi-BICs for degenerate four-wave mixing.

Dielectric metasurfaces supporting quasi-bound states in the continuum (qBICs) enable high field enhancement with narrow-linewidth resonances in the visible and near-infrared ranges. The resonance emerges when distorting the meta-atom's geometry away from a symmetry-protected BIC condition and, usually, a given design can sustain one or two of these states. In this work, we introduce a silicon-on-silica metasurface that simultaneously supports up to four qBIC resonances in the near-infrared region. This is achieved by combining multiple symmetry-breaking distortions on an elliptical cylinder array. By pumping two of these resonances, the nonlinear process of degenerate four-wave mixing is experimentally realized. By comparing the nonlinear response with that of an unpatterned silicon film, the near-field enhancement inside the nanostructured dielectric is revealed. The presented results demonstrate independent geometric control of multiple qBICs and their interaction through wave mixing processes, opening new research pathways in nanophotonics, with potential applications in information multiplexing, multi-wavelength sensing and nonlinear imaging.

A multi-mode super-fano mechanism for enhanced third harmonic generation in silicon metasurfaces

We present strong enhancement of third harmonic generation in an amorphous silicon metasurface consisting of elliptical nano resonators. We show that this enhancement originates from a new type of multi-mode Fano mechanism. These ‘Super-Fano’ resonances are investigated numerically in great detail using full-wave simulations. The theoretically predicted behavior of the metasurface is experimentally verified by linear and nonlinear transmission spectroscopy. Moreover, quantitative nonlinear measurements are performed, in which an absolute conversion efficiency as high as ηmax ≈ 2.8 × 10−7 a peak power intensity of 1.2 GW cm−2 is found. Compared to an unpatterned silicon film of the same thickness amplification factors of up to ~900 are demonstrated. Our results pave the way to exploiting a strong Fano-type multi-mode coupling in metasurfaces for high THG in potential applications.

Spatiotemporal Mapping of Hole Nucleation and Growth during Block Copolymer Terracing with High-Speed Atomic Force Microscopy.

As a platform for investigating two-dimensional phase separation, we track the structural evolution of block copolymer thin films during thermal annealing with environmentally controlled atomic force microscopy (AFM). Upon thermal annealing, block copolymer films with incommensurate thickness separate into a terraced morphology decorated with holes. With in situ imaging at 200 °C, we follow the continuous progression of terrace formation in a single region of a cylinder-forming poly(styrene-block-methyl methacrylate) thin film, beginning with the disordered morphology on an unpatterned silicon substrate and continuing through nucleation and coarsening stages. Topographic AFM imaging with nanoscale resolution simultaneously captures ensemble hole growth statistics while locally tracking polymer diffusion through measurements of the film thickness. At early times, we observe homogeneous hole nucleation and isotropic growth, with kinetics following the predictions of classical nucleation theory. At later times, however, we find anomalous hole growth which arises due to the combination of Ostwald ripening and coalescence mechanisms. In each case, our real-space observations highlight the importance of hole interactions for determining coarsening kinetics, mediated either through the interconnected phase for Ostwald ripening or through binary collision events for coalescence.

Hierarchical Self-Assembly and Chemical Imaging of Nanoscale Domains in Polymer Blend Thin Films

Self-assembly of polymers driven by intermolecular and intramolecular interactions leads to rich structural variations in thin films of polymer blends. In this work, ordering of poly(3-hexylthiophene-2,5-diyl) (P3HT) to form nanoparticles (NPs) and the self-assembly pattern of the NPs in poly(4-vinylpyridine) (P4VP) matrix are revealed by using scattering-type scanning near-field optical microscopy (s-SNOM). The P3HT NPs are formed spontaneously when the P3HT/P4VP/chloroform solution is spin-cast on unpatterned silicon wafer at room temperature. We find that the P3HT NPs organize within the P4VP matrix forming continuous stripes along the parallel striations, depending on the solution composition and spin-coating angular speed. The spacing between the parallel P3HT stripes that runs along the center of the ridges varies from sample to sample within 4–12 μm, whereas the width of the P3HT stripes confined within the ridges ranges from 0.2 to 1.1 μm as determined from the s-SNOM infrared phase contrast. The sizes of the P3HT NPs range from 5 to over 100 nm depending on the composition of the blend as determined by using an atomic force microscope after selectively dissolving the P4VP matrix. The smallest size observed in our experiment is significantly smaller than the smallest diameter (larger than 20 nm) reported in the literature. The results presented here show that interaction between immiscible polymers during solvent evaporation can be manipulated to control hierarchical self-assembly from molecular ordering to mesoscale dimensions, and high-resolution chemical imaging is necessary to resolve nanoscale domains so that solution processes can be optimized.

Nanoscale mapping of optically inaccessible bound-states-in-the-continuum

Bound-states-in-the-continuum (BIC) is an emerging concept in nanophotonics with potential impact in applications, such as hyperspectral imaging, mirror-less lasing, and nonlinear harmonic generation. As true BIC modes are non-radiative, they cannot be excited by using propagating light to investigate their optical characteristics. In this paper, for the 1st time, we map out the strong near-field localization of the true BIC resonance on arrays of silicon nanoantennas, via electron energy loss spectroscopy with a sub-1-nm electron beam. By systematically breaking the designed antenna symmetry, emissive quasi-BIC resonances become visible. This gives a unique experimental tool to determine the coherent interaction length, which we show to require at least six neighboring antenna elements. More importantly, we demonstrate that quasi-BIC resonances are able to enhance localized light emission via the Purcell effect by at least 60 times, as compared to unpatterned silicon. This work is expected to enable practical applications of designed, ultra-compact BIC antennas such as for the controlled, localized excitation of quantum emitters.

Nanosecond mid-infrared pulse generation via modulated thermal emissivity

We demonstrate the generation of nanosecond mid-infrared pulses via fast modulation of thermal emissivity enabled by the absorption of visible pump pulses in unpatterned silicon and gallium arsenide. The free-carrier dynamics in these materials result in nanosecond-scale modulation of thermal emissivity, which leads to nanosecond pulsed thermal emission. To our knowledge, the nanosecond thermal-emissivity modulation in this work is three orders of magnitude faster than what has been previously demonstrated. We also indirectly observed subnanosecond thermal pulses from hot carriers in semiconductors. The experiments are well described by our multiphysics model. Our method of converting visible pulses into the mid infrared using modulated emissivity obeys different scaling laws and can have significant wavelength tunability compared to approaches based on conventional nonlinearities.

Enhanced Four-Wave Mixing in Doubly Resonant Si Nanoresonators

Frequency conversion is one of the main applications of nonlinear optical processes in which a signal is produced at a different wavelength from the excitation wavelength. In particular, four-wave mixing (FWM) is a third order nonlinear optical process that allows, for instance, the generation of visible frequencies by tuning near-infrared laser pumps. Here, in order to augment the very weak FWM conversion efficiency, we design silicon Mie resonators that exhibit two resonances of the internal electric field intensity around the frequency range of the laser pumps. The linear extinction spectrum of the individual Si resonator is first measured by bright field spectroscopy and compared with numerical simulations to confirm the existence of the two resonances corresponding to electric and magnetic dipole excitations. The FWM signal is then measured for a single Si nanoresonator when the first pump is set to the electric resonance while tuning the frequency of the second pump across the magnetic dipolar resonance. We show that the FWM signal generated in the visible spectrum is maximum when the frequency of the tunable pump corresponds to the maximum of the internal electric field intensity. At this position, the FWM signal is enhanced by more than 2 orders of magnitude compared with the FWM signal generated by the unpatterned silicon film.

Fano-resonant silicon photonic crystal slab for efficient third-harmonic generation.

Strong light-matter interactions in resonant photonic nanostructures open up opportunities for enhancing nonlinear responses. In this work, by applying Fano resonances, we experimentally demonstrate efficient third-harmonic generation (THG) obtained with 2D silicon photonic crystal slabs (PCSs) thanks to the field enhancement in the dielectric layer. A 160-fold enhancement of THG is observed in the silicon PCS compared to the unpatterned silicon film. Through slightly changing the radius of the PCS, tunable THG on a single chip is obtained, paving a way for the optical manipulation of harmonic generation.

Nonradiating Silicon Nanoantenna Metasurfaces as Narrowband Absorbers

High-refractive-index (HRI) nanostructures support optically induced electric dipole (ED) and magnetic dipole (MD) modes that can be used to control scattering and achieve narrowband absorption. In this work, a high-absorptance device is proposed and realized by using amorphous silicon nanoantenna (a-Si NA) arrays that suppress backward and forward scattering with engineered structures and in particular periods. The overlap of ED and MD resonances, by designing an array with a specific period and exciting lattice resonances, is experimentally demonstrated. The absorptance of a-Si NA arrays increases 3-fold in the near-infrared range in comparison to unpatterned silicon films. Nonradiating a-Si NA arrays can achieve high absorptance with a small resonance bandwidth (Q = 11.89) at a wavelength of 785 nm. The effect is observed not only due to the intrinsic loss of material but by overlapping the ED and MD resonances.

1.3-μm InAs quantum-dot micro-disk lasers on V-groove patterned and unpatterned (001) silicon.

We report comparison of lasing dynamics in InAs quantum dot (QD) micro-disk lasers (MDLs) monolithically grown on V-groove patterned and planar Si (001) substrates. TEM characterizations reveal abrupt interfaces and reduced threading dislocations in the QD active regions when using the GaAs-on-V-grooved-Si template. The improved crystalline quality translates into lower threshold power in the optically pumped continuous-wave MDLs. Concurrent evaluations were also made with devices fabricated simultaneously on lattice-matched GaAs substrates. Lasing behaviors from 10 K up to room temperature have been studied systematically. The analyses spotlight insights into the optimal epitaxial scheme to achieve low-threshold lasing in telecommunication wavelengths on exact Si (001) substrates.

Nonlinear Fano-Resonant Dielectric Metasurfaces.

Strong nonlinear light-matter interaction is highly sought-after for a variety of applications including lasing and all-optical light modulation. Recently, resonant plasmonic structures have been considered promising candidates for enhancing nonlinear optical processes due to their ability to greatly enhance the optical near-field; however, their small mode volumes prevent the inherently large nonlinear susceptibility of the metal from being efficiently exploited. Here, we present an alternative approach that utilizes a Fano-resonant silicon metasurface. The metasurface results in strong near-field enhancement within the volume of the silicon resonator while minimizing two photon absorption. We measure a third harmonic generation enhancement factor of 1.5 × 10(5) with respect to an unpatterned silicon film and an absolute conversion efficiency of 1.2 × 10(-6) with a peak pump intensity of 3.2 GW cm(-2). The enhanced nonlinearity, combined with a sharp linear transmittance spectrum, results in transmission modulation with a modulation depth of 36%. The modulation mechanism is studied by pump-probe experiments.

Photonic surfaces for designable nonlinear power shaping

We propose a method for designing nonlinear input-output power response based on absorptive resonances of nanostructured surfaces. We show that various power transmission trends can be obtained by placing a photonic resonance mode at the appropriate detuning from the laser wavelength. We demonstrate our results in a silicon photonic crystal slab at a laser wavelength of 808 nm. We quantify the overall spectral red shift as a function of laser power. The shift results from absorptive heating and the thermo-optic effect. We then demonstrate devices with increasing, decreasing, and non-monotonic transmission as a function of laser power. The transmission changes are up to 7.5 times larger than in unpatterned silicon. The strong nonlinear transmission is due to a combination of resonantly enhanced absorption, reduced thermal conductivity, and the resonant transmission lineshape. Our results illustrate the possibility of designing different nonlinear power trends within a single materials platform at a given wavelength of interest.

Seeing through a mask

seeing through a mask

The kinetics of dewetting ultra-thin Si layers from silicon dioxide

In this study, we investigate the kinetically driven dewetting of ultra-thin silicon films on silicon oxide substrate under ultra-high vacuum, at temperatures where oxide desorption and silicon lost could be ruled out. We show that in ultra-clean experimental conditions, the three different regimes of dewetting, namely (i) nucleation of holes, (ii) film retraction and (iii) coalescence of holes, can be quantitatively measured as a function of temperature, time and thickness. For a nominal flat clean sample these three regimes co-exist during the film retraction until complete dewetting. To discriminate their roles in the kinetics of dewetting, we have compared the dewetting evolution of flat unpatterned crystalline silicon layers (homogeneous dewetting), patterned crystalline silicon layers (heterogeneous dewetting) and amorphous silicon layers (crystallization-induced dewetting). The first regime (nucleation) is described by a breaking time which follows an exponential evolution with temperature with an activation energy EH ∼ 3.2 eV. The second regime (retraction) is controlled by surface diffusion of matter from the edges of the holes. It involves a very fast redistribution of matter onto the flat Si layer, which prevents the formation of a rim on the edges of the holes during both heterogeneous and homogeneous dewetting. The time evolution of the linear dewetting front measured during heterogeneous dewetting follows a characteristic power law x ∼ t0.45 consistent with a surface diffusion-limited mechanism. It also evolves as x ∼ h−1 as expected from mass conservation in the absence of thickened rim. When the surface energy is isotropic (during dewetting of amorphous Si) the dynamics of dewetting is considerably modified: firstly, there is no measurable breaking time; secondly, the speed of dewetting is two orders of magnitude larger than for crystalline Si; and thirdly, the activation energy of dewetting is much smaller due to the different driving force, which is based on the crystallization and redistribution of matter around the crystalline nuclei. The third regime (coalescence) corresponds to the merging of the dewetted fronts and of the islands positioned along the edges of the holes. The dynamics of this regime is much slower since it requires overcoming an additional nucleation barrier, while the surface energy reduction is quite low (low decrease of the covered surface area).

Nanomembrane transfer process for intricate photonic device applications

We demonstrate a process for the fabrication and transfer of silicon nanomembranes (Si-NMs) that have been released from their host substrates and redeposited on foreign flexible or flat substrates. The transfer process developed allows intricate photonic devices to be transferred via NMs to a variety of new substrate materials. This allows the transferred devices to benefit from the material properties of both substrate and NM. Our process is designed to transfer and stack large-area photonic devices without compromising their optical performance. The process has been used to transfer large-area unpatterned silicon NMs, in excess of 2.5 cm(2), and photonic devices with intricate device designs containing various fill factors. We have also demonstrated transferred photonic crystal devices that have maintained structural integrity and functionality.

Transfer of micro and nano-photonic silicon nanomembrane waveguide devices on flexible substrates

This paper demonstrates transfer of optical devices without extra un-patterned silicon onto low-cost, flexible plastic substrates using single-crystal silicon nanomembranes. Employing this transfer technique, stacking two layers of silicon nanomembranes with photonic crystal waveguide in the first layer and multi mode interference couplers in the second layer is shown, respectively. This technique is promising to realize high density integration of multilayer hybrid structures on flexible substrates.

On the origin of dissimilar pore evolution on patterned and unpatterned (100) n-type silicon

Via systematic investigation of the anodization of both patterned and unpatterned specimens, phenomena of pronounced discrepancy with respect to pore size, pore density and pore etch-rate were evidenced. Based on the detailed analysis of scanning electron microscope (SEM) micrographs and current-voltage curves, the competition between physical and chemical elements was found to be crucial to understanding the observations. The results indicate that the size, density and growth-speed of pores may act as an evident function of the initial morphology of the sample surface, despite a nearly fixed width of the space charge region. Electric-field effect as well as current-burst-model (CBM) was employed to interpret the underlying mechanism.

Particle Removal Efficiency and Damage Analysis on Silicon Wafers after Megasonic Cleaning in Solvents

The increasing complexity of semiconductor devices imposes challenging requirements on particle contamination and surface damage. To meet these requirements novel surface-cleaning processes are evaluated, which combine physical energy with organic solvents. In this work, the performance of megasonic cleaning with deionized water (DIW) and N-methylpyrrolidone (NMP) was evaluated in terms of particle removal efficiency (PRE) and damage analysis. The goal was to define an optimum process window where the PRE was maximum and the damage was minimum. Particle removal and damage analysis were performed on unpatterned silicon wafers and with patterned polysilicon lines, respectively, under identical sonic power and process parameters. A comparison between these two solvents reveals that at low sonic power the particle-cleaning performances in DIW and NMP are similar. At high sonic power, in both solvents a detailed analysis of the PRE and damage indicates a non-homogeneous trend over the surface of the wafer. More particularly, in DIW higher PRE and damage are noticed towards the edge of the wafer. In NMP, the opposite trend was observed. However, an equivalent performance was obtained at a lower sonic power in case of NMP compared to DIW. Further understanding of megasonic cleaning in solvents, and an optimization of the process parameters are the key to improve the performance of megasonic cleaning in organic solvents like NMP.

Selective formation of silicon nanowires on pre-patterned substrates

In this paper, the selective growth of silicon nanowires (SiNWs) was studied. With the aid of photolithography, the vertically aligned silicon nanowires were selectively formed on the patterned substrates via an electroless metal deposition (EMD) method under normal conditions (room temperature, 1atm). Low-pressure chemical vapor deposition (LPCVD) silicon nitride was used as the masking layer for SiNWs preparation. The scanning electron microscope was used to examine the etching results. Both the patterned and the unpatterned silicon substrates were used for study. The results indicated that the growth rates of the SiNWs upon the patterned and the unpatterned substrates are different. For the patterned substrates, the growth rate of SiNWs is dependent upon the pattern shape. The influence of length-to-width ratio for the rectangular-shaped patterns was studied. It is concluded that by designing the proper length-to-width ratio, the nanowires with different lengths can be fabricated simultaneously on the same substrate.