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© 2023 Optica Publishing Group. Users may use, reuse, and build upon the article, or use the article for text or data mining, so long as such uses are for non-commercial purposes and appropriate attribution is maintained. All other rights are reserved. Nonlinear silicon photonics offers unique abilities to generate, manipulate and detect optical signals in nano-devices, with applications based on field localization and large third order nonlinearity. However, at the nanoscale, inefficient nonlinear processes, absorption, and the lack of realistic models limit the nano-engineering of silicon. Here we report measurements of second and third harmonic generation from undoped silicon membranes. Using experimental results and simulations we identify the effective mass of valence electrons, which determines second harmonic generation efficiency, and oscillator parameters that control third order processes. We can then accurately predict the nonlinear optical properties of complex structures, without introducing and artificially separating the effective ¿(2) into surface and volume contributions, and by simultaneously including effects of linear and nonlinear dispersions. Our results suggest that judicious exploitation of the nonlinear dispersion of ordinary semiconductors can provide reasonable nonlinear efficiencies and transformational device physics well into the UV range. The authors thank Zack Coppens and Dana Dement for useful discussions and help with the sample. LRS, JT, and CC acknowledge to US Army Research Laboratory Cooperative Agreement N° W911NF1920279 issued by US ARMY ACC-APG-RTP and Spanish Agencia Estatal de Investigación (project no. PID2019-105089GBI00/AEI/10.130397501100011033). MAV was partially sponsored by the Army Research Laboratory under Cooperative Agreement N° W911NF2020078.

The predominant methods currently used to determine nonlinear optical constants like the nonlinear refractive index n2 or the third order susceptibility χ(3) rely mostly on experimental, open and closed z-scan techniques and beam deflection methods. While these methods work well when the linear absorption is relatively small or negligible, the retrieval process is more complicated for a strongly scattering, dispersive or absorbing medium. The study of optics at the nanoscale in the picosecond or femtosecond laser pulsed regimes demands the development of new theoretical tools, and diverse experimental approaches, to extract and verify both linear and nonlinear optical dispersions exhibited by matter, especially when material constituents are fashioned into nanostructures of arbitrary shape. We present a practical, combined experimental and theoretical approach based on the hydrodynamic model that uses experimental results of harmonic generation conversion efficiencies to retrieve complex, nonlinear dispersion curves, not necessarily only for third order processes. We provide examples for materials that are of special interest to nanophotonics, for example, silicon, gold, and indium tin oxide (ITO), which displays nonlocal effects and a zero-crossing of the real part of the dielectric constant. The results for silicon and gold compare well with analytical predictions of nonlinear dispersion based on the nonlinear oscillator model. Based on our assessment of third harmonic generation conversion efficiencies in silicon, we predict χω(3) and χ3ω(3) are of order 10−17 (m/V)2 in the visible and near IR ranges, with respective peaks of 10−14 (m/V)2 and 10−16 (m/V)2 in the UV range. Similarly, gold’s χω(3) and χ3ω(3) are of order 10−17–10−16 (m/V)2, and predict χω(3)∼10−17(m/V)2 and χ3ω(3)∼10−18(m/V)2 for ITO. These results clearly suggest that judicious exploitation of the nonlinear dispersion of ordinary semiconductors has the potential to transform device physics in spectral regions that extend well into the UV range.

Understanding how light interacts with matter at the nanoscale is pivotal if one is to properly engineer nano-antennas, filters and other devices whose geometrical features approach atomic size. We report experimental results on second and third harmonic generation from 20 nm- and 70 nm-thick gold layers, for TE- and TM-polarized incident light pulses. We discuss the relative roles that bound electrons and an intensity dependent free electron density (hot electrons) play in third harmonic generation. While planar structures are generally the simplest to fabricate, metal layers that are only a few nanometers thick and partially transparent are almost never studied. Yet, transmission offers an additional reference point to compare experimental measurements with theoretical models. Our experimental results are explained well within the context of the microscopic hydrodynamic model that we employ to simulate second and third harmonic conversion efficiencies. Using our experimental observations we estimate ∣ χ 1064 n m ( 3 ) ∣≈ 10 − 18 ( m/V ) 2 , triggered mostly by hot electrons.

The use of semiconductors, metals and conductive oxides in the process of fabrication of actual nano devices is at the front edge of nowadays technology, exploiting the properties of light propagation and localization at nanometric scale in new and surprising ways. At these scales the usual theory describing the nonlinear (NL) effects of electromagnetic fields should be revisited and analyzed. We report a collection of experimental results of nonlinear harmonic generation in different nanolayers: semiconductors, conductive oxides and metals. The comparison of these experimental results with numerical predictions of our theoretical model identifies, distinguishes and explains the different nonlinear contributions to the harmonics generated by these materials at nanoscale. Our model accounts for surface, magnetic and bulk nonlinearities arising from free and bound charges, preserving linear and nonlinear dispersion, nonlocal effects due to pressure and viscosity.

We present an experimental study of second harmonic generation from a 20nm-thick indium tin oxide layer in the proximity of its epsilon-near-zero condition. We report measurements of second harmonic efficiencies as a function of the input wavelength and angle of incidence close to the epsilon-near-zero crossing point. We perform theoretical simulations using a hydrodynamical model that is able to capture all major physical mechanisms driving the nonlinear electrodynamic behaviour of conductive oxides. The experimental and theoretical results are compared and a very good quantitative and qualitative agreement is found.

We report a comparative experimental and theoretical study of second harmonic generation from a 20nm-thick indium tin oxide nanolayer in the proximity of the epsilon-near-zero condition. We record the efficiency of the second harmonic signal both as a function of wavelength as well as of the angle of incidence around the epsilon-near-zero crossing point. We compare our experimental results with numerical simulations based on a hydrodynamical model able to capture all major physical mechanisms driving the electrodynamic behavior of conductive oxide layers, with unique aspects of the different nonlinear sources. We found a very good quantitative and qualitative agreement between experiment and theory.

The use of semiconductors, metals, or ordinary dielectrics in the process of fabrication of nanodevices is at the front edge of nowadays technology, exploiting the properties of light propagation and localization at nanometric scale in new and surprising ways. Understanding accurately how light interacts with these materials at the nanoscale is crucial if one is to properly engineer nano-devices. When the nanoscale is reached, light-matter interactions display new phenomena where conventional approximations may not always be applicable and they should be either revised or voided. In this work, we measure the efficiency of second and third harmonic generation from gold nanolayers. The experimental results are compared with numerical simulations based on a detailed microscopic hydrodynamic model that considers different effects playing a role in the nonlinear response, not usually considered by more generic models. The agreement between experimental and theoretical results proves the importance of all these contributions.

We explore the outcomes of detailed microscopic models by calculating second- and third-harmonic generation from thin film surfaces with discontinuous free-electron densities. These circumstances can occur in structures consisting of a simple metal mirror, or arrangements composed of either different metals or a metal and a free electron system like a conducting oxide. Using a hydrodynamic approach we highlight the case of a gold mirror, and that of a two-layer system containing indium tin oxide (ITO) and gold. We assume the gold mirror surface is characterized by a free-electron cloud of varying density that spills into the vacuum, which as a result of material dispersion exhibits epsilon-near-zero conditions and local field enhancement at the surface. For a bylayer consisting of a thin ITO and gold films, if the wave is incident from the ITO side the electromagnetic field is presented with a free-electron discontinuity at the ITO/gold interface, and wavelength-dependent, epsilon-near-zero conditions that enhance local fields and conversion efficiencies, and determine the surface's emission properties. We evaluate the relative significance of additional nonlinear sources that arise when a free-electron discontinuity is present, and show that harmonic generation can be sensitive to the density of the screening free-electron cloud, and not its thickness. Our findings also suggest the possibility to control surface harmonic generation through surface charge engineering., Comment: 19 pages, 6 figures, 49 references

We study inhibition of absorption, transparency, energy and momentum transport of the inhomogeneous component of harmonic pulses in dielectrics and semiconductors, at visible and UV wavelengths, focusing on materials like GaP. In these spectral regions GaP is characterized by large absorption, metallic behavior or a combination of both. We show that phase locking causes the generated inhomogeneous signals to propagate through a bulk metallic medium without being absorbed, that is occurs even in centrosymmetric materials via the magnetic Lorentz force, and that the transport of energy and momentum is quite peculiar and seemingly anomalous. These results make it clear that there are new opportunities in ultrafast nonlinear optics and nano-plasmonics in new wavelength ranges., 16 pages, 5 figures, 1 video

We theoretically investigate second harmonic generation that originates from the nonlinear, magnetic Lorentz force term from single and multiple apertures carved on thick, opaque metal substrates. The linear transmission properties of apertures on metal substrates have been previously studied in the context of the extraordinary transmission of light. The transmission process is driven by a number of physical mechanisms, whose characteristics and relative importance depend on the thickness of the metallic substrate, slit size, and slit separation. In this work we show that a combination of cavity effects and surface plasmon generation gives rise to enhanced second harmonic generation in the regime of extraordinary transmittance of the pump field. We have studied both forward and backward second harmonic generation conversion efficiencies as functions of the geometrical parameters, and how they relate to pump transmission efficiency. The resonance phenomenon is evident in the generated second harmonic signal, as conversion efficiency depends on the duration of incident pump pulse, and hence its bandwidth. Our results show that the excitation of tightly confined modes as well as the combination of enhanced transmission and nonlinear processes can lead to several potential new applications such as photo-lithography, scanning microscopy, and high-density optical data storage devices., Keywords: Enhanced Transmission, Second Harmonic Generation, Surface Plasmon, Sub-wavelength Slit

We are designing and fabricating arrays of subwavelength SP structures in metal films and combining these structures with EO polymers to understand the interaction of the EO polymer with the enhanced electric fields of the plasmons. We have designed and modeled resonance structures to maximize extraordinary transmittance. We are making a systematic study of SP structure shapes by studying circular holes, elliptical holes and slits. Initially we have fabricated and begun optical evaluation of subwavelength slits in gold films. Slits with 32 nm width and 120 nm width have been fabricated by a focused ion beam system. Preliminary optical transmittance measurements in the visible and NIR are underway and will be compared to theoretical modeling.

International Quantum Electronics Conference 2004, San Francisco, California United States, 16–21 May 2004, We propose a device based on a one-dimensional photonic band gap structure that is optimized for the generation of coherent, THz radiation tunable up to 10 THz.

We proposed a coherent source based on parametric down-conversion in a photonic crystal. Our design is based on the band edge or defect-mode field enhancement phenomena near a photonic band gap. The numerical results show that a range of bandwidths, intensities, and frequencies up to 12 THz can be obtained.

In this paper we describe a way to achieve the extraordinary transmission regime from sub-wavelength slits carved on semiconductor substrates. Unlike metals, the dielectric permittivity of typical semiconductors like GaAs or GaP is negative beginning in the extreme UV range (lambda