The field of nonlinear optics (NLO) has been continuously growing over the past decades, and several NLO data tables were published before the turn of the century. After the year 2000, there have been major advances in materials science and technology beneficial for NLO research, but a data table providing an overview of the post-2000 developments in NLO has so far been lacking. Here, we introduce a new set of NLO data tables listing a representative collection of experimental works published since 2000 for bulk materials, solvents, 0D-1D-2D materials, metamaterials, fiber waveguiding materials, on-chip waveguiding materials, hybrid waveguiding systems, and THz NLO materials. In addition, we provide a list of best practices for characterizing NLO materials. The presented data tables and best practices form the foundation for a more adequate comparison, interpretation, and practical use of already published NLO parameters and those that will be published in the future.
The field of Nonlinear Optics (NLO), launched about 60 years ago, has gained considerable momentum over the past two decades, resulting in an enormous growth in NLO publications for a wide range of material categories, including bulk materials, 0D-1D-2D materials, metamaterials, fiber waveguiding materials, on-chip waveguiding materials, and hybrid waveguiding systems. However, a convenient summary of NLO data collected since 2000 for these different material types has been lacking and would be a valuable resource for researchers in the field. Here, we present a new set of data tables showcasing a representative list of NLO properties taken from the literature since 2000 on the above-mentioned material categories. Furthermore, we provide best practices for performing and reporting NLO experiments. These best practices underpin the selection process that we used for including papers in the tables, and also form the foundation for a more adequate comparison, interpretation, and use of the NLO parameters published today and those that will be published in the future.
Nonlinear optical effects in epsilon-near-zero materials have become an area of significant interest to the community within the last 10 years. From demonstrations of refractive index tuning, enhanced harmonic generation, and time varying interactions, a wide range of effects and nonlinear properties have been shown to be influenced by the epsilon-near-zero condition. In this talk, we will a higher level look at refractive index tuning in epsilon-near-zero materials (predominately free-carrier-based materials), highlighting why the epsilon-near-zero conditions provides increased index tuning as well as what features are intrinsic to the epsilon-near-zero condition and what features are dictated by external effects. Breaking down the interaction is intended to highlight what properties are difficult to control and what properties can be readily tuned to maximize effects. This is intended to highlight trade-offs in performance and implementation and facilitate discussion related to selecting the best materials, excitation conditions, and designs as epsilon-near-zero materials attempt to transition from laboratory curiosities to potential applications.
Epsilon-near-zero materials are a rapidly expanding field due to their enhanced light matter interaction. These materials have shown large changes in refractive index on the order of the linear index; however, this is associated with large absorption changes. Here we experimentally and theoretically show a method to mitigate the absorption changes in the film while doubling the refractive index modulation. Using beam deflection, a nonlinear technique to measure χ^((3)), individual excitation processes can be controlled in time and space on a film so the nonlinear refractive index change can double on a sample, while the absorption change can be nullified.
Chalcogenide phase change materials (PCMs) are uniquely suited for spectral tuning applications due to their contrasting dielectric material properties. Recent headway has been made towards realizing tunable photonic devices using twodimensional, sub-wavelength resonators by carefully designing geometries that optimize optical, electrical, and thermal performances using multi-physics analyses and machine learning. In this paper, we tackle two other essential aspects for creating application-specific, tunable PCM devices: (1) scalability of the device size and (2) high-throughput fabrication techniques. We employ a deep ultraviolet (DUV) stepper projection lithography to manufacture over 100 densely packed GST metasurfaces, each with a sample size of 5×7 mm2, all on a 4-inch Al2O3 wafer. These metasurface structures were discovered using artificial neural network (ANN) techniques and confirmed by finite-difference-time domain calculations. The primary structures under investigation were nanobar configurations enabling amplitude modulation at short-wave infrared wavelengths to realize efficient optical switches for free space optical multiplexing. The DUV fabrication technique can easily be extended to other metasurface geometries to demonstrate multi-functional, non-volatile photonic devices.
Recently, transparent conducting oxides such as indium tin oxide and aluminum-doped zinc oxide have been characterized in their epsilon-near-zero crossover regions due to their strong enhancement of light-matter interaction. A newer technique, known as beam deflection, can be used to enable single-detector measurements that characterizes the complex nonlinear refractive index by detecting the angular deflection and transmission of a probe beam. Here we describe two key nonidealities in beam deflection measurements, 1) the spatio-temporal interaction of the beams with a finite relative angular separation, 2) the apparent angular deviation occurring due to strong spatially non-uniform absorption.
Epsilon-near-zero (ENZ) materials have been key players in recent photonic applications due to their versatility in growth, excellent compatibility, and ability to be dynamically modulated. From a foundation in the recently developed carrier kinetic models of nonlinearities in ENZ materials, we discuss our efforts to realize scalable and high-quality Al:ZnO (AZO) films via a unique atomic layer deposition (ALD) process, and the use of AZO in both switching and frequency shifting applications. Throughout, we highlight the advantages and challenges that exist and conclude with an outlook for ENZ materials in the area of nonlinear optics.
Since the invention of the laser, nonlinear optical phenomena have been a cornerstone of photonics research empowering advances in both continuous and pulsed lasers, molecular spectroscopy, and sub-diffraction imaging others. Although many nonlinear media have been explored through the years, ever more compact and efficient platforms remain a key driver in the field. Recently epsilon-near-zero (ENZ) materials, media with a spectral range where|Re{ε}| < 1, have emerged as a compact and versatile approach to enhance various nonlinear processes such as refractive index tuning, harmonic generation, and phase conjugation. In this talk, we discuss the unique underlying conditions that make ENZ materials a promising nonlinear platform and employ a framework of carrier kinetics to describe the nonlinear effects in Drude-based ENZ materials such as the transparent conducting oxides (TCOs). Through this approach, we focus on the large and ultrafast reflection and transmission modulation in TCOs enabled by the intensity-dependent refractive index, highlighting general trends as well as optimal material and excitation conditions. In particular, the role of absorption and non-parabolicity of the energy bands are discussed, culminating in a general figure of merit for comparing the performance of new potential ENZ materials. Finally, we describe recent advances utilizing the ultrafast refractive index tuning to generate an adiabatic frequency shift of a probe beam’s spectrum.
Near-Zero-Index (NZI) media have recently received significant attention for enhanced nonlinear optical processes such as the intensity dependent refractive index (IDRI). For NZI materials in the infrared, this effect is generally described as a result of free-electron effects such as excess carrier and hot-electron generation. Yet, many works model the response through the Kerr effect, a bound-electron polarization process exhibiting an instantaneous response and polarization sensitivity that are not observed in NZI materials. The similar dispersions in absorption for NZI and resonant materials enables the Kerr index to be a reasonable approximation, but its origin limits the predictive ability of the model. For example, the non-degenerate Kerr model predicts a diverging n_2 as the material loss tends towards zero. However, this condition would eliminate the absorption of the pump resulting in a vanishing nonlinear interaction. To aid the description of nonlinearities in NZI media, we have developed carrier kinetic models for the IDRI rooted in free electron effects. From this, our model shows that for low loss films, the quality factor n_2/FWHM in fact increases with additional loss, largely due to an significant increase in n_2 which outpaces the increase in breadth. This suggests the difficult task to reduce the loss in NZI materials may not be necessary for applications where the maximum IDRI or modulation is desired. As a result, the carrier kinetic models can more accurately predict the behavior of materials, e.g. in response to varying loss, as well as optimize pumping conditions and couple multiple excitation schemes.
Titanium nitride is being studied as an alternative plasmonic material for its tunability and high durability. TiN can be grown with high quality and competitive optical properties, but the current magnetron sputtering method used to achieve this quality requires a high temperature. For low temperature or CMOS compatible design, Atomic Layer Deposition (ALD) is a promising method; ALD TiN films are conformal allowing ultrathin, few monolayer, thicknesses. However, TiN films deposited with ALD have struggled to reach the metallicity and quality of sputtered films. Here, we present a study on films produced via Plasma Enhanced Atomic Layer Deposition (PE-ALD) that approach the metallicity of sputtered films while remaining relatively low loss compared to similar films that are achieved with a CMOS compatible method.
Several TiN films on sapphire and silicon of comparable thicknesses (~70nm) and varied temperature, 375 to 475 C, are studied by spectroscopic ellipsometry and x-ray diffraction to characterize optical properties and film quality. Peak optical properties occurred at a deposition temperature at 375 C which we attribute to the precursor, tetrakis(dimethlamino) titanium(IV), gas breakdown temperature ~425 C (lower deposition temperatures currently being explored). This film exhibits a figure of merit (-Re{ε}/Im{ε}) of 2 compared to other ALD films of 1.2 and sputtered films as high as 3.6. XRD results show epitaxial quality films with lattice constants that approach bulk as temperature is increased. These conflicting trends suggest that transitioning to a different precursor may allow for an optical property improvement of materials at a higher temperature deposition.
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