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Broad Frequency Shift of Parametric Processes in Epsilon-Near-Zero Time-Varying Media

The ultrafast changes of material properties induced by short laser pulses can lead to a frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in spectral regions where the material features a near-zero real part of the permittivity. Here, we investigate the frequency shift for fields generated by four-wave mixing. In our experiment, we observed a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) in the phase conjugated radiation generated by a 500 nm aluminium-doped zinc oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

36 MATERIALS SCIENCE↗

Dynamical Control of Broadband Coherent Absorption in ENZ Films

Interferometric effects between two counter-propagating beams incident on an optical system can lead to a coherent modulation of the absorption of the total electromagnetic radiation with 100% efficiency even in deeply subwavelength structures. Coherent perfect absorption (CPA) rises from a resonant solution of the scattering matrix and often requires engineered optical properties. For instance, thin film CPA benefits from complex nanostructures with suitable resonance, albeit at a loss of operational bandwidth. In this work, we theoretically and experimentally demonstrate a broadband CPA based on light-with-light modulation in epsilon-near-zero (ENZ) subwavelength films. We show that unpatterned ENZ films with different thicknesses exhibit broadband CPA with a near-unity maximum value located at the ENZ wavelength. By using Kerr optical nonlinearities, we dynamically tune the visibility and peak wavelength of the total energy modulation. Our results based on homogeneous thick ENZ media open a route towards on-chip devices that require efficient light absorption and dynamical tunability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Large-Area, Highly Crystalline DNA-Assembled Metasurfaces Exhibiting Widely Tunable Epsilon-Near-Zero Behavior

Metasurfaces prepared via bottom-up nanoparticle assembly enable the deliberate manipulation of light in the optical regime, resulting in media with unprecedented optical responses. Here, we report a scalable method to grow highly crystalline 2D metasurfaces comprised of colloidal gold nanocubes, over macroscopic areas, using DNA-mediated assembly under equilibrium conditions. Using an effective medium description, we predict that these plasmonic metasurfaces behave as dielectric media with high refractive indices that can be dynamically tuned by tuning DNA length. Furthermore, we predict that when coupled with an underlying thin gold film, the real permittivity of these metasurfaces exhibits a crossover region between positive and negative values, known as the epsilon-near-zero (ENZ) condition, which can be tuned between 1.5 - 2.6 μm by changing DNA length. Optical characterization performed on the DNA-assembled metasurfaces reveals that the predicted optical properties agree well with measured response. Overall, we propose an efficient method for realizing large-area plasmonic metasurfaces that enable dynamic control over unique optical characteristics. High-index and ENZ metasurfaces operating in the telecommunications regime could have significant implications in high-speed optical computing, optical communications, optical imaging, and other areas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Giant enhancement of nonreciprocity in gyrotropic heterostructures

Abstract Nonreciprocity is a highly desirable feature in photonic media since it allows for control over the traveling electromagnetic waves, in a way that goes far beyond ordinary filtering. One of the most conventional ways to achieve nonreciprocity is via employing gyrotropic materials; however, their time-reversal-symmetry-breaking effects are very weak and, hence, large, bulky setups combined with very strong magnetic biases are required for technologically useful devices. In this work, artificial heterostructures are introduced to enhance the effective nonreciprocal behavior by reducing the contribution of the diagonal susceptibilities in the collective response; in this way, the off-diagonal ones, that are responsible for nonreciprocity, seem bigger. In particular, alternating gyrotropic and metallic or plasmonic films make an epsilon-near-zero (ENZ) effective-medium by averaging the diagonal permittivities of opposite sign, representing the consecutive layers. The homogenization process leaves unaltered the nonzero off-diagonal permittivities of the original gyrotropic substance, which become dominant and ignite strong nonreciprocal response. Realistic material examples that could be implemented experimentally in the mid-infrared spectrum are provided while the robustness of the enhanced nonreciprocity in the presence of actual media losses is discussed and bandwidth limitations due to the unavoidable frequency dispersion are elaborated. The proposed concept can be extensively utilized in designing optical devices that serve a wide range of applications from signal isolation and wave circulation to unidirectional propagation and asymmetric power amplification.

42 ENGINEERING↗

Nonlinear Loss Engineering in Near‐Zero‐Index Bulk Materials

Transparent conducting oxides (TCOs) show unprecedented optical nonlinearities in the near infrared wavelength range, where the real part of their linear refractive index approaches zero. More specifically, the Kerr nonlinearities of these materials have sparked widespread attention due to their magnitude and speed. However, due to the absorptive nature of these nonlinear processes, it is of fundamental interest to further investigate the imaginary component of the nonlinear index. The present work studies the nonlinear optical absorption properties of aluminium‐doped zinc oxide (AZO) thin films in their near‐zero‐index (NZI) spectral window. It is found that the imaginary part of the refractive index is reduced under optical excitation such that the field penetration depth more than doubles. An optically induced shift of the NZI bandwidth of ≈120 nm for a pump intensity of 1.3 TW cm −2 is also demonstrated. Looking into the optically induced spectral redistribution of the probe signal, local net gain is recorded, which is ascribed to a nonlinear adiabatic energy transfer. The present study adds key information about the fundamental interplay between real and imaginary nonlinear indices in NZI media, while advancing parametric amplification as viable direction for loss compensation.

36 MATERIALS SCIENCE↗

Time-refraction optics with single cycle modulation

Abstract We present an experimental study of optical time-refraction caused by time-interfaces as short as a single optical cycle. Specifically, we study the propagation of a probe pulse through a sample undergoing a large refractive index change induced by an intense modulator pulse. In these systems, increasing the refractive index abruptly leads to time-refraction where the spectrum of all the waves propagating in the medium is red-shifted, and subsequently blue-shifted when the refractive index relaxes back to its original value. We observe these phenomena in the single-cycle regime. Moreover, by shortening the temporal width of the modulator to ∼5–6 fs, we observe that the rise time of the red-shift associated with time-refraction is proportionally shorter. The experiments are carried out in transparent conducting oxides acting as epsilon-near-zero materials. These observations raise multiple questions on the fundamental physics occurring within such ultrashort time frames, and open the way for experimenting with photonic time-crystals, generated by periodic ultrafast changes to the refractive index, in the near future.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗