Terahertz Pulse Generation with Binary Phase Control in Nonlinear InAs Metasurface.

The effect of terahertz (THz) pulse generation has revolutionized broadband coherent spectroscopy and imaging at THz frequencies. However, THz pulses typically lack spatial structure, whereas structured beams are becoming essential for advanced spectroscopy applications. Nonlinear optical metasurfaces with nanoscale THz emitters can provide a solution by defining the beam structure at the generation stage. We develop a nonlinear InAs metasurface consisting of nanoscale optical resonators for simultaneous generation and structuring of THz beams. We find that THz pulse generation in the resonators is governed by optical rectification. It is more efficient than in ZnTe crystals, and it allows us to control the pulse polarity and amplitude, offering a platform for realizing binary-phase THz metasurfaces. To illustrate this capability, we demonstrate an InAs metalens, which simultaneously generates and focuses THz pulses. The control of spatiotemporal structure using nanoscale emitters opens doors for THz beam engineering and advanced spectroscopy and imaging applications.

Resonant metasurfaces for generating complex quantum states.

Quantum state engineering, the cornerstone of quantum photonic technologies, mainly relies on spontaneous parametric downconversion and four-wave mixing, where one or two pump photons spontaneously decay into a photon pair. Both of these nonlinear effects require momentum conservation for the participating photons, which strongly limits the versatility of the resulting quantum states. Nonlinear metasurfaces have subwavelength thickness and allow the relaxation of this constraint; when combined with resonances, they greatly expand the possibilities of quantum state engineering. Here, we generated entangled photons via spontaneous parametric downconversion in semiconductor metasurfaces with high-quality factor, quasi-bound state in the continuum resonances. By enhancing the quantum vacuum field, our metasurfaces boost the emission of nondegenerate entangled photons within multiple narrow resonance bands and over a wide spectral range. A single resonance or several resonances in the same sample, pumped at multiple wavelengths, can generate multifrequency quantum states, including cluster states. These features reveal metasurfaces as versatile sources of complex states for quantum information.

Correction to "Terahertz Pulse Generation from GaAs Metasurfaces".

[This corrects the article DOI: 10.1021/acsphotonics.1c01908.].

Terahertz Pulse Generation from GaAs Metasurfaces.

Ultrafast optical excitation of select materials gives rise to the generation of broadband terahertz (THz) pulses. This effect has enabled the field of THz time-domain spectroscopy and led to the discovery of many physical mechanisms behind THz generation. However, only a few materials possess the required properties to generate THz radiation efficiently. Optical metasurfaces can relax stringent material requirements by shifting the focus onto the engineering of local electromagnetic fields to boost THz generation. Here we demonstrate the generation of THz pulses in a 160 nm thick nanostructured GaAs metasurface. Despite the drastically reduced volume, the metasurface emits THz radiation with efficiency comparable to that of a thick GaAs crystal. We reveal that along with classical second-order volume nonlinearity, an additional mechanism contributes strongly to THz generation in the metasurface, which we attribute to surface nonlinearity. Our results lay the foundation for engineering of semiconductor metasurfaces for efficient and versatile THz radiation emitters.

The Interplay of Symmetry and Scattering Phase in Second Harmonic Generation from Gold Nanoantennas.

Nonlinear phenomena are central to modern photonics but, being inherently weak, typically require gradual accumulation over several millimeters. For example, second harmonic generation (SHG) is typically achieved in thick transparent nonlinear crystals by phase-matching energy exchange between light at initial, ω, and final, 2ω, frequencies. Recently, metamaterials imbued with artificial nonlinearity from their constituent nanoantennas have generated excitement by opening the possibility of wavelength-scale nonlinear optics. However, the selection rules of SHG typically prevent dipole emission from simple nanoantennas, which has led to much discussion concerning the best geometries, for example, those breaking centro-symmetry or incorporating resonances at multiple harmonics. In this work, we explore the use of both nanoantenna symmetry and multiple harmonics to control the strength, polarization and radiation pattern of SHG from a variety of antenna configurations incorporating simple resonant elements tuned to light at both ω and 2ω. We use a microscopic description of the scattering strength and phases of these constituent particles, determined by their relative positions, to accurately predict the SHG radiation observed in our experiments. We find that the 2ω particles radiate dipolar SHG by near-field coupling to the ω particle, which radiates SHG as a quadrupole. Consequently, strong linearly polarized dipolar SHG is only possible for noncentro-symmetric antennas that also minimize interference between their dipolar and quadrupolar responses. Metamaterials with such intra-antenna phase and polarization control could enable compact nonlinear photonic nanotechnologies.

Measuring chromatic aberrations in imaging systems using plasmonic nanoparticles.

We demonstrate a method to measure chromatic aberrations of microscope objectives with metallic nanoparticles using white light. Extinction spectra are recorded while scanning a single nanoparticle through a lens's focal plane. We show a direct correlation between the focal wavelength and the longitudinal chromatic focal shift through our analysis of the variations between the scanned extinction spectra at each scan position and the peak extinction over the entire scan. The method has been tested on achromat and apochromat objectives using aluminum disks varying in size from 260-520 nm. Our method is straightforward, robust, low cost, and broadband with a sensitivity suitable for assessing longitudinal chromatic aberrations in high-numerical-aperture apochromatic corrected lenses.

Spectral interferometric microscopy reveals absorption by individual optical nanoantennas from extinction phase.

Optical antennas transform light from freely propagating waves into highly localized excitations that interact strongly with matter. Unlike their radio frequency counterparts, optical antennas are nanoscopic and high frequency, making amplitude and phase measurements challenging and leaving some information hidden. Here we report a novel spectral interferometric microscopy technique to expose the amplitude and phase response of individual optical antennas across an octave of the visible to near-infrared spectrum. Although it is a far-field technique, we show that knowledge of the extinction phase allows quantitative estimation of nanoantenna absorption, which is a near-field quantity. To verify our method we characterize gold ring-disk dimers exhibiting Fano interference. Our results reveal that Fano interference only cancels a bright mode's scattering, leaving residual extinction dominated by absorption. Spectral interference microscopy has the potential for real-time and single-shot phase and amplitude investigations of isolated quantum and classical antennas with applications across the physical and life sciences.