We present a method to measure quadratic Terahertz optical nonlinearities in Terahertz time-domain spectroscopy. We use a rotating linear polarizer (a polarizing chopper) to modulate the amplitude of the incident THz pulse train. We use a phase-sensitive lock-in detection at the fundamental and the second harmonic of the modulation frequency to separate the materials responses that are linear and quadratic in Terahertz electric field. We demonstrate this method by measuring the quadratic Terahertz Kerr effect in the presence of the much stronger linear electro-optic effect in the (110) GaP crystal. We propose that the method can be used to detect Terahertz second harmonic generation in noncentrosymmetric media in time-domain spectroscopy, with broad potential applications in nonlinear Terahertz photonics and related technology.
Atomically thin transition metal dichalcogenides are highly promising for integrated optoelectronic and photonic systems due to their exciton-driven linear and nonlinear interaction with light. Integrating them into optical fibers yields novel opportunities in optical communication, remote sensing, and all-fiber optoelectronics. However, scalable and reproducible deposition of high quality monolayers on optical fibers is a challenge. Here, we report the chemical vapor deposition of monolayer MoS2 and WS2 crystals on the core of microstructured exposed core optical fibers and their interaction with the fibers guided modes. We demonstrate two distinct application possibilities of 2D-functionalized waveguides to exemplify their potential. First, we simultaneously excite and collect excitonic 2D material photoluminescence with the fiber modes, opening a novel route to remote sensing. Then we show that third harmonic generation is modified by the highly localized nonlinear polarization of the monolayers, yielding a new avenue to tailor nonlinear optical processes in fibers. We anticipate that our results may lead to significant advances in optical fiber based technologies.
Light with light control of surface plasmon polaritons is theoretically demonstrated. A barely simple and compact source of these waves consists in a finite number of slits (evenly spaced) perforating a metal film. The system scatters electromagnetic fields in one side of the metal film when it is illuminated from the opposite side by a polarized light source. High intensity light sources moreover efficiently generate light at second harmonic and higher frequencies in the metal led by optical nonlinearities. It is shown how the mixing of fields scattered by the slits from a weak beam at $lambda$ wavelength, with the second harmonic fields generated by a high intensity $2 lambda$ beam, creates a destructive interference of surface plasmons in one of the two possible directions of emission from the slits, while these are enhanced along the opposite direction. The unidirectional launching of surface plasmons is due to the different properties of symmetry at $lambda$ whether they are linearly or nonlinearly generated. It is envisaged a nanodevice which might allow sending digital information codified in the surface plasmon field or be used to build ultra-narrow bandwidth surface plasmon frequency combs.
We present an electrically switchable graphene terahertz (THz) modulator with a tunable-by-design optical bandwidth and we exploit it to compensate the cavity dispersion of a quantum cascade laser (QCL). Electrostatic gating is achieved by a metal-grating used as a gate electrode, with an HfO2/AlOx gate dielectric on top. This is patterned on a polyimide layer, which acts as a quarter wave resonance cavity, coupled with an Au reflector underneath. We get 90% modulation depth of the intensity, combined with a 20 kHz electrical bandwidth in the 1.9 _ 2.7 THz range. We then integrate our modulator with a multimode THz QCL. By adjusting the modulator operational bandwidth, we demonstrate that the graphene modulator can partially compensates the QCL cavity dispersion, resulting in an integrated laser behaving as a stable frequency comb over 35% of the laser operational range, with 98 equidistant optical modes and with a spectral coverage of ~ 1.2 THz. This has significant potential for frontier applications in the terahertz, as tunable transformation-optics devices, active photonic components, adaptive and quantum optics, and as a metrological tool for spectroscopy at THz frequencies.
We report ionic strength-dependent phase shifts in second harmonic generation (SHG) signals from charged interfaces that verify a recent model in which dispersion between the fundamental and second harmonic beams modulates observed signal intensities. We show how phase information can be used to unambiguously separate the chi(2) and interfacial potential-dependent chi(3) terms that contribute to the total signal and provide a path to test primitive ion models and mean field theories for the electrical double layer with experiments to which theory must conform. Finally, we demonstrate the new method on supported lipid bilayers and comment on the ability of our new instrument to identify hyper-Rayleigh scattering contributions to common homodyne SHG measurements in reflection geometries.
Graphene offers a possibility for actively controlling plasmon confinement and propagation by tailoring its spatial conductivity pattern. However, implementation of this concept has been hampered because uncontrollable plasmon reflection is easily induced by inhomogeneous dielectric environment. In this work, we demonstrate full electrical control of plasmon reflection/transmission at electronic boundaries induced by a zinc-oxide-based dual gate, which is designed to minimize the dielectric modulation. Using Fourier-transform infrared spectroscopy, we show that the plasmon reflection can be varied continuously with the carrier density difference between the adjacent regions. By utilizing this functionality, we show the ability to control size, position, and frequency of plasmon cavities. Our approach can be applied to various types of plasmonic devices, paving the way for implementing a programmable plasmonic circuit.