We report on the optical properties from terahertz (THz) to Near-Infrared (NIR) of the layered magnetic compound CrI3 at various temperatures, both in the paramagnetic and ferromagnetic phase. In the NIR spectral range, we observe an insulating electronic gap around 1.1 eV which strongly hardens with decreasing temperature. The blue shift observed represents a record in insulating materials and it is a fingerprint of a strong electron-phonon interaction. Moreover, a further gap hardening is observed below the Curie temperature, indicating the establishment of an effective interaction between electrons and magnetic degrees of freedom in the ferromagnetic phase. Similar interactions are confirmed by the disappearance of some phonon modes in the same phase, as expected from a spin-lattice interaction theory. Therefore, the optical properties of CrI3 reveal a complex interaction among electronic, phononic and magnetic degrees of freedom, opening many possibilities for its use in 2-Dimensional heterostructures.
16 August 2023 in ACS Applied Electronic Materials
Optical vector beams have great potential in many applications, for example, optical tweezers, information transmission and processing, laser surface structuring, particle acceleration, and vortex dichroism spectroscopy. However, reported vector beams in the terahertz (THz) spectral range are limited to exhibit only low-order topological charges. Therefore, methodologies to generate THz vector beam bearing tailored topological charge are highly desired. This work investigates how to generate THz vector beams with a tailored topological charge via the optical rectification process in a 111-cut ZnTe crystal pumped with a vector optical beam and how to manipulate the vector THz beam's polarization state through the initial polarization angle. We theoretically and experimentally demonstrate that the transduction process produces THz topological charge twice that of the infrared pump, also admitting the opposite sign. Given the well-developed technology to design infrared vector beams, the proposed method can generate THz vector beams with tailored topological charges.
THz-based technologies and research applications have seen a rapid increment in recent period together with the development of novel radiation sources based both on relativistic electrons and laser techniques. In this framework, laser-induced plasma filament plays an important role in generating intense and broadband THz radiation. Although many attentions have been paid to THz emission from two-color plasma filaments, one-color plasma emission has been scarcely investigated. In particular, the polarization state of one-color THz emission is still controversial due to the limitations of the existing THz detection techniques, which are incapable of simultaneously detecting elliptically and radially polarized THz radiation. In this manuscript, we develop a novel detection method and unambiguously demonstrate for the first time that one-color laser-induced plasma filament simultaneously emits elliptically and radially polarized THz radiation. These polarization states suggest that the generation mechanism results from electric quadrupole, showing a new route for producing more complex polarization states and THz vortex beams.
HMQ-TMS (2-(4-hydroxy-3-methoxystyryl)-1-methylquinolinium 2,4,6-trimethylbenzenesulfonate) is a recently discovered anisotropic organic crystal that can be exploited for the production of broadband high-intensity terahertz (THz) radiation through the optical rectification (OR) technique. HMQ-TMS plays a central role in THz technology due to its broad transparency range, large electro-optic coefficient and coherence length, and excellent crystal properties. However, its anisotropic optical properties have not been deeply researched yet. Here, from polarized reflectance and transmittance measurements along the and axes of a HMQ-TMS single-crystal, we extract both the refraction index n and the extinction coefficient k between 50 and 35,000 cm . We further measure the THz radiation generated by optical rectification at different infrared (IR) wavelengths and along the two and axes. These data highlight the remarkable anisotropic linear and nonlinear optical behavior of HMQ-TMS crystals, expanding the knowledge of its properties and applications from the THz to the UV region.
The diffusion of light by random materials is a general phenomenon that appears in many different systems, spanning from colloidal suspension in liquid crystals to disordered metal sponges and paper composed of random fibers. Random scattering is also a key element behind mimicry of several animals, such as white beetles and chameleons. Here, random scattering is related to micro and nanosized spatial structures affecting a broad electromagnetic region. In this work, we have investigated how random scattering modulates the optical properties, from terahertz to ultraviolet light, of a novel functional material, i.e., a three-dimensional graphene (3D Graphene) network based on interconnected high-quality two-dimensional graphene layers. Here, random scattering generates a high-frequency pass-filter behavior. The optical properties of these graphene structures bridge the nanoworld into the macroscopic world, paving the way for their use in novel optoelectronic devices.