Ultrashort energetic terahertz (THz) pulses have opened up exciting new avenues of research in the field of light-matter interactions. For material studies in small laboratories, researchers often require widely tunable femtosecond THz pulses with a peak field strength close to MV/cm. Currently, these pulses can be generated through optical rectification and difference frequency generation in crystals without inversion symmetry. We present in this talk a novel approach for generating THz pulses with no frequency tuning gap. Our method is based on Raman-resonance-enhanced four-wave mixing in centrosymmetric media, specifically diamond. We demonstrate that this technique enables the generation of highly stable, few-cycle pulses with near-Gaussian spatial and temporal profiles. Using a 0.5-mm-thick diamond, we were able to generate THz pulses with a stable and controllable carrier-envelope phase. These pulses carried approximately 15 nJ of energy per pulse at 10 THz, with a peak field strength of about 1 MV/cm at the focus. Experimental measurements of the THz pulse characteristics were in good agreement with theoretical predictions. We also discuss the way to improve output energy.
Precise and ultrafast control over photo-induced charge currents across nanoscale interfaces could lead to important applications in energy harvesting, ultrafast electronics, and coherent terahertz sources. Recent studies have shown that several relativistic mechanisms, including inverse spin-Hall effect, inverse Rashba–Edelstein effect, and inverse spin-orbit-torque effect, can convert longitudinally injected spin-polarized currents from magnetic materials to transverse charge currents, thereby harnessing these currents for terahertz generation. However, these mechanisms typically require external magnetic fields and exhibit limitations in terms of spin-polarization rates and efficiencies of relativistic spin-to-charge conversion. We present a nonrelativistic and nonmagnetic mechanism that directly utilizes the photoexcited high-density charge currents across the interface. We demonstrate that the electrical anisotropy of conductive oxides RuO2 and IrO2 can effectively deflect injected charge currents to the transverse direction, resulting in efficient and broadband terahertz radiation. Importantly, this mechanism has the potential to offer much higher conversion efficiency compared to previous methods, as conductive materials with large electrical anisotropy are readily available, whereas further increasing the spin-Hall angle of heavy-metal materials would be challenging. Our findings offer exciting possibilities for directly utilizing these photoexcited high-density currents across metallic interfaces for ultrafast electronics and terahertz spectroscopy.
The ability to generate and manipulate broadband chiral terahertz waves is essential for applications in material imaging, terahertz sensing, and diagnosis. It can also open up new possibilities for nonlinear terahertz spectroscopy and coherent control of chiral molecules and magnetic materials. The existing methods, however, often suffer from low efficiency, narrow bandwidth, or poor flexibility. Here, we propose a novel type of laser-driven terahertz emitters, consisting of metasurface-patterned magnetic multilayer heterostructures, that can overcome the shortcomings of the conventional approaches. Such hybrid terahertz emitters combine the advantages of spintronic emitters for being ultrabroadband, efficient, and highly flexible, as well as those of metasurfaces for the powerful control capabilities over the polarization state of emitted terahertz waves on an ultracompact platform. Taking a stripe-patterned metasurface as an example, we demonstrate the efficient generation and manipulation of broadband chiral terahertz waves. The ellipticity can reach >0.75 over a broad terahertz bandwidth (1 to 5 THz), representing a high-quality and efficient source for few-cycle circularly polarized terahertz pulses with stable carrier waveforms. Flexible control of ellipticity and helicity is also demonstrated with our systematic experiments and numerical simulations. We show that the terahertz polarization state is dictated by the interplay between laser-induced spintronic-origin currents and the screening charges/currents in the metasurfaces, which exhibits tailored anisotropic properties due to the predesigned geometric confinement effects. Our work opens a new pathway to metasurface-tailored spintronic emitters for efficient vector-control of electromagnetic waves in the terahertz regime.
We experimentally demonstrate that temporally confined spatial solitons can be realized by space-time coupled propagation of strong femtosecond pulses in a nonlinear optical resonator, consisting of periodic layered Kerr media (PLKM). A universal relationship between the characteristic beam size and the critical nonlinear phase of the solitary modes is revealed, defining different regions of soliton stability. Taking advantage of the unique characters of these solitary modes, we demonstrate supercontinuum generation and pulse compression of initially 260 μJ, 170 fs pulses down to 22 fs in a single-stage PLKM resonator with an efficiency >90%.
Graphene-based electric power generation that converts mechanical energy of flow of ionic droplets over the device surface into electricity has emerged as a promising candidate for blue-energy network. Yet the lack of a microscopic understanding of the underlying mechanism has prevented ability to optimize and control the performance of such devices. This requires information on interfacial structure and charging behavior at the molecular level. Here, we use sum-frequency vibrational spectroscopy (SFVS) to probe the interface of device composed of aqueous solution, graphene and supporting polymer substrate. We discover that the surface dipole layer of the polymer is responsible for ion attraction toward and adsorption at the graphene surface that leads to electricity generation in graphene. Graphene itself does not attract ions and only acts as a conducting sheet for the induced carrier transport. Replacing the polymer by an organic ferroelectric substrate could enhance the efficiency and allow switching of the electricity generation. Our microscopic understanding of the electricity generation process paves the way for the rational design of scalable and more efficient droplet-motion-based energy transducer devices.
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