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.
Dynamically controlling terahertz (THz) waves with an ultracompact device is highly desired, but previously realized tunable devices are bulky in size and/or exhibit limited light-tuning functionalities. Here, we experimentally demonstrate dynamic modulation on THz waves with a dielectric metasurface in mode-selective or mode-unselective manners through pumping the system at different optical wavelengths. Quasi-normal-mode theory reveals that the physics is governed by the spatial overlap between wave functions of resonant modes and regions inside resonators perturbed by pump laser excitation at different wavelengths. We further design/fabricate a dielectric metasurface and experimentally demonstrate that it can dynamically control the polarization state of incident THz waves, dictated by the strength and wavelength of the pumping light. We finally numerically demonstrate pump wavelength-controlled optical information encryption based on a carefully designed dielectric metasurface. Our studies reveal that pump light wavelength can be a new external knob to dynamically control THz waves, which may inspire many tunable metadevices with diversified functionalities.
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%.
It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date the connection between out-ofequilibrium and equilibrium phase transitions was not known, nor how fast the out-of-equilibrium phase transitions can proceed. In this work, by combining time- and angle-resolved photoemission (Tr-ARPES) with time-resolved transverse magneto-optical Kerr (Tr-TMOKE) spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: the spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, while demagnetization and the collapse of the exchange splitting occur on much longer timescales. Third, we find that the transient electron temperature alone dictates the magnetic response. By comparing results obtained from different methods, we show that the critical behaviors are essential for fully explaining the fluence-dependent magnetization dynamics measured using magneto-optical spectroscopy
Tabletop-scale coherent EUV generated through high-harmonic generation (HHG) produces light in the form of an attosecond pulse train that uniquely combines characteristics of good energy resolution (≈100-300meV) with sub-fs time resolution. This makes HHG an ideal source for studying the fastest dynamics in materials. Furthermore, using angle-resolved photoemission spectroscopy (ARPES), it is possible to extract detailed information about electron dynamics over the entire Brillouin zone. In recently published work, we combined HHG with ARPES to identify a sub-femtosecond excited-state lifetime for the first time. Photoemission occurs as a three-step process: 1) An electron is photoexcited from the valence band to far above the Fermi energy; 2) it transports to the surface, and 3) it overcomes the work function and exits. If the electron is promoted into a highlyexcited unoccupied band in the material (as opposed to a free-electron-like state), we observe the electron emission lifetime to increase in a measurable way—the Ni band 22 eV above the Fermi level has a lifetime of 212±30 attoseconds. Furthermore, by comparing photoemission from Cu and Ni, we reveal the influence of attosecond-timescale electron screening vs scattering by the electrons near the fermi surface. This work for the first time demonstrates the relevance of attosecond spectroscopy to the study of intrinsic properties and band structure in materials, as opposed to the strong-field induced dynamics studied extensively to-date.
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