Terahertz electromagnetic radiation is extremely useful for numerous applications such as imaging and spectroscopy. Therefore, it is highly desirable to have an efficient table-top emitter covering the 1-to-30-THz window whilst being driven by a low-cost, low-power femtosecond laser oscillator. So far, all solid-state emitters solely exploit physics related to the electron charge and deliver emission spectra with substantial gaps. Here, we take advantage of the electron spin to realize a conceptually new terahertz source which relies on tailored fundamental spintronic and photonic phenomena in magnetic metal multilayers: ultrafast photo-induced spin currents, the inverse spin-Hall effect and a broadband Fabry-Pérot resonance. Guided by an analytical model, such spintronic route offers unique possibilities for systematic optimization. We find that a 5.8-nm-thick W/CoFeB/Pt trilayer generates ultrashort pulses fully covering the 1-to-30-THz range. Our novel source outperforms laser-oscillatordriven emitters such as ZnTe(110) crystals in terms of bandwidth, terahertz-field amplitude, flexibility, scalability and cost. IntroductionThe terahertz (THz) window, loosely defined as the frequency range from 0.3 to 30 THz in the electromagnetic spectrum, is located between the realms of electronics and optics 1,2 . As this region coincides with many fundamental resonances of materials, THz radiation enables very selective spectroscopic insights into all phases of matter with high temporal 3,4 and spatial 5,6,7,8 resolution. Consequently, numerous applications in basic research 3,4 , imaging 5 and quality control 8 have emerged.To fully exploit the potential of THz radiation, energy-efficient and low-cost sources of ultrashort THz pulses are required. Most broadband table-top emitters are driven by femtosecond laser pulses that generate the required THz charge current by appropriately mixing the various optical frequencies 9,10 . Sources made from solids usually consist of semiconducting or insulating structures with naturally or artificially broken inversion symmetry. When the incident photon energy is below the semiconductor band gap, optical rectification causes a charge displacement that follows the intensity envelope of the incident pump pulse 9,10,11,12,13,14,15,16,17 . For above-band-gap excitation, the response is dominated by a photocurrent 18,19,20,21,22,23,24 with a temporally step-like onset and, thus, generally smaller bandwidth than optical rectification 9 . Apart from rare exceptions 14 , however, most semiconductors used are polar 1,2,12,13,15,16,17,21,22 and strongly attenuate THz radiation around optical phonon resonances, thereby preventing emission in the so-called Reststrahlen band located between ~1 and 15 THz.The so far most promising sources covering the full THz window are photocurrents in transient gas plasmas 9,10,25,26,27,28,29 . The downside of this appealing approach is that the underlying ionization process usually requires amplified laser pulses with high threshold energies on the order of 0....
Multiple optical harmonic generation-the multiplication of photon energy as a result of nonlinear interaction between light and matter-is a key technology in modern electronics and optoelectronics, because it allows the conversion of optical or electronic signals into signals with much higher frequency, and the generation of frequency combs. Owing to the unique electronic band structure of graphene, which features massless Dirac fermions, it has been repeatedly predicted that optical harmonic generation in graphene should be particularly efficient at the technologically important terahertz frequencies. However, these predictions have yet to be confirmed experimentally under technologically relevant operation conditions. Here we report the generation of terahertz harmonics up to the seventh order in single-layer graphene at room temperature and under ambient conditions, driven by terahertz fields of only tens of kilovolts per centimetre, and with field conversion efficiencies in excess of 10, 10 and 10 for the third, fifth and seventh terahertz harmonics, respectively. These conversion efficiencies are remarkably high, given that the electromagnetic interaction occurs in a single atomic layer. The key to such extremely efficient generation of terahertz high harmonics in graphene is the collective thermal response of its background Dirac electrons to the driving terahertz fields. The terahertz harmonics, generated via hot Dirac fermion dynamics, were observed directly in the time domain as electromagnetic field oscillations at these newly synthesized higher frequencies. The effective nonlinear optical coefficients of graphene for the third, fifth and seventh harmonics exceed the respective nonlinear coefficients of typical solids by 7-18 orders of magnitude. Our results provide a direct pathway to highly efficient terahertz frequency synthesis using the present generation of graphene electronics, which operate at much lower fundamental frequencies of only a few hundreds of gigahertz.
The nature of the photoconductivity in solution-processed films of methylammonium lead iodide perovskite is investigated by determining the variation of the photoconductive response with temperature. Ultrabroadband terahertz (THz) photoconductivity spectra in the 0.3-10 THz range can be reproduced well by a simple Drude-like response at room temperature, where free charge carrier motion is characterized by an average scattering time. The scattering time determined from Drude fits in the 0.3-2THz region increases from ∼4 fs at 300 K (tetragonal phase; mobility of ∼27 cm(2) V(-1) s(-1)) to almost ∼25 fs at 77 K (orthorhombic phase, mobility of ∼150 cm(2) V(-1) s(-1)). For the tetragonal phase (temperature range 150< T < 300 K) the scattering time shows a ∼T(-3/2) dependence, approaching the theoretical limit for pure acoustic phonon (deformation potential) scattering. Hence, electron-phonon, rather than impurity scattering, sets the upper limit on free charge transport for this perovskite.
The outstanding charge transport properties of graphene enable numerous electronic applications of this remarkable material, many of which are expected to operate at ultrahigh speeds. In the regime of ultrafast, sub-picosecond electric fields, however, the very high conduction properties of graphene are not necessarily preserved, with the physical picture explaining this behaviour remaining unclear. Here we show that in graphene, the charge transport on an ultrafast timescale is determined by a simple thermodynamic balance maintained within the graphene electronic system acting as a thermalized electron gas. The energy of ultrafast electric fields applied to graphene is converted into the thermal energy of its entire charge carrier population, near-instantaneously raising the electronic temperature. The dynamic interplay between heating and cooling of the electron gas ultimately defines the ultrafast conductivity of graphene, which in a highly nonlinear manner depends on the dynamics and the strength of the applied electric fields.
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