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....
The latest concepts for quantum computing and data storage envision to address and manipulate single spins. A limitation for single atoms or molecules in contact to a metal surface are the short lifetime of excited spin states, typically picoseconds, due to the exchange of energy and angular momentum with the itinerant electrons of the substrate [1-4]. Here we show that paramagnetic molecules on a superconducting substrate exhibit excited spin states with a lifetime of approximately 10 ns. We ascribe this increase in lifetime by orders of magnitude to the depletion of electronic states within the energy gap at the Fermi level. This prohibits pathways of energy relaxation into the substrate and allows for electrically pumping the magnetic molecule into higher spin states, making superconducting substrates premium candidates for spin manipulation. We further show that the proximity of the scanning tunneling microscope tip modifies the magnetic anisotropy
Three-dimensional topological insulators are fascinating materials with insulating bulk yet metallic surfaces that host highly mobile charge carriers with locked spin and momentum. Remarkably, surface currents with tunable direction and magnitude can be launched with tailored light beams. To better understand the underlying mechanisms, the current dynamics need to be resolved on the timescale of elementary scattering events (∼10 fs). Here, we excite and measure photocurrents in the model topological insulator Bi2Se3 with a time resolution of 20 fs by sampling the concomitantly emitted broadband terahertz (THz) electromagnetic field from 0.3 to 40 THz. Strikingly, the surface current response is dominated by an ultrafast charge transfer along the Se–Bi bonds. In contrast, photon-helicity-dependent photocurrents are found to be orders of magnitude smaller than expected from generation scenarios based on asymmetric depopulation of the Dirac cone. Our findings are of direct relevance for broadband optoelectronic devices based on topological-insulator surface currents.
The magnetism of single atoms and molecules is governed by the atomic scale environment. In general, the reduced symmetry of the surrounding splits the d states and aligns the magnetic moment along certain favorable directions. Here, we show that we can reversibly modify the magnetocrystalline anisotropy by manipulating the environment of single iron(II) porphyrin molecules adsorbed on Pb(111) with the tip of a scanning tunneling microscope. When we decrease the tip-molecule distance, we first observe a small increase followed by an exponential decrease of the axial anisotropy on the molecules. This is in contrast to the monotonous increase observed earlier for the same molecule with an additional axial Cl ligand ( Nat. Phys. 2013 , 9 , 765 ). We ascribe the changes in the anisotropy of both species to a deformation of the molecules in the presence of the attractive force of the tip, which leads to a change in the d level alignment. These experiments demonstrate the feasibility of a precise tuning of the magnetic anisotropy of an individual molecule by mechanical control.
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