Ultrafast photocurrents in MoSe2_2 probed by terahertz spectroscopy

We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe$_2$. We identify several distinct mechanisms producing THz radiation in response to an ultrashort ($30\,$fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscillations at about $23\,$THz in the emission from the BL sample. We attribute the oscillations to quantum beats between two excitonic states with energetic separation of $\sim100\,$meV.Comment: This is the Accepted Manuscript version of an article accepted for publication in 2D Materials. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at https://doi.org/10.1088/2053-1583/abd527 7 pages, 9 figure

Ultrafast photocurrents in MoSe2 probed by terahertz spectroscopy

We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe2. We identify several distinct mechanisms producing THz radiation in response to an ultrashort (30 fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscillations at about 23 THz in the emission from the BL sample. We attribute the oscillations to quantum beats between two excitonic states with energetic separation of similar to 100 meV

Tunable ultrabroadband hybrid THz emitter combining a spintronic THz source and a GaSe crystal

Linear terahertz time-domain spectroscopy (THz-TDS) is a sensitive probe for material characterization including thickness measurements of thin layers. These applications critically rely on a sufficiently large bandwidth, which is not straightforwardly available in typical THz-TDS systems. Here, we introduce a hybrid THz-emitter concept based on a spintronic THz emitter that is deposited onto a thin freestanding GaSe nonlinear crystal. By tuning the parameters of this hybrid emitter, we generate an ultrabroadband spectrum covering the full range from 1 to 40 THz without any gaps at high spectral amplitudes, resulting in ultrashort THz-pulse durations of only 32 fs. Finally, we demonstrate the straightforward tunability of the carrier-envelope phase from unipolar or bipolar THz pulses with ultrashort duration

Terahertz Spin‐to‐Charge Conversion by Interfacial Skew Scattering in Metallic Bilayers

The efficient conversion of spin to charge transport and vice versa is of major relevance for the detection and generation of spin currents in spin‐based electronics. Interfaces of heterostructures are known to have a marked impact on this process. Here, terahertz (THz) emission spectroscopy is used to study ultrafast spin‐to‐charge‐current conversion (S2C) in about 50 prototypical F|N bilayers consisting of a ferromagnetic layer F (e.g., Ni81Fe19, Co, or Fe) and a nonmagnetic layer N with strong (Pt) or weak (Cu and Al) spin‐orbit coupling. Varying the structure of the F/N interface leads to a drastic change in the amplitude and even inversion of the polarity of the THz charge current. Remarkably, when N is a material with small spin Hall angle, a dominant interface contribution to the ultrafast charge current is found. Its magnitude amounts to as much as about 20% of that found in the F|Pt reference sample. Symmetry arguments and first‐principles calculations strongly suggest that the interfacial S2C arises from skew scattering of spin‐polarized electrons at interface imperfections. The results highlight the potential of skew scattering for interfacial S2C and propose a promising route to enhanced S2C by tailored interfaces at all frequencies from DC to terahertz

Emission of coherent THz magnons in an antiferromagnetic insulator triggered by ultrafast spin–phonon interactions

Antiferromagnetic materials have been proposed as new types of narrowband THz spintronic devices owing to their ultrafast spin dynamics. Manipulating coherently their spin dynamics, however, remains a key challenge that is envisioned to be accomplished by spin-orbit torques or direct optical excitations. Here, we demonstrate the combined generation of broadband THz (incoherent) magnons and narrowband (coherent) magnons at 1 THz in low damping thin films of NiO/Pt. We evidence, experimentally and through modeling, two excitation processes of spin dynamics in NiO: an off-resonant instantaneous optical spin torque in (111) oriented films and a strain-wave-induced THz torque induced by ultrafast Pt excitation in (001) oriented films. Both phenomena lead to the emission of a THz signal through the inverse spin Hall effect in the adjacent heavy metal layer. We unravel the characteristic timescales of the two excitation processes found to be 300 fs, respectively, and thus open new routes towards the development of fast opto-spintronic devices based on antiferromagnetic materials

Laser-induced terahertz spin transport in magnetic nanostructures arises from the same force as ultrafast demagnetization

Laser-induced terahertz spin transport (TST) and ultrafast demagnetization (UDM) are central but so far disconnected phenomena in femtomagnetism and terahertz spintronics. Here, we use broadband terahertz emission spectroscopy to reliably measure both processes in one setup. We find that the rate of UDM in a single simple ferromagnetic metal film F such as Co70Fe30 or Ni80Fe20 has the same time evolution as TST from F into an adjacent normal-metal layer N such as Pt or W. As this remarkable agreement refers to two very different samples, an F layer vs an F|N stack, it does not result from the trivial fact that TST out of F reduces the F magnetization at the same rate. Instead, our observation strongly suggests that UDM in F and TST in F|N are driven by the same force, which is fully determined by the state of the ferromagnet. An analytical model quantitatively explains our measurements and reveals that both UDM in the F sample and TST in the associated F|N stack arise from a generalized spin voltage, i.e., an excess of magnetization, which is defined for arbitrary, nonthermal electron distributions. We also conclude that contributions due to a possible temperature difference between F and N, i.e., the spin-dependent Seebeck effect, and optical intersite spin transfer are minor in our experiment. Based on these findings, one can apply the vast knowledge of UDM to TST to significantly increase spin-current amplitudes and, thus, open promising pathways toward energy-efficient ultrafast spintronic devices

Terahertz Spin-to-Charge Current Conversion in Stacks of Ferromagnets and the Transition-Metal Dichalcogenide NbSe2

Transition-metal dichalcogenides (TMDCs) are an aspiring class of materials with unique electronic and optical properties and potential applications in spin-based electronics. Here, terahertz emission spectroscopy is used to study spin-to-charge current conversion (S2C) in the TMDC NbSe2 in ultra-high-vacuum-grown F|NbSe2 thin-film stacks, where F is a layer of ferromagnetic Fe or Ni. Ultrafast laser excitation triggers an ultrafast spin current that is converted into an in-plane charge current and, thus, a measurable THz electromagnetic pulse. The THz signal amplitude as a function of the NbSe2 thickness shows that the measured signals are fully consistent with an ultrafast optically driven injection of an in-plane-polarized spin current into NbSe2. Modeling of the spin-current dynamics reveals that a sizable fraction of the total S2C originates from the bulk of NbSe2 with the opposite, negative sign of the spin Hall angle as compared to Pt. By a quantitative comparison of the emitted THz radiation from F|NbSe2 to F|Pt reference samples and the results of ab initio calculations, it is estimated that the spin Hall angle of NbSe2 for an in-plane polarized spin current lies between -0.2% and -1.1%, while the THz spin-current relaxation length is of the order of a few nanometers

Impact of gigahertz and terahertz transport regimes on spin propagation and conversion in the antiferromagnet IrMn

Control over spin transport in antiferromagnetic systems is essential for future spintronic applications with operational speeds extending to ultrafast time scales. Here, we study the transition from the gigahertz (GHz) to terahertz (THz) regime of spin transport and spin-to-charge current conversion (S2C) in the prototypical antiferromagnet IrMn by employing spin pumping and THz spectroscopy techniques. We reveal a factor of 4 shorter characteristic propagation lengths of the spin current at THz frequencies (∼0.5 nm) as compared to GHz experiments (∼2 nm). This observation may be attributed to different transport regimes. The conclusion is supported by extraction of sub-picosecond temporal dynamics of the THz spin current. We identify no relevant impact of the magnetic order parameter on S2C signals and no scalable magnonic transport in THz experiments. A significant role of the S2C originating from interfaces between IrMn and magnetic or non-magnetic metals is observed, which is much more pronounced in the THz regime and opens the door for optimization of the spin control at ultrafast time scales

Terahertz Néel spin-orbit torques drive nonlinear magnon dynamics in antiferromagnetic Mn2Au

Antiferromagnets have large potential for ultrafast coherent switching of magnetic order with minimum heat dissipation. In materials such as Mn2Au and CuMnAs, electric rather than magnetic fields may control antiferromagnetic order by Néel spin-orbit torques (NSOTs). However, these torques have not yet been observed on ultrafast time scales. Here, we excite Mn2Au thin films with phase-locked single-cycle terahertz electromagnetic pulses and monitor the spin response with femtosecond magneto-optic probes. We observe signals whose symmetry, dynamics, terahertz-field scaling and dependence on sample structure are fully consistent with a uniform in-plane antiferromagnetic magnon driven by field-like terahertz NSOTs with a torkance of (150 ± 50) cm2 A−1 s−1. At incident terahertz electric fields above 500 kV cm−1, we find pronounced nonlinear dynamics with massive Néel-vector deflections by as much as 30°. Our data are in excellent agreement with a micromagnetic model. It indicates that fully coherent Néel-vector switching by 90° within 1 ps is within close reach

Accessing ultrafast spin-transport dynamics in copper using broadband terahertz spectroscopy

We study the spatiotemporal dynamics of ultrafast electron spin transport across nanometer-thick copper layers using broadband terahertz spectroscopy. Our analysis of temporal delays, broadening and attenuation of the spin-current pulse revealed ballistic-like propagation of the pulse peak, approaching the Fermi velocity, and diffusive features including a significant velocity dispersion. A comparison to the frequency-dependent Ficks law identified the diffusion-dominated transport regime for distances larger than 2 nm. The findings lie the groundwork for designing future broadband spintronic devices.Comment: Main text consists of 3 figures and 4 pages of tex