Perturbative regime of terahertz high-harmonics generation in topological insulators

In this Letter, terahertz high harmonic generation processes in topological insulators of the bismuth and antimony chalcogenides family are investigated. Field conversion efficiencies are determined and clean cubic and quintic power-law scaling is observed for third and fifth harmonics, up to driving terahertz fields of 140 kV/cm. This is in contrast to all previous experiments on terahertz harmonics generation in Dirac materials where a non-perturbative regime has been observed already at few 10s kV/cm driving fields. Our nonlinear THz spectroscopy experiments are complemented by THz pump - optical probe measurements showing distinctly different relaxation dynamics of the carriers in the topologically-protected Dirac states at the surfaces and the bulk. The THz-induced dynamics of surface states reveal ultrafast relaxation that prevents accumulation effects, and results in a clear perturbative regime of THz harmonics generation that is different to graphene or Dirac semimetals with their slower relaxation times in the few ps regime

Terahertz signatures of ultrafast Dirac fermion relaxation at the surface of topological insulators

Topologically protected surface states present rich physics and promising spintronic, optoelectronic, and photonic applications that require a proper understanding of their ultrafast carrier dynamics. Here, we investigate these dynamics in topological insulators (TIs) of the bismuth and antimony chalcogenide family, where we isolate the response of Dirac fermions at the surface from the response of bulk carriers by combining photoexcitation with below-bandgap terahertz (THz) photons and TI samples with varying Fermi level, including one sample with the Fermi level located within the bandgap. We identify distinctly faster relaxation of charge carriers in the topologically protected Dirac surface states (few hundred femtoseconds), compared to bulk carriers (few picoseconds). In agreement with such fast cooling dynamics, we observe THz harmonic generation without any saturation effects for increasing incident fields, unlike graphene which exhibits strong saturation. This opens up promising avenues for increased THz nonlinear conversion efficiencies, and high-bandwidth optoelectronic and spintronic information and communication applications.Parts of this research were carried out at ELBE at the Helmholtz-Zentrum Dresden-Rossendorf e.V., a member of the Helmholtz Association. The films are grown in IRE RAS within the framework of the state task. This work was supported by the RFBR grants Nos. 18-29-20101, 19-02-00598. N.A., S.K., and I.I. acknowledge support from the European Union’s Horizon 2020 research and innovation program under grant agreement No. 737038 (TRANSPIRE). T.V.A.G.O. and L.M.E. acknowledge the support by the Würzburg-Dresden Cluster of Excellence on Complexity and Topology in Quantum Matter (ct.qmat). K.-J.T. acknowledges funding from the European Union’s Horizon 2020 research and innovation program under Grant Agreement No. 804349 (ERC StG CUHL) and financial support through the MAINZ Visiting Professorship. ICN2 was supported by the Severo Ochoa program from Spanish MINECO Grant No. SEV-2017-0706

Non-perturbative terahertz high-harmonic generation in the three-dimensional Dirac semimetal Cd3As2

Harmonic generation is a general characteristic of driven nonlinear systems, and serves as an efficient tool for investigating the fundamental principles that govern the ultrafast nonlinear dynamics. Here, we report on terahertz-field driven high-harmonic generation in the three-dimensional Dirac semimetal Cd3As2 at room temperature. Excited by linearly-polarized multi-cycle terahertz pulses, the third-, fifth-, and seventh-order harmonic generation is very efficient and detected via time-resolved spectroscopic techniques. The observed harmonic radiation is further studied as a function of pump-pulse fluence. Their fluence dependence is found to deviate evidently from the expected power-law dependence in the perturbative regime. The observed highly non-perturbative behavior is reproduced based on our analysis of the intraband kinetics of the terahertz-field driven nonequilibrium state using the Boltzmann transport theory. Our results indicate that the driven nonlinear kinetics of the Dirac electrons plays the central role for the observed highly nonlinear response. © 2020, The Author(s)

Inertial spin dynamics in ferromagnets

The understanding of how spins move and can be manipulated at pico- and femtosecond timescales has implications for ultrafast and energy-efficient data-processing and storage applications. However, the possibility of realizing commercial technologies based on ultrafast spin dynamics has been hampered by our limited knowledge of the physics behind processes on this timescale. Recently, it has been suggested that inertial effects should be considered in the full description of the spin dynamics at these ultrafast timescales, but a clear observation of such effects in ferromagnets is still lacking. Here, we report direct experimental evidence of intrinsic inertial spin dynamics in ferromagnetic thin films in the form of a nutation of the magnetization at a frequency of ~0.5 THz. This allows us to reveal that the angular momentum relaxation time in ferromagnets is on the order of 10 ps

Terahertz signatures of ultrafast Dirac fermion relaxation at the surface of topological insulators

Kovalev S, Tielrooij K-J, Deinert J-C, et al. Terahertz signatures of ultrafast Dirac fermion relaxation at the surface of topological insulators. NPJ QUANTUM MATERIALS. 2021;6(1): 84.Topologically protected surface states present rich physics and promising spintronic, optoelectronic, and photonic applications that require a proper understanding of their ultrafast carrier dynamics. Here, we investigate these dynamics in topological insulators (TIs) of the bismuth and antimony chalcogenide family, where we isolate the response of Dirac fermions at the surface from the response of bulk carriers by combining photoexcitation with below-bandgap terahertz (THz) photons and TI samples with varying Fermi level, including one sample with the Fermi level located within the bandgap. We identify distinctly faster relaxation of charge carriers in the topologically protected Dirac surface states (few hundred femtoseconds), compared to bulk carriers (few picoseconds). In agreement with such fast cooling dynamics, we observe THz harmonic generation without any saturation effects for increasing incident fields, unlike graphene which exhibits strong saturation. This opens up promising avenues for increased THz nonlinear conversion efficiencies, and high-bandwidth optoelectronic and spintronic information and communication applications