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Register a new userNonlinear terahertz electro-optical responses in metals
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I. Paul
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Motivated by the recent developments in terahertz spectroscopy using pump-probe setups, we develop the theory of finite frequency nonlinear electro-optical responses in centrosymmetric metals starting from basic time dependent perturbation theory. We express the nonlinear current kernel as a sum of several causal response functions. These functions cannot be evaluated using perturbative field theory methods. Consequently, we associate each response function with an imaginary time ordered current correlation function, which can be factorized using Wicks theorem. The mapping between the response functions and the correlation functions, suitably analytically continued to real frequencies, is proven exactly. We derive constraints satisfied by the nonlinear current kernel and we prove a generalized $f$-sum rule for the nonlinear conductivity, all of which are consequences of particle number conservation. We apply the theory to compute the gauge invariant nonlinear conductivity of a system of noninteracting electrons in the presence of weak disorder. As special cases of this generalized nonlinear response, we discuss its third harmonic and its instantaneous terahertz Kerr signals. Our formalism can be used to compute the nonlinear conductivity in symmetry broken phases such as density waves and nematic states.
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We theoretically study THz-light-driven high-harmonic generation (HHG) in the spin-liquid states of the Kitaev honeycomb model with a magnetostriction coupling between spin and electric polarization. To compute the HHG spectra, we numerically solve the Lindblad equation, taking account of the dissipation effect. We find that isotropic Kitaev models possess a dynamical symmetry, which is broken by a static electric field, analogous to HHG in electron systems. We show that the HHG spectra exhibit characteristic continua of Majorana fermion excitations, and their broad peaks can be controlled by applying static electric or magnetic fields. In particular, the magnetic-field dependence of the HHG spectra drastically differs from those of usual ordered magnets. These results indicate that an intense THz laser provides a powerful tool to observe dynamic features of quantum spin liquids.
Chiral magnets, which break both spatial inversion and time reversal symmetries, carry a potential for quadratic optical responses. Despite the possibility of enhanced and controlled responses through the magnetic degree of freedom, the systematic understanding remains yet to be developed. We here study nonlinear optical responses in a prototypical chiral magnetic state with a one-dimensional conical order by using the second-order response theory. We show that the photovoltaic effect and the second harmonic generation are induced by asymmetric modulation of the electronic band structure under the conical magnetic order, and the coefficients, including the sign, change drastically depending on the frequency of incident lights, the external magnetic field, and the strength of spin-charge coupling. We find that both effects can be enormously large compared to those in the conventional nonmagnetic materials. Our results would pave the way for next-generation optical electronic devices, such as unconventional solar cells and optical sensors, based on chiral magnets.
Strong optical pulses at mid-infrared and terahertz frequencies have recently emerged as a powerful tool to manipulate and control the solid state and especially complex condensed matter systems with strongly correlated electrons. The recent developments in high-power sources in the 0.1-30 THz frequency range, both from table-top laser systems and Free-Electron Lasers, has provided access to excitations of molecules and solids, which can be stimulated at their resonance frequencies. Amongst these, we discuss free electrons in metals, superconducting gaps and Josephson plasmons in layered superconductors, vibrational modes of the crystal lattice (phonons), as well as magnetic excitations. This Review provides an overview and illustrative examples of how intense THz transients can be used to resonantly control matter, with particular focus on strongly correlated electron systems and high-temperature superconductors.
Nonlinear optical (NLO) responses of topological materials are under active research in recent years. Yet by far most studies focused on the bulk properties, whereas the surface effects and the difference between surface and bulk responses have not been systematically studied. In this work, we develop a generic Greens function framework to investigate the surface NLO properties of topological materials. The Greens function framework can naturally incorporate many body effects and can be easily extended to high order NLO responses. Using $rm T_d WTe_2$ as an example, we reveal that the surface can behave disparately from the bulk under light illumination. Remarkably, the shift and circular current on the surface can flow in opposite directions to that in the bulk. Moreover, the light induced spin current on the surface can be orders of magnitude stronger than that in the bulk. We also study the responses under inhomogeneous field and higher order NLO effect, which are all distinct on the surface. These anomalous surface NLO responses suggest that light can be a valuable tool for probing the surface states of topological materials, while on the other hand, the surface effects shall be prudently considered when investigating the optical properties of topological materials.
Chiral topological semimetals are materials that break both inversion and mirror symmetries. They host interesting phenomena such as the quantized circular photogalvanic effect (CPGE) and the chiral magnetic effect. In this work, we report a comprehensive theoretical and experimental analysis of the linear and non-linear optical responses of the chiral topological semimetal RhSi, which is known to host multifold fermions. We show that the characteristic features of the optical conductivity, which display two distinct quasi-linear regimes above and below 0.4 eV, can be linked to excitations of different kinds of multifold fermions. The characteristic features of the CPGE, which displays a sign change at 0.4 eV and a large non-quantized response peak of around 160 $mu textrm{A V}^{-2}$ at 0.7 eV, are explained by assuming that the chemical potential crosses a flat hole band at the Brillouin zone center. Our theory predicts that, in order to observe a quantized CPGE in RhSi, it is necessary to increase the chemical potential as well as the quasiparticle lifetime. More broadly our methodology, especially the development of the broadband terahertz emission spectroscopy, could be widely applied to study photo-galvanic effects in noncentrosymmetric materials and in topological insulators in a contact-less way and accelerate the technological development of efficient infrared detectors based on topological semimetals.
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