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Register a new userHigh-harmonic generation by electric polarization, spin current, and magnetization
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High-harmonic generation (HHG), a typical nonlinear optical effect, has been actively studied in electron systems such as semiconductors and superconductors. As a natural extension, we theoretically study HHG from electric polarization, spin current and magnetization in magnetic insulators under terahertz (THz) or gigahertz (GHz) electromagnetic waves. We use simple one-dimensional spin chain models with or without multiferroic coupling between spins and the electric polarization, and study the dynamics of the spin chain coupled to an external ac electric or magnetic field. We map spin chains to two-band fermions and invoke an analogy of semiconductors and superconductors. With a quantum master equation and Lindblad approximation, we compute the time evolution of the electric polarization, spin current, and magnetization, showing that they exhibit clear harmonic peaks. We also show that the even-order HHG by magnetization dynamics can be controlled by static magnetic fields in a wide class of magnetic insulators. We propose experimental setups to observe these HHG, and estimate the required strength of the ac electric field $E_0$ for detection as $E_0sim100$kV/cm--1MV/cm, which corresponds to the magnetic field $B_0sim0.1$T--1T. The estimated strength would be relevant also for experimental realizations of other theoretically-proposed nonlinear optical effects in magnetic insulators such as Floquet engineering of magnets.
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By using the Floquet eigenstates, we derive a formula to calculate the high-harmonic components of the electric current (HHC) in the setup where a monochromatic laser field is turned on at some time. On the basis of this formulation, we study the HHC spectrum of electrons on a one-dimensional chain with the staggered potential to study the effect of multiple sites in the unit cell such as the systems with charge density wave (CDW) order. With the help of the solution for the Floquet eigenstates, we analytically show that two plateaus of different origins emerge in the HHC spectrum. The widths of these plateaus are both proportional to the field amplitude, but inversely proportional to the laser frequency and its square, respectively. We also show numerically that multi-step plateaus appear when both the field amplitude and the staggered potential are strong.
Competition and cooperation among orders is at the heart of many-body physics in strongly correlated materials and leads to their rich physical properties. It is crucial to investigate what impact many-body physics has on extreme nonlinear optical phenomena, with the possibility of controlling material properties by light. However, the effect of competing orders and electron-electron correlations on highly nonlinear optical phenomena has not yet been experimentally clarified. Here, we investigated high-order harmonic generation from the Mott-insulating phase of Ca2RuO4. Changing the gap energy in Ca2RuO4 as a function of temperature, we observed a strong enhancement of high order harmonic generation at 50 K, increasing up to several hundred times compared to room temperature. We discovered that this enhancement can be well-reproduced by an empirical scaling law that depends only on the material gap energy and photon emission energy. Such scaling law cannot be explained by a simple two-band model under the single electron approximation. Our results suggest that the highly nonlinear optical response of strongly correlated materials is deeply coupled to their electron-electron correlations and resultant many-body electronic structure.
Skyrmions, once a hypothesized field-theoretical object believed to describe the nature of elementary particles, became common sightings in recent years among several non-centrosymmetric metallic ferromagnets. For more practical applications of Skyrmionic matter as carriers of information, thus realizing the prospect of Skyrmionics, it is necessary to have the means to create and manipulate Skyrmions individually. We show through extensive simulation of the Landau-Lifshitz-Gilbert equation that a circulating current imparted to the metallic chiral ferromagnetic system can create isolated Skyrmionic spin texture without the aid of external magnetic field.
We consider noninteracting electrons coupled to laser fields, and study perturbatively the effects of the lattice potential involving disorder on the harmonic components of the electric current, which are sources of high-order harmonic generation (HHG). By using the Floquet-Keldysh Green functions, we show that each harmonic component consists of the coherent and the incoherent parts, which arise respectively from the coherent and the incoherent scatterings by the local ion potentials. As the disorder increases, the coherent part decreases, the incoherent one increases, and the total harmonic component of the current first decreases rapidly and then approaches a nonzero value. Our results highlight the importance of the periodicity of crystals, which builds up the Bloch states extending over the solid. This is markedly different from the traditional HHG in atomic gases, where the positions of individual atoms are irrelevant.
The transition metal thiophosphates $M$PS$_3$ ($M$ = Mn, Fe, Ni) are a class of van der Waals stacked insulating antiferromagnets that can be exfoliated down to the ultrathin limit. MnPS$_3$ is particularly interesting because its N$acute{textrm{e}}$el ordered state breaks both spatial-inversion and time-reversal symmetries, allowing for a linear magneto-electric phase that is rare among van der Waals materials. However, it is unknown whether this unique magnetic structure of bulk MnPS$_3$ remains stable in the ultrathin limit. Using optical second harmonic generation rotational anisotropy, we show that long-range linear magneto-electric type N$acute{textrm{e}}$el order in MnPS$_3$ persists down to at least 5.3 nm thickness. However an unusual mirror symmetry breaking develops in ultrathin samples on SiO$_2$ substrates that is absent in bulk materials, which is likely related to substrate induced strain.
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