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Register a new userLinear magneto-electric phase in ultrathin MnPS$_{3}$ probed by optical second harmonic generation
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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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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.
In second harmonic generation, the phase of the optical field is doubled which has important implication. Here the phase doubling effect is utilized to solve a long-standing challenge in power scaling of single frequency laser. When a (-{pi}/2, {pi}/2) binary phase modulation is applied to a single frequency seed laser to broaden the spectrum and suppress the stimulated Brillouin scattering in high power fiber amplifier, the second harmonic of the phase-modulated laser will return to single frequency, because the (-{pi}/2, {pi}/2) modulation is doubled to (-{pi}, {pi}) for the second harmonic. A compression rate as high as 95% is demonstrated in the experiment limited by the electronic bandwidth of the setup, which can be improved with optimized devices.
A systematic {it ab initio} study of the second-order nonlinear optical properties of BN nanotubes within density functional theory in the local density approximation has been performed. Highly accurate full-potential projector augmented-wave method was used. Specifically, the second-harmonic generation ($chi_{abc}^{(2)}$) and linear electro-optical ($r_{abc}$) coefficients of a large number of the single-walled zigzag, armchair and chiral BN nanotubes (BN-NT) as well as the double-walled zigzag (12,0)@(20,0) BN nanotube and the single-walled zigzag (12,0) BN-NT bundle have been calculated. Importantly, unlike carbon nanotubes, both the zigzag and chiral BN-NTs are found to exhibit large second-order nonlinear optical behavior with the $chi_{abc}^{(2)}$ and $r_{abc}$ coefficients being up to thirty times larger than that of bulk BN in both zinc-blende and wurtzite structures, indicating that BN-NTs are promising materials for nonlinear optical and opto-electric applications. Though the interwall interaction in the double-walled BN-NTs is found to reduce the second-order nonlinear optical coefficients significantly, the interwall interaction in the single-walled BN-NT bundle has essentially no effect on the nonlinear optical properties. The prominant features in the spectra of $chi_{abc}^{(2)}(-2omega,omega,omega)$ of the BN-NTs are suscessfully correlated with the features in the linear optical dielectric function $epsilon (omega)$ in terms of single-photon and two-photon resonances.
We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $Delta<F_m>/<F_m>$ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries.
We consider phase separated states in magnetic oxides (MO) thin films. We show that these states have a non-zero electric polarization. Moreover, the polarization is intimately related to a spatial distribution of magnetization in the film. Polarized states with opposite polarization and opposite magnetic configuration are degenerate. An external electric field removes the degeneracy and allows to switch between the two states. So, one can control electric polarization and magnetic configuration of the phase separated MO thin film with the external electric field.
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