Magnetic spin moment reduction in photoexcited ferromagnets through exchange interaction quenching: Beyond the rigid band approximation

The exchange interaction among electrons is one of the most fundamental quantum mechanical interactions in nature and underlies any magnetic phenomena from ferromagnetic ordering to magnetic storage. The current technology is built upon a thermal or magnetic field, but a frontier is emerging to directly control magnetism using ultrashort laser pulses. However, little is known about the fate of the exchange interaction. Here we report unambiguously that photoexcitation is capable of quenching the exchange interaction in all three $3d$ ferromagnetic metals. The entire process starts with a small number of photoexcited electrons which build up a new and self-destructive potential that collapses the system into a new state with a reduced exchange splitting. The spin moment reduction follows a Bloch-like law as $M_z(\Delta E)=M_z(0)(1-{\Delta E}/{\Delta E_0})^{\frac{1}{\beta}}$, where $\Delta E$ is the absorbed photon energy and $\beta$ is a scaling exponent. A good agreement is found between the experimental and our theoretical results. Our findings may have a broader implication for dynamic electron correlation effects in laser-excited iron-based superconductors, iron borate, rare-earth orthoferrites, hematites and rare-earth transition metal alloys.Comment: 16 pages, 3 figures, one supplementary material fil

Generating high-order optical and spin harmonics from ferromagnetic monolayers

High-order harmonic generation (HHG) in solids has entered a new phase of intensive research, with envisioned band-structure mapping on an ultrashort time scale. This partly benefits from a flurry of new HHG materials discovered, but so far has missed an important group. HHG in magnetic materials should have profound impact on future magnetic storage technology advances. Here we introduce and demonstrate HHG in ferromagnetic monolayers. We find that HHG carries spin information and sensitively depends on the relativistic spin-orbit coupling; and if they are dispersed into the crystal momentum ${\bf k}$ space, harmonics originating from real transitions can be ${\bf k}$-resolved and carry the band structure information. Geometrically, the HHG signal is sensitive to spatial orientations of monolayers. Different from the optical counterpart, the spin HHG, though probably weak, only appears at even orders, a consequence of SU(2) symmetry. Our findings open an unexplored frontier -- magneto-high-order harmonic generation.Comment: 19 pages, 4 figure

Strong and nearly 100%\% spin-polarized second-harmonic generation from ferrimagnet Mn2_{2}RuGa

Second-harmonic generation (SHG) has emerged as a promising tool for detecting electronic and magnetic structures in noncentrosymmetric materials, but 100$\%$ spin-polarized SHG has not been reported. In this work, we demonstrate nearly 100$\%$ spin-polarized SHG from half-metallic ferrimagnet Mn$_{2}$RuGa. A band gap in the spin-down channel suppresses SHG, so the spin-up channel contributes nearly all the signal, as large as 3614 pm/V about 10 times larger than that of GaAs. In the spin-up channel, $\chi_{xyz}^{(2)}$ is dominated by the large intraband current in three highly dispersed bands near the Fermi level. With the spin-orbit coupling (SOC), the reduced magnetic point group allows additional SHG components, where the interband contribution is enhanced. Our finding is important as it predicts a large and complete spin-polarized SHG in a all-optical spin switching ferrimagnet. This opens the door for future applications

A Formalization of The Natural Gradient Method for General Similarity Measures

In optimization, the natural gradient method is well-known for likelihood maximization. The method uses the Kullback-Leibler divergence, corresponding infinitesimally to the Fisher-Rao metric, which is pulled back to the parameter space of a family of probability distributions. This way, gradients with respect to the parameters respect the Fisher-Rao geometry of the space of distributions, which might differ vastly from the standard Euclidean geometry of the parameter space, often leading to faster convergence. However, when minimizing an arbitrary similarity measure between distributions, it is generally unclear which metric to use. We provide a general framework that, given a similarity measure, derives a metric for the natural gradient. We then discuss connections between the natural gradient method and multiple other optimization techniques in the literature. Finally, we provide computations of the formal natural gradient to show overlap with well-known cases and to compute natural gradients in novel frameworks

Extended Calculations of Spectroscopic Data: Energy Levels, Lifetimes and Transition rates for O-like ions from Cr XVII to Zn XXIII

Employing two state-of-the-art methods, multiconfiguration Dirac--Hartree--Fock and second-order many-body perturbation theory, the excitation energies and lifetimes for the lowest 200 states of the $2s^2 2p^4$, $2s 2p^5$, $2p^6$, $2s^2 2p^3 3s$, $2s^2 2p^3 3p$, $2s^2 2p^3 3d$, $2s 2p^4 3s$, $2s 2p^4 3p$, and $2s 2p^4 3d$ configurations, and multipole (electric dipole (E1), magnetic dipole (M1), and electric quadrupole (E2)) transition rates, line strengths, and oscillator strengths among these states are calculated for each O-like ion from Cr XVII to Zn XXIII. Our two data sets are compared with the NIST and CHIANTI compiled values, and previous calculations. The data are accurate enough for identification and deblending of new emission lines from the sun and other astrophysical sources. The amount of data of high accuracy is significantly increased for the $n = 3$ states of several O-like ions of astrophysics interest, where experimental data are very scarce

Non-Abelian toplogical superconductors from topological semimetals and related systems under superconducting proximity effect

Non-Abelian toplogical superconductors are characterized by the existence of {zero-energy} Majorana fermions bound in the quantized vortices. This is a consequence of the nontrivial bulk topology characterized by an {\em odd} Chern number. It is found that in topological semimetals with a single two-bands crossing point all the gapped superconductors are non-Abelian ones. Such a property is generalized to related but more generic systems which will be useful in the search of non-Abelian superconductors and Majorana fermions