The photoinduced magnetism in manganese-tetracyanoethylene (Mn-TCNE) molecule-based magnets is ascribed to charge-transfer excitations from manganese to TCNE. Charge-transfer energies
are calculated using Density Functional Theory; photoinduced magnetization is described using a
model Hamiltonian based on a double-exchange mechanism. Photoexciting electrons from the manganese
core spin into the lowest unoccupied orbital of TCNE with photon energies around 3 eV
increases the magnetization through a reduction of the canting angle of the manganese core spins
for an average electron density on TCNE less than one. When photoexciting with a smaller energy,
divalent TCNE molecules are formed. The delocalization of the excited electron causes a local spin flip of a manganese core spin.
Hole systems are characterized by an effective spin 3/2. It was shown that the spin density matrix for spin-3/2 systems can be decomposed into a sequence of multipoles that has important higher-order contributions beyond the ones known for electron systems [R. Winkler, Phys. Rev. B 70, 125301 (2004)]. We show here that the hole spin polarization (i.e., the dipole) and the higher-order multipoles can precess due to the usual spin-orbit coupling in the valence band, yet in the absence of a magnetic field. The hole spin precession is important in the context of spin relaxation and offers the possibility of new device applications. We discuss a setup based on recent experiments in which this precession can be observed and show that it gives rise to an alternating spin polarization.
Core-level X-ray photoemission spectra for copper, manganese, and ruthenium compounds are calculated. A strong dependence of the spectral line shape on electron/hole doping, magnetic and orbital ordering is observed. The changes can be explained in terms of the competition between local and nonlocal screening effects. In contrast to earlier claims, we find that the changes do not result from additional quasiparticle states at the Fermi level but from a strong coupling of the different screening channels to changes in the ground state. The strong sensitivity of core-level XPS on the surrounding transition-metal atoms enables the study of temperature- and doping-induced changes in orbital occupation and ordering.
The Resonant Inelastic X-ray Scattering (RIXS) cross section at the L and M edges of transition-metal compounds is studied using an effective scattering operator. The intensities of the elastic peak and for spin-flip processes are derived. A detailed analysis of the polarization and angular dependence of L- and M-edge RIXS for divalent copper compounds, such as the high-Tc superconductors, is given.
Density plot of the RIXS intensities at the L3 edge for a 90o scattering geometry as a function of the angle q of the incoming radiation with the surface normal and the angle j between the polarization vector and the scattering plane. The ground state has a hole in the x2-y25orbital. The intensities for scattering into x2-y26 and xy 6 are zero.