Polarization-dependent photon spectroscopy (dichroism) of the second-harmonic generation (SHG) response is shown to reveal chiral and magnetic properties of a sample. Two dichroic signals are allowed with electric-dipole (E1) and electric-quadrupole (E2) scattering events, and both require circular polarization in the primary beam. Explicit expressions for electronic multipoles, which benefit from equivalent electronic operators, in NCD and MCD of the SHG response are derived using theoretical techniques from atomic physics.
It is proven that the sum rules for X-ray magnetic dichroism (XMCD) spectra that are used to separate spin and orbital contributions to the magnetic moment are formally correct for an arbitrary strength of electron-electron interactions. However, their practical application for strongly correlated systems can become complicated due to the spectral density weight spreading over a broad energy interval. Relevance of incoherent spectral density for the XMCD sum rules is illustrated by a simple model of a ferromagnet with orbital degrees of freedom.
We have investigated the valence, spin, and orbital state of the Co ions in the one-dimensional cobaltate Ca3Co2O6 using x-ray absorption and x-ray magnetic circular dichroism at the Co-L2,3 edges. The Co ions at both the octahedral Co_oct and trigonal Co_trig sites are found to be in a 3+ state. From the analysis of the dichroism we established a low-spin state for the Co_oct and a high-spin state with an anomalously large orbital moment of 1.7 muB at the Co3+ trig ions. This large orbital moment along the c-axis chain and the unusually large magnetocrystalline anisotropy can be traced back t…
Ca_1-xSr_xRuO_3, which is ferromagnetic for Sr concentration x > 0.3, has been studied by x-ray magnetic circular dichroism (XMCD) in Ru 3p and O 1s core-level x-ray absorption. XMCD signals appear at x ~ 0.3 and monotonically increases with x in the ferromagnetic phase. While the monotonic increase of the XMCD signals with x is of a typical Stoner-type, the absence of appreciable change in the spectral line shapes of both the Ru 3p and O 1s XMCD spectra indicate that the itinerant-electron ferromagnetism in Ca_1-xSr_xRuO_3 is influenced by strong electron correlation.
Although the Ni_4 cluster includes more information regarding the Ni band structure with respect to the Anderson impurity model, it also favors very peculiar ground states which are incompatible with a coherent picture of all dichroism experiments.
Recent photoemission work on underdoped cuprates between Tc and T*, the pseudogap temperature, are interpreted within the framework of a previously developed negative-U scenario. From this exposition, incorporating a developed 2q diagonal striping model, detailed understanding follows of the ARPES results, together with certain STM and far infrared optical data. Identification of the origin of the magnetic circular dichroism and related effects exhibited by such materials below T* also appears to have been achieved.
We have performed x-ray magnetic circular dichroism (XMCD) measurements on the iron-based superconductor Sr$_2$VFeAsO$_{3-δ}$ to study the origin of weak ferromagnetism (WFM) reported for this compound. While Fe 3$d$ electrons show a magnetic response similar to the other iron pnictides, signals from V 3$d$ electrons remain finite at zero magnetic field and may be responsible for the WFM.
We theoretically investigate the origin of the x-ray magnetic circular dichroism (XMCD) spectra at the K edges of Mn and Ga in the ferromagnetic phase of Mn3GaC on the basis of an ab initio calculation. Taking account of the spin-orbit interaction in the LDA scheme, we obtain the XMCD spectra in excellent agreement with the recent experiment. We have analyzed the origin of each structure, and thus elucidated the mechanism of inducing the orbital polarization in the p symmetric states. We also discuss a simple sum rule connecting the XMCD spectra with the orbital moment in the p symmetric state…
A differential coupling of topological surface states to left- versus right-circularly polarized light is the basis of many opto-spintronics applications of topological insulators. Here we report direct evidence of circular dichroism from the surface states of Bi$_2$Se$_3$ using a laser-based time-of-flight angle-resolved photoemission spectroscopy. By employing a novel sample rotational analysis, we resolve unusual modulations in the circular dichroism photoemission pattern as a function of both energy and momentum, which perfectly mimic the predicted but hitherto un-observed three-dimensiona…
X-ray magnetic circular dichroism (XMCD) is generally not observed for antiferromagnetic (AFM) states because XMCD signals from the antiparallelly coupled spins cancel each other. In this letter, we theoretically show the presence of an XMCD signal from compensated two-dimensional triangle AFM structures on a Kagome lattice. The calculation reveals the complete correspondence between the XMCD spectra and the sign of the spin chirality: the XMCD signal only appears when the spin chirality is negative. This XMCD signal originates from the different absorption coefficients of the three sublattice…
We report on the growth and characterization of ferromagnetic Gd-doped EuO thin films. We prepared samples with Gd concentrations up to 11% by means of molecular beam epitaxy under distillation conditions, which allows a very precise control of the doping concentration and oxygen stoichiometry. Using soft x-ray magnetic circular dichroism at the Eu and Gd M4,5 edges, we found that the Curie temperature ranged from 69 K for pure stoichiometric EuO to about 170 K for the film with the optimal Gd doping of around 4%. We also show that the Gd magnetic moment couples ferromagnetically to that of Eu…
We study the spin-dependent electronic structure of UTe and UT_{2}Si_{2} (T=Cu and Mn) compounds with a combination of x-ray magnetic circular dichroism measurements and first principle calculations. By exploiting the presence of sizable quadrupolar and dipolar contributions to the U L_{2,3}-edge x-ray absorption cross section we are able to provide unique information on the extent of hybridization between 5f and 6d/3d electronic states, a key parameter regulating the physical properties of all actinide materials. Since this information is hardly accessible to other probes, the new methodology…
We report resonant inelastic x-ray scattering (RIXS) excited by circularly polarized x-rays on Mn-Zn ferrite at the Mn L2,3-resonances. We demonstrate that crystal field excitations, as expected for localized systems, dominate the RIXS spectra and thus their dichroic asymmetry cannot be interpreted in terms of spin-resolved partial density of states, which has been the standard approach for RIXS dichroism. We observe large dichroic RIXS at the L2-resonance which we attribute to the absence of metallic core hole screening in the insulating Mn-ferrite. On the other hand, reduced L3-RIXS dichrois…
We report an ARPES investigation of the circular dichroism in the first Brillouin zone (BZ) of under- and overdoped Pb-Bi2212 samples. We show that the dichroism has opposite signs for bonding and antibonding components of the bilayer-split CuO-band and is antisymmetric with respect to reflections in both mirror planes parallel to the c-axis. Using this property of the energy and momentum intensity distributions we prove the existence of the bilayer splitting in the normal state of the underdoped compound and compare its value with the splitting in overdoped sample. In agreement with previous …
We have performed x-ray magnetic circular dichroism (XMCD) and valence-band photoemission studies of the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te. XMCD signals due to ferromagnetism were observed at the Cr 2p absorption edge. Comparison with atomic multiplet calculations suggests that the magnetically active component of the Cr ion was divalent under the tetrahedral crystal field with tetragonal distortion along the crystalline a-, b-, and c-axes. In the valence-band spectra, spectral weight near the Fermi level was strongly suppressed, suggesting the importance of Jahn-Teller ef…
Surface magnetic properties of perovskite manganites have been a recurrent topic during last years since they play a major role in the implementation of magnetoelectronic devices. Magneto-optical techniques, such as X-ray magnetic circular dichroism, turn out to be a very efficient tool to study surface magnetism due to their sensitivity to magnetic and chemical variations across the sample depth. Nevertheless, the application of the sum rules for the determination of the spin magnetic moment might lead to uncertainties as large as 40% in case of Mn ions. To overcome this problem we present an…
A detailed theoretical study on the electronic structure and magnetic properties of half-metallic ferromagnet CrO$_2$ was carried out by means of relativistic full-potential linear muffin-tin orbital method within the generalized gradient approximation (GGA) to the exchange correlation potential. Our calculation favours the [001] magnetization axis to be the easy axis of magnetization when compared to the [100] axis which is in agreement with the experiments. The calculated spin and orbital magnetic moments of Cr agrees well with the experimental and other theoretical works. The Cr L$_{2,3}$ x…
We have investigated the electronic structure of ZnO:Mn and ZnO:Mn,N thin films using x-ray magnetic circular dichroism (XMCD) and resonance-photoemission spectroscopy. From the Mn 2$p$$\rightarrow3d$ XMCD results, it is shown that, while XMCD signals only due to paramagnetic Mn$^{2+}$ ions were observed in ZnO:Mn, nonmagnetic, paramagnetic and ferromagnetic Mn$^{2+}$ ions coexist in ZnO:Mn,N. XMCD signals of ZnO:Mn,N revealed that the localized Mn$^{2+}$ ground state and Mn$^{2+}$ state hybridized with ligand hole coexisted, implying $p$-$d$ exchange coupling. In the valence-band spectra, spe…
