Critical slowing down near the multiferroic phase transition in MnWO4_4

By using broadband dielectric spectroscopy in the radiofrequency and microwave range we studied the magnetoelectric dynamics in the multiferroic chiral antiferromagnet MnWO$_4$. Above the multiferroic phase transition at $T_{N2} \approx 12.6$ K we observe a critical slowing down of the corresponding magnetoelectric fluctuations resembling the soft-mode behavior in canonical ferroelectrics. This electric field driven excitation carries much less spectral weight than ordinary phonon modes. Also the critical slowing down of this mode scales with an exponent larger than one which is expected for magnetic second order phase transition scenarios. Therefore the investigated dynamics have to be interpreted as the softening of an electrically active magnetic excitation, an electromagnon.Comment: 5 pages, 4 figures, appendi

The biaxial nonlinear crystal BiB3O6 as a polarization entangled photon source using non-collinear type-II parametric down-conversion

We describe the full characterization of the biaxial nonlinear crystal BiB3O6 (BiBO) as a polarization entangled photon source using non-collinear type-II parametric down-conversion. We consider the relevant parameters for crystal design, such as cutting angles, polarization of the photons, effective nonlinearity, spatial and temporal walk-offs, crystal thickness and the effect of the pump laser bandwidth. Experimental results showing entanglement generation with high rates and a comparison to the well investigated beta-BaB2O4 (BBO) crystal are presented as well. Changing the down-conversion crystal of a polarization entangled photon source from BBO to BiBO enhances the generation rate as if the pump power was increased by more than three times. Such an improvement is currently required for the generation of multiphoton entangled states.Comment: 15 pages, 13 figures, published versio

The spin-12\frac{1}{2} XXZ chain system Cs2_2CoCl4_4 in a transverse magnetic field

Comparing high-resolution specific heat and thermal expansion measurements to exact finite-size diagonalization, we demonstrate that Cs$_2$CoCl$_4$ for a magnetic field along the crystallographic b axis realizes the spin-$\frac{1}{2}$ XXZ chain in a transverse field. Exploiting both thermal as well as virtual excitations of higher crystal field states, we find that the spin chain is in the XY-limit with an anisotropy $J_z/J_\perp \approx 0.12$ substantially smaller than previously believed. A spin-flop Ising quantum phase transition occurs at a critical field of $\mu_0 H_b^{\rm cr} \approx 2$ T before around 3.5 T the description in terms of an effective spin-$\frac{1}{2}$ chain becomes inapplicable.Comment: 5 pages, 3 figure

Second harmonic generation on incommensurate structures: The case of multiferroic MnWO4

A comprehensive analysis of optical second harmonic generation (SHG) on an incommensurate (IC) magnetically ordered state is presented using multiferroic MnWO4 as model compound. Two fundamentally different SHG contributions coupling to the primary IC magnetic order or to secondary commensurate projections of the IC state, respectively, are distinguished. Whereas the latter can be described within the formalism of the 122 commensurate magnetic point groups the former involves a breakdown of the conventional macroscopic symmetry analysis because of its sensitivity to the lower symmetry of the local environment in a crystal lattice. Our analysis thus foreshadows the fusion of the hitherto disjunct fields of nonlinear optics and IC order in condensed-matter systems

Spin-orbit coupling in a half-filled t2gt_{2g} shell: the case of 5d35d^3 K2_2ReCl6_6

The half-filled $t_{2g}$ shell of the $t_{2g}^3$ configuration usually, in LS coupling, hosts a S = 3/2 ground state with quenched orbital moment. This state is not Jahn-Teller active. Sufficiently large spin-orbit coupling $\zeta$ has been predicted to change this picture by mixing in orbital moment, giving rise to a sizable Jahn-Teller distortion. In $5d^3$ K$_2$ReCl$_6$ we study the electronic excitations using resonant inelastic x-ray scattering (RIXS) and optical spectroscopy. We observe on-site intra-$t_{2g}$ excitations below 2 eV and corresponding overtones with two intra-$t_{2g}$ excitations on adjacent sites, the Mott gap at 2.7 eV, $t_{2g}$-to-$e_g$ excitations above 3 eV, and charge-transfer excitations at still higher energy. The intra-$t_{2g}$ excitation energies are a sensitive measure of $\zeta$ and Hund's coupling $J_H$. The sizable value of $\zeta \approx$ 0.29 eV places K$_2$ReCl$_6$ into the intermediate coupling regime, but $\zeta/J_H \approx 0.6$ is not sufficiently large to drive a pronounced Jahn-Teller effect. We discuss the ground state wavefunction in a Kanamori picture and find that the S = 3/2 multiplet still carries about 97 % of the weight. However, the finite admixture of orbital moment allows for subtle effects. We discuss small temperature-induced changes of the optical data and find evidence for a lowering of the ground state by about 3 meV below the structural phase transitions.Comment: 16 pages, 14 figure

Resonant inelastic x-ray incarnation of Young’s double-slit experiment

Young’s archetypal double-slit experiment forms the basis for modern diffraction techniques: The elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young’s experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns, which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba 3 CeIr 2 O 9 with structural Ir dimers and strong spin-orbit coupling. The double “slits” in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures

Stimulated Raman Scattering in Melilite‐Type Crystals Ca2MgSi2O7 and Ca2Ga2SiO7

χ(3)‐nonlinear optical interactions in two melilite‐type stimulated Raman scattering (SRS)‐active non‐centrosymmetric crystals, Ca2MgSi2O7 and Ca2Ga2SiO7, formerly known as Nd3+‐laser media, are presented. Under picosecond pumping at 1.064 and 0.532 µm cascaded and cross‐cascaded effects occur in these tetragonal silicates. Besides the SRS‐promoting phonon modes with energy of ωSRS1 ≈ 908 cm−1 and ωSRS2 ≈ 668 cm−1 for Ca2MgSi2O7, and ωSRS1 ≈ 720 cm−1 and ωSRS2 ≈ 550 cm−1 for Ca2Ga2SiO7, respectively, combined phonon modes are observed. For Ca2MgSi2O7 new data in a broad wavelength range of refractive indices and their dispersion are given as well. The observed χ(3)‐nonlinear properties expand the functionality of the studied silicates and foreshadow their use in self‐frequency Raman laser converters (self‐SRS lasers)