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Phonons in the multiferroic langasite Ba$\_3$NbFe$\_3$Si$\_2$O$\_{14}$ : evidences for symmetry breaking  [PDF]
C Toulouse,M Cazayous,S De Brion,F Levy-Bertrand,H Barkaoui,P Lejay,L Chaix,M. B. Lepetit,J. B. Brubach,P Roy
Physics , 2015, DOI: 10.1103/PhysRevB.92.104302
Abstract: The chiral langasite Ba$\_3$NbFe$\_3$Si$\_2$O$\_{14}$ is a multiferroic compound. While its magnetic order below T$\_N$=27 K is now well characterised, its polar order is still controversial. We thus looked at the phonon spectrum and its temperature dependence to unravel possible crystal symmetry breaking. We combined optical measurements (both infrared and Raman spectroscopy) with ab initio calculations and show that signatures of a polar state are clearly present in the phonon spectrum even at room temperature. An additional symmetry lowering occurs below 120~K as seen from emergence of softer phonon modes in the THz range. These results confirm the multiferroic nature of this langasite and open new routes to understand the origin of the polar state.
Helical spin-waves, magnetic order, and fluctuations in the langasite compound Ba3NbFe3Si2O14  [PDF]
C. Stock,L. C. Chapon,A. Schneidewind,Y. Su,P. G. Radaelli,D. F. McMorrow,A. Bombardi,N. Lee,S. -W. Cheong
Physics , 2010, DOI: 10.1103/PhysRevB.83.104426
Abstract: We have investigated the spin fluctuations in the langasite compound Ba3NbFe3Si2O14 in both the ordered state and as a function of temperature. The low temperature magnetic structure is defined by a spiral phase characterized by magnetic Bragg peaks at q=(0,0,tau ~ 1/7) onset at TN=27 K as previously reported by Marty et al. The nature of the fluctuations and temperature dependence of the order parameter is consistent with a classical second order phase transition for a two dimensional triangular antiferromagnet. We will show that the physical properties and energy scales including the ordering wavevector, Curie-Weiss temperature, and the spin-waves can be explained through the use of only symmetric exchange constants without the need for the Dzyaloshinskii-Moriya interaction. This is accomplished through a set of ``helical" exchange pathways along the c direction imposed by the chiral crystal structure and naturally explains the magnetic diffuse scattering which displays a strong vector chirality up to high temperatures well above the ordering temperature. This illustrates a strong coupling between magnetic and crystalline chirality in this compound.
Chiral spin-wave excitations of the spin-5/2 trimers in the langasite compound Ba3NbFe3Si2O14  [PDF]
Jens Jensen
Physics , 2011, DOI: 10.1103/PhysRevB.84.104405
Abstract: The inelastic scattering of neutrons from magnetic excitations in the antiferromagnetic phase of the langasite compound Ba3NbFe3Si2O14 is analyzed theoretically. In the calculations presented, the strongly coupled spin-5/2 Fe triangles are accounted for as trimerized units. The weaker interactions between the trimers are included within the mean-field/random-phase approximation. The theory is compared with linear spin-wave theory, and a model is developed which leads to good agreement with the published results from unpolarized and polarized neutron-scattering experiments.
Effect of divalent Ba cation substitution with Sr on coupled multiglass state in the magnetoelectric multiferroic compound Ba3NbFe3Si2O14  [PDF]
Satyapal Singh Rathore,Satish Vitta
Physics , 2014, DOI: 10.1038/srep09751
Abstract: (Ba/Sr)3NbFe3Si2O14 is a magnetoelectric multiferroic with an incommensurate antiferromagnetic spiral magnetic structure which induces electric polarization at 26 K. The structure, as revealed by x-rays and neutrons, as well as static and dynamic magnetic and dielectric properties of these compounds have been studied down to 6 K under different conditions. Both the compounds have similar crystal structure but with different lattice constants down to 6 K. The Ba-and Sr-compounds exhibit a transition at 26 K and 25 K respectively, as indicated by the specific heat capacity and dc specific magnetization, into an antiferromagnetic state. Although Ba and Sr are isovalent, they exhibit very different static and dynamic magnetic behavior. The Ba-compound exhibits both thermal and magnetic field hysteresis with the thermal hysteresis decreasing with increasing magnetic field, a behavior typical of glasses. The glassy behavior is also clearly seen in the ac susceptibility studies which show a dispersive peak in the range 40 K to 90 K in the frequency range 10^1 Hz to 10^4 Hz. The dispersive behavior follows a cluster glass critical slowing dynamics with a freezing temperature of 35 K and a critical exponent of 3.9, a value close to the 3-D Ising model. The Sr-compound however does not exhibit any dispersive behavior except for the invariant transition at 25 K in ac susceptibility with no magnetic field hysteresis at all temperatures. The dielectric constant studied in the frequency range 10^1 Hz to 10^6 Hz also reflects the magnetic behavior of the two compounds. The Ba-compound has two distinct dispersive peaks near TN and in the range 40 K to 125 K while the Sr-compound has a single dispersive peak in the range 40 K to 80 K. The activation energy of the high temperature dispersive peak in both compounds however is found to be similar, 71 meV and 65 meV respectively for Ba- and Sr-compounds.
Impurity and spin effects on the magneto-spectroscopy of a THz-modulated nanostructure  [PDF]
Vidar Gudmundsson,Chi-Shung Tang,Andrei Manolescu
Physics , 2003, DOI: 10.1103/PhysRevB.68.165343
Abstract: We present a grid-free DFT model appropriate to explore the time evolution of electronic states in a semiconductor nanostructure. The model can be used to investigate both the linear and the nonlinear response of the system to an external short-time perturbation in the THz regime. We use the model to study the effects of impurities on the magneto-spectroscopy of a two-dimensional electron gas in a nanostructure excited by an intense THz radiation. We do observe a reduction in the binding energy of the impurity with increasing excitation strength, and at a finite magnetic field we find a slow onset of collective spin-oscillations that can be made to vanish with a stronger excitation.
Molecular Orientation by Intense Single Cycle THz Pulses  [PDF]
Sharly Fleischer,Yan Zhou,Robert W. Field,Keith A. Nelson
Physics , 2011, DOI: 10.1103/PhysRevLett.107.163603
Abstract: Intense single-cycle THz pulses resonantly interacting with molecular rotations are shown to induce significant field-free orientation under ambient conditions. We calculate and measure the angular distribution associated with THz-driven rotational motion and correlate the THz-induced orientation and alignment in an OCS gas sample.
Magneto-elastic couplings in the distorted diamond-chain compound azurite  [PDF]
Pham Thanh Cong,Bernd Wolf,Rudra Sekhar Manna,Ulrich Tutsch,Mariano de Souza,Andreas Brühl,Michael Lang
Physics , 2014, DOI: 10.1103/PhysRevB.89.174427
Abstract: We present results of ultrasonic measurements on a single crystal of the distorted diamond-chain compound azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$. Pronounced elastic anomalies are observed in the temperature dependence of the longitudinal elastic mode $c_{22}$ which can be assigned to the relevant magnetic interactions in the system and their couplings to the lattice degrees of freedom. From a quantitative analysis of the magnetic contribution to $c_{22}$ the magneto-elastic coupling $G$ = $\partial J_2$/$\partial \epsilon_b$ can be determined, where $J_2$ is the intra-dimer coupling constant and $\epsilon_b$ the strain along the intra-chain $b$ axis. We find an exceptionally large coupling constant of $|G| \sim ($3650 $\pm$ 150) K highlighting an extraordinarily strong sensitivity of $J_2$ against changes of the $b$-axis lattice parameter. These results are complemented by measurements of the hydrostatic pressure dependence of $J_2$ by means of thermal expansion and magnetic susceptibility measurements performed both at ambient and finite hydrostatic pressure. We propose that a structural peculiarity of this compound, in which Cu$_2$O$_6$ dimer units are incorporated in an unusually stretched manner, is responsible for the anomalously large magneto-elastic coupling.
Parity Broken Chiral Spin Dynamics in Ba$_3$NbFe$_3$Si$_2$O$_{14}$  [PDF]
Mickael Loire,Virginie Simonet,Sylvain Petit,Karol Marty,Pierre Bordet,Pascal Lejay,Jacques Ollivier,Mechthild Enderle,Paul Steffens,Eric Ressouche,Andrej Zorko,Rafik Ballou
Physics , 2010, DOI: 10.1103/PhysRevLett.106.207201
Abstract: The spin wave excitations emerging from the chiral helically modulated 120$^{\circ}$ magnetic order in a langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ enantiopure crystal were investigated by unpolarized and polarized inelastic neutron scattering. A dynamical fingerprint of the chiral ground state is obtained, singularized by (i) spectral weight asymmetries answerable to the structural chirality and (ii) a full chirality of the spin correlations observed over the whole energy spectrum. The intrinsic chiral nature of the spin waves elementary excitations is shown in absence of macroscopic time reversal symmetry breaking.
Single domain magnetic helicity and triangular chirality in structurally enantiopure Ba3NbFe3Si2O14  [PDF]
Karol Marty,Virginie Simonet,Eric Ressouche,Rafik Ballou,Pascal Lejay,Pierre Bordet
Physics , 2008, DOI: 10.1103/PhysRevLett.101.247201
Abstract: A novel doubly chiral magnetic order is found out in the structurally chiral langasite compound Ba$_3$NbFe$_3$Si$_2$O$_{14}$. The magnetic moments are distributed over planar frustrated triangular lattices of triangle units. On each of these they form the same triangular configuration. This ferro-chiral arrangement is helically modulated from plane to plane. Unpolarized neutron scattering on a single crystal associated with spherical neutron polarimetry proved that a single triangular chirality together with a single helicity is stabilized in an enantiopure crystal. A mean field analysis allows discerning the relevance on this selection of a twist in the plane to plane supersuperexchange paths.
Finite Rotations  [PDF]
Oscar Bolina,J. A. da Silva Neto
Physics , 1998, DOI: 10.1119/1.879944
Abstract: We present an elementary discussion of two basic properties of angular displacements, namely, the anticommutation of finite rotations and the commutation of infinitesimal rotations, and show how commutation is achieved as the angular displacements get smaller and smaller.
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