Brillouin and neutron scattering study of hexagonal ABX3 ternary halides
thesisposted on 10.04.2013 by Dayang M.A. Hashim
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The interest in one dimensional (1D) magnetism has been strongly renewed with the synthesis of many magnetic compounds which exhibit a quasi one dimensional magnetic behaviour. One of the peculiarities of this 1D system is the absence of a long range magnetic ordered phase at any finite temperature for the ideal 1D system with short range interaction. Tetramethylammonium manganese chloride (CH3)4NMnCl3(TMMC) exhibits the properties of an ideal one dimensional antiferromagnets for temperature above 1 K, the transition to a three dimensional (3D) long range ordered state only occurs at 0.84K. In addition to its magnetic transition, TMMC exhibits structural phase transition due to the ordering of the tetramethylammonium (TMA) ions which makes also this compound very attractive from a lattice dynamical point of view. Structural phase transitions of tetramethylammonium manganese chloride (TMMC), tetramethylammonium manganese bromide (TMMB) and tetramethylammonium manganese chloride doped with 8% Cu (TMMC:Cu) of the hexagonal type compounds are investigated using the Brillouin scattering method. These crystals show pronounced acoustic anomalies in the region of the structural phase transition. The acoustic anomalies were observed by measuring sound velocity and hence the elastic constant can be deduced. The phase transition temperatures were observed at 129.6K and 388.6K (TMMC), 114.6K and 377.6K (TMMB) and at 108.6K and 359.6K (TMMC:Cu). The elastic constant at room temperature were C11 = 2.10 (TMMC) and C11 = 1.59 (TMMB) in units of 1010 Nm-2. The phase transition of these compounds were further investigated macroscopically using the Differential Scanning Calorimetry (DSC) method. Activation energies of TMMC, TMMC:Cu, TMMB and deuterated TMMB at the phase transition were determined using this method. The values are 70.612 kJ/mol (TMMC), 49.224 kJ/mol (TMMC:Cu), 51.747 kJ/mol (TMMB) and 69.909 kJ/mol (d12-TMMB). The elastic constant of the linear chain antiferromagnet CsNiCl3 and RbNiCl3 was also determined using the Brillouin scattering method. The room temperature measurements give C11 = 3.77 (3.71) and C33 = 5.62 (5.42) in units of 1010 Nm·2 for CsNiCl3 and RbNiCl3 respectively. The phonon dispersion curves at room temperature in the hexagonal CsFeBr3 have been studied using the inelastic neutron scattering technique. From the initial slope of the dispersion curve, the sound velocity was deduced which enable us to calculate the elastic constant of CsFeBr3 at room temperature. The values obtained are C11 = 7.33, C66 = 1.01, C33 = 2.58 and C44 = 0.56 in units of 1010 Nm·2.