The prototypical phase change material GeTe shows an enigmatic phase transition at Tc ca. 650 K from rhombohedral (R3m) to cubic (Fm-3m) symmetry. While local probes see little change in bonding, in contrast, average structure probes imply a displaci
ve transition. Here we use high energy X-ray scattering to develop a model consistent with both the local and average structure pictures. We detect a correlation length for domains of the R3m structure which shows power law decay upon heating. Unlike a classical soft mode, it saturates at ca. 20 {AA} above Tc. These nanoclusters are too small to be observed by standard diffraction techniques, yet contain the same local motif as the room temperature structure, explaining previous discrepancies. Finally, a careful analysis of the pair distribution functions implies that the 0.6 % negative thermal expansion (NTE) at the R3m -Fm-3m transition is associated with the loss of coherence between these domains.
We reinvestigate the pressure dependence of the crystal structure and antiferromagnetic phase transition in MnTe$_2$ by the rigorous and reliable tool of high pressure neutron powder diffraction. First-principles density functional theory calculation
s are carried out in order to gain microscopic insight. The measured Neel temperature of MnTe$_2$ is found to show unusually large pressure dependence of $12$ K GPa$^{-1}$. This gives rise to large violation of Blochs rule given by $alpha=frac{dlog T_N}{dlog V}=-frac{10}{3} approx -3.3$, to a $alpha$ value of -6.0 $pm$ 0.1 for MnTe$_2$. The ab-initio calculation of the electronic structure and the magnetic exchange interactions in MnTe$_2$, for the measured crystal structures at different pressures, gives the pressure dependence of the Neel temperature, $alpha$ to be -5.61, in close agreement with experimental finding. The microscopic origin of this behavior turns to be dictated by the distance dependence of the cation-anion hopping interaction strength.
The recent surge of interest in phase change materials GeTe, Ge$_2$Sb$_2$Te$_5$, and related compounds motivated us to revisit the structural phase transition in GeTe in more details than was done before. Rhombohedral-to-cubic ferroelectric phase tra
nsition in GeTe has been studied by high resolution neutron powder diffraction on a spallation neutron source. We determined the temperature dependence of the structural parameters in a wide temperature range extending from 309 to 973 K. Results of our studies clearly show an anomalous volume contraction of 0.6% at the phase transition from the rhombohedral to cubic phase. In order to better understand the phase transition and the associated anomalous volume decrease in GeTe we have performed phonon calculations based on the density functional theory. Results of the present investigations are also discussed with respect to the experimental data obtained for single crystals of GeTe.
We report the characterisation of natural samples of the cubic pyrite mineral MnS2 using very high resolution synchrotron X-ray diffraction techniques. At low temperatures we find a new low temperature polymorph, which results from coupling between m
agnetic and lattice degrees of freedom. Below the magnetic ordering temperature T_N= 48 K, we detect a pseudo-tetragonal distortion with a tiny c/a ratio of 1.0006. The structure can be refined in the space group Pbca. The symmetry lowering reduces magnetic frustration in the fcc Mn2+ lattice and is likely responsible for the previously reported lock-in of the magnetic propagation vector. This behaviour is similar to the frustration driven symmetry breaking reported in other three-dimensional Heisenberg magnets like the chromate spinels
We investigated the dispersion of nuclear spin waves in Nd$_2$CuO$_4$ by using neutron spin-echo spectroscopy at millikelvin temperatures. Our results show unambiguously the existence of dispersion of nuclear spin waves in Nd$_2$CuO$_4$ at T = 30 mK.
A fit of the dispersion data with the spin wave dispersion formula gave the Suhl-Nakamura interaction range to be of the order of 10 {AA}.
We report the results of inelastic neutron scattering investigation on the model antiferromagnet CoF$_2$ by time-of-flight neutron spectroscopy. We measured the details of the scattering function $S(Q,omega)$ as a function of temperature with two dif
ferent incident neutron wavelengths. The temperature and Q dependence of the measured scattering function suggests the presence of magnon-phonon coupling in almost all branches. The present results are in agreement with the strong magnetoelastic effects observed previously.
We investigated low energy nuclear spin excitations in the layered compound CoCl$_2$ by high resolution back-scattering neutron spectroscopy. We detected inelastic peaks at $E = 1.34 pm 0.03$ $mu$eV on both energy loss and energy sides of the central
elastic peak at $T = 2$ K. The energy of the inelastic peaks decrease with temperature continuously and become zero at $T_N approx 25$ K at which the two ielastic peaks merge with the central elastic peak. We interpret the low energy excitations to be due to the transition between hyperfine field split nuclear levels. The present data together with the data on other Co compounds show that the energy of the nuclear spin excitations of a number of compounds follow a linear relationship with the electronic magnetic moment of the Co ion whereas that of other compounds deviate appreciably from this linear behaviour. We ascribe this anomalous behaviour to the presence of unquenched orbital moments of the Co ions.
We report a combination of physical property and neutron scattering measurements for polycrystalline samples of the one-dimensional spin chain compound CoV2O6. Heat capacity measurements show that an effective S = 1/2 state is found at low temperatur
es and that magnetic fluctuations persist up to 6.Tn. Above Tn = 6.3 K, measurements of the magnetic susceptibility as a function of T and H show that the nearest neighbour exchange is ferromagnetic. In the ordered state, we have discovered a crossover from a metamagnet with strong fluctuations between 5 K and Tn to a state with a 1/3 magnetisation plateau at 2 < T < 5 K. We use neutron powder diffraction measurements to show that the AFM state has incommensurate long range order and inelastic time of flight neutron scattering to examine the magnetic fluctuations as a function of temperature. Above Tn, we find two broad bands between 3.5 and 5 meV and thermally activated low energy features which correspond to transitions within these bands. These features show that the excitations are deconfined solitons rather than the static spin reversals predicted for a uniform FM Ising spin chain. Below Tn, we find a ladder of states due to the confining effect of the internal field. A region of weak confinement below Tn, but above 5 K, is identified which may correspond to a crossover between 2D and 3D magnetic ordering.
