Browsing by Author "Pshenychnyi, Roman"

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    Controlling structural instability in the Cu$_{12-x}$Ni$_x$Sb$_4$S$_{13}$ ($x$\,=\,0, 0.05, 0.2, 0.5) tetrahedrites
    (Technische Universität Bergakademie Freiberg, 2026-01-08) Bolielyi, Oleksandr; Dobrozhan, Oleksandr; Levytskyi, Volodymyr; Tsirlin, Alexander A.; Pshenychnyi, Roman; Leithe-Jasper, Andreas; Gumeniuk, Roman
    Cu$_{12-x}$Ni$_x$Sb$_4$S$_{13}$ ($x\,=\,0, 0.05, 0.2, 0.5$) tetrahedrites were synthesized by the polyol method. Measurements of magnetic susceptibility, specific heat capacity as well as electrical and thermal transport properties indicated a structural phase transition (SPT) of 1$^{\mathrm{st}}$ order at $T_k\,=\,75-85$\,K, which is accompanied by strong changes in electronic density of states (EDOS) and entropy for $x\,=\,0, 0.05, 0.2$ whereas only weak changes were observed at $x\,=\,0.5$. However, further temperature dependent synchrotron high-resolution powder X-ray diffraction (HR PXRD) studies indicated compounds with Ni-content $x\,=\,0$ and 0.5 to remain body-centered cubic [space group (SG) $I\bar{4}3m$, $a\,\approx\,10.4(1)$\,\AA] down to 10\,K, whereas crystal structures of $x\,=\,0, 0.05$ and 0.2 became tetragonal, (SG $P\bar{4}c2$, $a_\mathrm{tetr}\,\approx\,a_\mathrm{cub}\sqrt{2}$, $c_\mathrm{tetr}\,\approx\,a_\mathrm{cub}$) below $T_k$. Comparing changes of EDOS at the Fermi level [$\Delta N^{(E_\mathrm{F})}$] deduced from magnetic and thermodynamic data with those calculated from density functional theory (DFT) assuming the validity of the rigid-band approximation, we found $\Delta N^{(E_\mathrm{F})}_\mathrm{theor}\,\approx\,0$ when compared with cubic and tetragonal arragements for Cu$_{11.5x}$Ni$_{0.5}$Sb$_4$S$_{13}$, which indicate the latter to be unstable. This study shows that SPT in tetrahedites is facilitated by the presence of minor amount of a dopant.