No Arabic abstract
We present a structural analysis of the substituted system (Ba$_{1-x}$Sr$_{x}$)CuSi$_{2}$O$_{6}$, which reveals a stable tetragonal crystal structure down to 1.5 K. We explore the structural details with lowtemperature neutron and synchrotron powder diffraction, room-temperature and cryogenic highresolution NMR, as well as magnetic- and specific-heat measurements and verify that a structural phase transition into the orthorhombic structure which occurs in the parent compound BaCuSi2O6, is absent for the x = 0.1 sample. Furthermore, synchrotron powder-diffraction patterns show a reduction of the unit cell for x = 0.1 and magnetic measurements prove that the Cu-dimers are preserved, yet with a slightly reduced intradimer coupling Jintra. Pulse-field magnetization measurements reveal the emergence of a field-induced ordered state, tantamount to Bose-Einsteincondensation (BEC) of triplons, within the tetragonal crystal structure of $I,4_{1}/acd$. This material offers the opportunity to study the critical properties of triplon condensation in a simple crystal structure.
We present a route to grow single crystals of Ba$_{0.9}$Sr$_{0.1}$CuSi$_{2}$O$_{6}$ suitable for inelastic neutron studies via the floating zone technique. Neutron single crystal diffraction was utilized to check their bulk quality and orientation. Finally, the high quality of the grown crystals was proven by X-ray diffraction and magnetic susceptibility.
In $A_{3}$Cr$_{2}$O$_{8}$, where $A$ = Sr or Ba, the Cr$^{5+}$ ions surrounded by oxygen ions in a tetrahedral coordination are Jahn-Teller active. The Jahn-Teller distortion leads to a structural transition and a related emergence of three twinned monoclinic domains below the structural phase transition. This transition is highly dynamic over an extended temperature range for $A$ = Sr. We have investigated mixed compounds Ba$_{3-x}$Sr$_{x}$Cr$_{2}$O$_{8}$ with $x=2.9$ and $x=2.8$ by means of X-ray and neutron diffraction, Raman scattering and calorimetry. Based on the obtained evolution of the phonon frequencies, we find a distinct suppression of the orbital-lattice fluctuation regime with increasing Ba content. This stands in contrast to the linear behaviour exhibited by unit cell volumes, atomic positions and intradimer spin-spin exchange interactions.
Ba$_3$Mn$_2$O$_8$ is a geometrically frustrated spin dimer compound. We investigate the effect of site disorder on the zero field phase diagram of this material by considering the solid solution Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$, where nonmagnetic V$^{5+}$ ions partially substitute magnetic Mn$^{5+}$ ions. This substitution results in unpaired $S=1$ moments for half-substituted dimers, which are ungapped and therefore susceptible to types of magnetic order not present in the parent compound. AC susceptibility measurements of compositions between $x=0.046$ and $x=0.84$ show a sharp frequency- and composition-dependent kink at temperatures below 210mK, suggesting that unpaired spins form a spin glass. The case for a glassy state is made clearer by the absence of any sharp features in the specific heat. However, Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$ is not a paradigmatic spin glass. Whereas both the freezing temperature and the Weiss temperature (determined from susceptibility above 1K) vary strongly as a function of composition, the heat capacity per unpaired spin is found to be insensitive (above the glass transition) to the density of unpaired spins for the broad regime $0.18leq x leq 0.84$. This surprising result is consistent with a scenario in which nearest-neighbor unpaired spins form local, possibly fluctuating, spin-singlets prior to the eventual spin freezing. The spin glass state is only found for temperatures below the energy scale of single-ion anisotropy, suggestive this plays a significant role in determining the eventual ground state. Possible ground states in the dilute limit ($x < 0.04$ and $x > 0.9$) are also discussed.
We report incommensurate diffuse (ICD) scattering appearing in the high-temperature-tetragonal (HTT) phase of La$_{2-x}$(Sr,Ba)$_{x}$CuO$_{4}$ with $0.07 leq x leq 0.20$ observed by the neutron diffraction technique. For all compositions, a sharp superlattice peak of the low-temperature-orthorhombic (LTO) structure is replaced by a pair of ICD peaks with the modulation vector parallel to the CuO$_6$ octahedral tilting direction, that is, the diagonal Cu-Cu direction of the CuO$_2$ plane, above the LTO-HTT transition temperature $T_s$. The temperature dependences of the incommensurability $delta$ for all samples scale approximately as $T/T_s$, while those of the integrated intensity of the ICD peaks scale as $(T-T_s)^{-1}$. These observations together with absence of ICD peaks in the non-superconducting $x=0.05$ sample evince a universal incommensurate lattice instability of hole-doped 214 cuprates in the superconducting regime.
Hidden magnetic order of Sr$_2$Ir$_{1-x}$Rh$_x$O$_4$, $x = 0.05$ and 0.1, has been studied using muon spin relaxation spectroscopy. In zero applied field and weak longitudinal fields ($mu_0H_L lesssim 2$~mT), muon spin relaxation data can be well described by exponentially-damped static Lorentzian Kubo-Toyabe functions, indicating that static and dynamic local fields coexist at each muon site. For $mu_0H_L gtrsim 2$~mT, the static rate is completely decoupled, and the exponential decay is due to dynamic spin fluctuations. In both zero field and $mu_0H_L = 1$--2~mT, the temperature dependencies of the exponential muon spin relaxation rate exhibit maxima at 215~K for $x = 0.05$ and 175~K for $x = 0.1$, suggesting critical slowing down of electronic spin fluctuations. The field dependencies of the dynamic spin fluctuation rates can be well described by the Redfield relation. The correlation time of this electronic spin fluctuation is in the range of~2--5~ns for Sr$_2$Ir$_{0.9}$Rh$_{0.1}$O$_4$, and shorter than 2~ns for Sr$_2$Ir$_{0.95}$Rh$_{0.05}$O$_4$. The rms fluctuating field is on the order of 1 mT, which is consistent with the polarized neutron diffraction cross-section.