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Register a new userCrystal field effects in the zig-zag chain compound SrTm$_2$O$_4$
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Added by
Abhijit Bhat Kademane
Publication date
2021
fields
Physics
and research's language is
English
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SrTm$_2$O$_4$ has been investigated using heat capacity, magnetic susceptibility, magnetization in pulsed fields, and inelastic neutron scattering measurements. These results show that the system is highly anisotropic, has gapped low-energy dispersing magnetic excitations, and remains in a paramagnetic state down to 2K. Two theoretical crystal field models were used to describe the single-ion properties of SrTm$_2$O$_4$without any optimization procedures; a standard point-charge model and a Density Functional Theory (DFT) based model that uses Wannier functions. The DFT model was found to better describe the system at low energy by predicting a singlet ground state for one Tm site and a doublet for the second Tm site and anisotropy of second site Tm dominating the anisotropy of the system. Additionally, muon spin rotation/relaxation ($mu^+$psr) spectra reveal oscillations, typically a sign of long-range magnetic order. We attribute these observations to lattice distortion induced by muon implantation, causing renormalization of the gap size.
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Static magnetic susceptibility chi, ac susceptibility chi_{ac} and specific heat C versus temperature T measurements on polycrystalline samples of In2VO5 and chi and C versus T measurements on the isostructural, nonmagnetic compound In2TiO5 are reported. A Curie-Wiess fit to the chi(T) data above 175 K for In2VO5 indicates ferromagnetic exchange between V^{4+} (S = 1/2) moments. Below 150 K the chi(T) data deviate from the Curie-Weiss behavior but there is no signature of any long range magnetic order down to 1.8 K. There is a cusp at 2.8 K in the zero field cooled (ZFC) chi(T) data measured in a magnetic field of 100 Oe and the ZFC and field cooled (FC) data show a bifurcation below this temperature. The frequency dependence of the chi_{ac}(T) data indicate that below 3 K the system is in a spin-glass state. The difference Delta C between the heat capacity of In2VO5 and In2TiO5 shows a broad anomaly peaked at 130 K. The entropy upto 300 K is more than what is expected for S = 1/2 moments. The anomaly in Delta C and the extra entropy suggests that there may be a structural change below 130 K in In2VO5.
Theoretical studies have predicted the existence of topological magnons in honeycomb compounds with zig-zag antiferromagnetic (AFM) order. Here we report the discovery of zig-zag AFM order in the layered and non-centrosymmetric honeycomb nickelate Ni$_2$Mo$_3$O$_8$ through a combination of magnetization, specific heat, x-ray and neutron diffraction and electron paramagnetic resonance measurements. It is the first example of such order in an integer-spin non-centrosymmetric structure ($P$$_6$3$mc$). Further, each of the two distinct sites of the bipartite honeycomb lattice has a unique crystal field environment, octahedral and tetrahedral Ni$^{2+}$ respectively, enabling independent substitution on each sublattice. Replacement of Ni by Mg on the octahedral site suppresses the long range magnetic order and results in a weakly ferromagnetic state. Conversely, substitution of Fe for Ni enhances the AFM ordering temperature. Thus Ni$_2$Mo$_3$O$_8$ provides a platform on which to explore the rich physics of $S = 1$ on the honeycomb in the presence of competing magnetic interactions with a non-centrosymmetric, formally piezeo-polar, crystal structure.
The bulk single crystals of $S = 1$ chain compound Ni(C$_3$H$_{10}$N$_2$)$_2$NO$_2$ClO$_4$ are grown by using a slow evaporation method at a constant temperature and a slow cooling method. It is found that the optimum condition of growing large crystals is via slow evaporation at 25 $^circ$C using 0.015 mol Ni(ClO$_4$)$_2$$cdot$6H$_2$O, 0.015 mol NaNO$_2$, and 0.03 mol 1,3-propanediamine liquid dissolved into 30 ml aqueous solvent. High-quality crystals with size up to $18 times 7.5 times 5$ mm$^3$ are obtained. The single crystals are characterized by measurements of x-ray diffraction, magnetic susceptibility, specific heat and thermal conductivity. The susceptibilities along three crystallographic axes are found to exhibit broad peaks at $sim 55$ K, and then decrease abruptly to zero at lower temperatures, which is characteristic of a Haldane chain system. The specific heat and the thermal conductivity along the $c$ axis can be attributed to the simple phononic contribution and are analyzed using the Debye approximation.
We demonstrate that the onset of complex spin orders in ACr$_2$O$_4$ spinels with magnetic A$=$Co, Fe and Cu ions lowers the lattice symmetry. This is clearly indicated by the emergence of anisotropic lattice dynamics -- as evidenced by the pronounced phonon splittings -- even when experiments probing static distortions fail. We show that the crystal symmetry in the magnetic phase is reduced from tetragonal to orthorhombic for FeCr$_2$O$_4$ and CuCr$_2$O$_4$ with Jahn-Teller active A-site ions. The conical spin structure in FeCr$_2$O$_4$ is also manifested in the phonon frequencies. In contrast, the multiferroic CoCr$_2$O$_4$ with no orbital degrees of freedom remains nearly cubic in its ground state.
Pr$_2$Zr$_2$O$_7$ is a pyrochlore quantum spin-ice candidate. Using Raman scattering spectroscopy we probe crystal electric field excitations of Pr$^{3+}$, and demonstrate the importance of their interactions with the lattice. We identify a vibronic interaction with a phonon that leads to a splitting of a doublet crystal field excitation at around 55~meV. We also probe a splitting of the non-Kramers ground state doublet of Pr$^{3+}$ by observing a double line of the excitations to the first excited singlet state $E^0_g rightarrow A_{1g}$. We show that the splitting has a strong temperature dependence, with the doublet structure most prominent between 50~K and 100~K, and the weight of one of the components strongly decreases on cooling. We suggest a static or dynamic deviation of Pr$^{3+}$ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures.
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