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Register a new userQuasi-2D magnetic correlations in Ni$_2$P$_2$S$_6$ probed by ${}^{31}$P NMR
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Detailed ${}^{31}$P nuclear magnetic resonance (NMR) measurements are presented on well-characterized single crystals of antiferromagnetic van der Waals Ni$_2$P$_2$S$_6$. An anomalous breakdown is observed in the proportionality of the NMR shift $K$ with the bulk susceptibility $chi$. This so-called $K$$-$$chi$ anomaly occurs in close proximity to the broad peak in $chi(T)$, thereby implying a connection to quasi-2D magnetic correlations known to be responsible for this maximum. Quantum chemistry calculations show that crystal field energy level depopulation effects cannot be responsible for the $K$$-$$chi$ anomaly. Appreciable in-plane transferred hyperfine coupling is observed, which is consistent with the proposed Ni$-$S$-$Ni super- and Ni$-$S$-$S$-$Ni super-super-exchange coupling mechanisms. Magnetization and spin$-$lattice relaxation rate ($T_1^{-1}$) measurements indicate little to no magnetic field dependence of the Neel temperature. Finally, $T_1^{-1}(T)$ evidences relaxation driven by three-magnon scattering in the antiferromagnetic state.
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We report an optimized chemical vapor transport method to grow single crystals of (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ where x = 0, 0.3, 0.5, 0.7 & 1. Single crystals up to 4,mm,$times$,3,mm,$times$,200,$mu$m were obtained by this method. As-grown crystals characterized by means of scanning electron microscopy, and powder x-ray diffraction measurements. The structural characterization shows that all crystals crystallize in monoclinic symmetry with the space group $C2/m$ (No. 12). We have further investigated the magnetic properties of this series of single crystals. The magnetic measurements of the all as-grown single crystals show long-range antiferromagnetic order along all crystallographic principal axes. Overall, the Neel temperature TN is non-monotonous, with increasing $Ni^{2+}$ doping the temperature of the antiferromagnetic phase transition first decreases from 80 K for pristine Mn$_2$P$_2$S$_6$ (x = 0) up to x = 0.5, and then increases again to 155 K for pure Ni$_2$P$_2$S$_6$ (x = 1). The magnetic anisotropy switches from out-of-plane to in-plane as a function of composition in (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ series. Transport studies under hydrostatic pressure on the parent compound Mn$_2$P$_2$S$_6$ evidence an insulator-metal transition at an applied critical pressure of ~22 GPa
We report our nuclear magnetic resonance (NMR) study on the structurally spin chain compound Ni$_2$NbBO$_6$ with complex magnetic coupling. The antiferromagnetic transition is monitored by the line splitting resulting from the staggered internal hyperfine field. The magnetic coupling configuration proposed by the first-principle density functional theory (DFT) is supported by our NMR spectral analysis. For the spin dynamics, a prominent peak at $Tsim35$ K well above the N{e}el temperature ($T_Nsim20$ K at $mu_0H=10$ T) is observed from the spin-lattice relaxation data. As compared with the dc-susceptibility, this behavior indicates a antiferromagnetic coupling with the typical energy scale of $sim3$ meV. Thus, the Ni$_2$NbBO$_6$ compound can be viewed as strongly ferromagnetically coupled armchair spin chains along the crystalline $b$-axis. These facts place strong constraints to the theoretical model for this compound.
We report $^{31}$P NMR measurements under various magnetic fields up to 7 T for the intermediate valence compound EuNi$_2$P$_2$, which shows heavy electronic states at low temperatures. In the high-temperature region above 40 K, the Knight shift followed the Curie--Weiss law reflecting localized $4f$ states. In addition, the behavior corresponding to the temperature variation of the average valence of Eu was observed in the nuclear spin-lattice relaxation rate $1/T_1$. With the occurrence of the Kondo effect, $1/T_1$ was clearly reduced below 40 K, and the Knight shift becomes almost constant at low temperatures. From these results, the formation of heavy quasiparticles by the hybridization of Eu $4f$ electrons and conduction electrons was clarified from microscopic viewpoints. Furthermore, a characteristic spin fluctuation was observed at low temperatures, which would be associated with valence fluctuations caused by the intermediate valence state of EuNi$_2$P$_2$.
The valence fluctuations which are related to the charge disproportionation of phosphorous ions $P^{4+} + P^{4+}rightarrow P^{3+} + P^{5+}$ are the origin of ferroelectric and quantum paraelectric states in Sn(Pb)$_2$P$_2$S$_6$ semiconductors. They involve recharging of SnPS$_3$ or PbPS$_3$ structural groups which could be represented as half-filled sites in the crystal lattice. Temperature-pressure phase diagram for Sn$_2$P$_2$S$_6$ compound and temperature-composition phase diagram for (Pb$_y$Sn$_{1-y}$)$_2$P$_2$S$_6$ mixed crystals, which include tricritical points and where a temperature of phase transitions decrease to 0 K, together with the data about some softening of low energy optic phonons and rise of dielectric susceptibility at cooling in quantum paraelectric state of Pb$_2$P$_2$S$_6$, are analyzed by GGA electron and phonon calculations and compared with electronic correlations models. The anharmonic quantum oscillators model is developed for description of phase diagrams and temperature dependence of dielectric susceptibility.
We report a systematic NMR study on [Sr$_4$Sc$_2$O$_6$]Fe$_2$(As$_{1-x}$P$_x$)$_2$, for which the local lattice parameters of the iron-pnictogen (Fe$Pn$) layer are similar to those of the series LaFe(As$_{1-x}$P$_{x}$)O, which exhibit two segregated antiferromagnetic (AFM) order phases, AFM1 at $x$=0-0.2 and AFM2 at $x$=0.4-0.7. Our results revealed that the parent AFM1 phase at $x$=0 disappears at $x$=0.3-0.4, corresponding to a pnictogen height ($h_{pn}$) from the Fe-plane of 1.3-1.32 AA, which is similar to that of LaFe(As$_{1-x}$P$_{x}$)O and various parent Fe-pnictides. By contrast, the AFM2 order reported for LaFe(As$_{0.4}$P$_{0.6}$)O does not appear at $xsim$0.8, although the local lattice parameters of the Fe$Pn$ layer and the microscopic electronic states are quite similar. Despite the absence of the {it static} AFM2 order, reemergent {it dynamical} AFM spin fluctuations were observed at approximately $xsim$0.8, which can be attributed to the instability of the AFM2 phase. We suggest this re-enhancement of AFM spin fluctuations to play a significant role in enhancing the $T_c$ to 17 K for $x$=0.8-1. Finally, we discuss the universality and diversity of the complicated magnetic ground states from a microscopic point of view, including the difference in the origins of the AFM1 and AFM2 phases, and their relations with the high superconducting transitions in Fe-pnictides.
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