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Register a new userTrue reentry of the glassy state in geometrically frustrated LiCr(1-x)Mn(x)O(2)
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The development of spin glass like state in a geometrically frustrated (GF) magnet is a matter of great debate. We investigated the effect of magnetic (Mn) and nonmagnetic (Ga) doping at the Cr site of the layered GF antiferromagnetic compound LiCrO2. 10% Ga doping at the Cr site does not invoke any metastability typical of a glassy magnetic state. However, similar amount of Mn doping certainly drives the system to a spin glass state which is particularly evident from the relaxation, magnetic memory and heat capacity studies. The onset of glassy state in 10% Mn doped sample is of reentrant type developing out of higher temperature antiferromagnetic state. The spin glass state in the Mn-doped sample shows a true reentry with the complete disappearance of the antiferromagnetic phase below the spin glass transition. Mn doping at the Cr site can invoke random ferromagnetic Cr-Mn bonds in the otherwise 120 degree antiferromagnetic triangular lattice leading to the non-ergodic spin frozen state. The lack of spin glass state on Ga doping indicates the importance of random ferromagnetic/antiferromagnetic bonds for the glassy ground state in LiCrO2. Spin glass state in GF system has been earlier observed even for small non-magnetic disorder, and our result indicates that the issue is quite nontrivial and depends strongly on the material system concerned.
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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.
Heavily doped Ba$_{1-x}$K$_{x}$Mn$_{2}$As$_{2}$ ($x$=0.19 and 0.26) single crystals were successfully grown, and investigated by the measurements of resistivity and anisotropic magnetic susceptibility. In contrast to the antiferromagnetic insulating ground state of the undoped BaMn$_{2}$As$_{2}$, the K-doped crystals show metallic conduction with weak ferromagnetism below $sim$50 K and Curie-Weiss-like in-plane magnetic susceptibility above $sim$50 K. Under high pressures up to 6 GPa, the low-temperature metallicity changes into a state characterized by a Kondo-like resistivity minimum without any signature of superconductivity above 2.5 K. Electronic structure calculations for $x$=0.25 using $2times2times1$ supercell reproduce the hole-doped metallic state. The density of states at Fermi energy have significant As 4$p$ components, suggesting that the 4$p$ holes are mainly responsible for the metallic conduction. Our results suggest that the interplay between itinerant 4$p$ holes and local 3$d$ moments is mostly responsible for the novel metallic state.
Magnetic fluctuations induced by geometric frustration of local Ir-spins disturb the formation of long range magnetic order in the family of pyrochlore iridates, R$_{2}$Ir$_{2}$O$_{7}$ (R = lanthanide)$^{1}$. As a consequence, Pr$_{2}$Ir$_{2}$O$_{7}$ lies at a tuning-free antiferromagnetic-to-paramagnetic quantum critical point and exhibits a diverse array of complex phenomena including Kondo effect, biquadratic band structure, metallic spin-liquid (MSL), and anomalous Hall effect$^{2-5}$. Using spectroscopic imaging with the scanning tunneling microscope, complemented with machine learning K-means clustering analysis, density functional theory, and theoretical modeling, we probe the local electronic states in single crystal of Pr$_{2}$Ir$_{2}$O$_{7}$ and discover an electronic phase separation. Nanoscale regions with a well-defined Kondo resonance are interweaved with a non-magnetic metallic phase with Kondo-destruction. Remarkably, the spatial nanoscale patterns display a correlation-driven fractal geometry with power-law behavior extended over two and a half decades, consistent with being in proximity to a critical point. Our discovery reveals a new nanoscale tuning route, viz. using a spatial variation of the electronic potential as a means of adjusting the balance between Kondo entanglement and geometric frustration.
Dielectric and magnetic properties have been studied for poly-crystalline samples of quasi-one-dimensional frustrated spin-1/2 system Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$(M=Ni and Zn) which does not exhibit a three-dimensional magnetic transition due to quantum spin fluctuation and low dimensionality. A broad peak in the magnetic susceptibility - temperature curves originated from a short range helical ordering at low temperature is suppressed by the Ni and Zn substitution for Cu sites. The capacitance is found to anomalously increase with decreasing T below ~50 K, which is also suppressed by the impurity doping. The behavior of the anomalous capacitance component is found to be strongly connected with that of the magnetic susceptibility for Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$ which indicates that the low-temperature dielectric response is driven by the magnetism.
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.
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