We report detailed 51V NMR spectra in a single crystal of MnV2O4. The vanadium spectrum reveals two peaks in the orbitally ordered state, which arise from different internal hyperfine fields at two different V sublattices. These internal fields evolve smoothly with externally applied field, and show no change in structure that would suggest a change of the orbital ordering. The result is consistent with the orbital ordering model recently proposed by Sarkar et al. [Phys. Rev. Lett. 102, 216405 (2009)] in which the same orbital that is a mixture of t_2g orbitals rotates by about 45$^\circ$ alternately within and between orbital chains in the I4_1/a tetragonal space group.
SrEr2O4 is a geometrically frustrated magnet which demonstrates rather unusual properties at low temperatures including a coexistence of long- and short-range magnetic order, characterized by two different propagation vectors. In the present work, the effects of crystal fields (CF) in this compound containing four magnetically inequivalent erbium sublattices are investigated experimentally and theoretically. We combine the measurements of the CF levels of the Er3+ ions made on a powder sample of SrEr2O4 using neutron spectroscopy with site-selective optical and electron paramagnetic resonance …
We report results of 27Al-NMR measurements on a single crystal of PrTi2Al20, in which the ground state of Pr3+ ions in the crystalline electric field is the nonmagnetic Gamma3 doublet. From the analysis of NMR spectra with the magnetic field applied precisely along the <111> and <100> directions, we determined the electric field gradient tensors for all three inequivalent Al sites (Al(1) ~ Al(3) sites) and the anisotropic Knight shifts for the Al(3) sites. The hyperfine coupling tensor at the Al(3) sites is strongly anisotropic and much larger than the classical dipolar coupling, indication im…
We report ^{13}C NMR spectra and nuclear spin lattice relaxation rate 1/T_1 for a quasi-one-dimensional quarter-filled organic material (TMTTF)_{2}AsF_{6}, which undergoes charge ordering (T_{CO} = 102 K) and spin-Peierls phase transitions (T_{SP} = 14 K). The ratio of two 1/T_1 for the charge accepting and donating TMTTF sites which grows from T_{CO} finally saturates in approaching T_{SP}, indicating one spin correlation function even in the charge ordered state. Below T_{SP}, however, the doubly split NMR lines from inequivalently charged molecules merge into one line, originated from the v…
Local spin and charge properties were studied on beta-Ag0.33V2O5, a pressure-induced superconductor, at ambient pressure using 51V-NMR and zero-field-resonance (ZFR) techniques. Three inequivalent Vi sites (i=1, 2, and 3) were identified from 51V-NMR spectra and the principal axes of the electric-field-gradient (EFG) tensor were determined in a metallic phase and the following charge-ordering phase. We found from the EFG analysis that the V1 sites are in a similar local environment to the V3 sites. This was also observed in ZFR spectra as pairs of signals closely located with each other. These…
We report $^{153}$Eu and $^{69,71}$Ga NMR under a zero magnetic field on the antiferromagnetic state of EuGa$_{4}$ with $T_{\rm{N}}\approx 16$ K. We have successfully observed a $^{153}$Eu zero-field NMR signal with well-resolved nuclear quadrupole splitting in the antiferromagnetic state of EuGa$_{4}$. $^{69,71}$Ga zero-field NMR spectra were also observed below $T_{\rm{N}}$. The internal field and nuclear quadrupole frequency are estimated from a simulation of the spectra by the exact diagonalization of the nuclear spin Hamiltonian matrix. The asymmetrically split zero-field NMR spectra were…
We report $^{125}$Te and $^{63,65}$Cu nuclear magnetic resonance (NMR) studies on single crystals of staircase Kagomé antiferromagnet PbCu3TeO7 ($T_{N1}\approx$ 36 K). A Curie constant as large as $Θ$~140 K is obtained by a Curie-Weiss fitting of the high-temperature Knight shift. The frustration factor f (= $Θ/T_N $)$\approx$ 4 implies intermediate frustration in this system. From the high-temperature Knight shift data of $^{125}$Te, its hyperfine coupling constant is estimated to be $^{125}A_{hf}$ = -67 kOe/$μ_B$, which suggests a strong interlayer coupling bridging the neighboring Kagomé la…
While standard heavy fermion metals feature a single spin-1/2 local moment per unit cell, more complicated systems with multiple distinct local moments have been synthesized as well, with Ce_3Pd_20(Si,Ge)_6 being one example. Here, we discuss the physics of a Kondo lattice model with two local-moment sublattices, coupled with different Kondo couplings to conduction electrons. The phase diagram will be strongly modified from that of the standard Kondo lattice if the characteristic screening temperatures of the distinct moments are well separated. Therefore, we investigate the interplay between …
We report a detailed study of the ground state helical magnetic structure in monophosphide FeP by means of ${}^{31}$P NMR spectroscopy. We show that the zero-field NMR spectrum of the polycrystalline sample provides strong evidence of an anisotropic distribution of local magnetic fields at the P site with substantially lower anharmonicity than that found at the Fe site by Mössbauer spectroscopy. From field-sweep ${}^{31}$P NMR spectra we conclude that a continuous spin-reorientation transition occurs in an external magnetic field range of 4 - 7 T, which is also confirmed by specific-heat measu…
Nuclear magnetic resonance (NMR) of 31P and 51V nuclei has been measured in a spin-1/2 alternating-chain compound (VO)_2P_2O_7. By analyzing the temperature variation of the 31P NMR spectra, we have found that (VO)_2P_2O_7 has two independent spin components with different spin-gap energies. The spin gaps are determined from the temperature dependence of the shifts at 31P and 51V sites to be 35 K and 68 K, which are in excellent agreement with those observed in the recent inelastic neutron scattering experiments [A.W. Garrett et al., Phys. Rev. Lett. 79, 745 (1997)]. This suggests that (VO)_2P…
We report a complete set of $^{59}$Co NMR data taken on the $x=2/3$ phase of sodium cobaltates Na$_{x}$CoO$_{2}$, for which we have formerly established the in plane Na ordering and its three dimensional stacking from a combination of symmetry arguments taken from Na and Co NQR/NMR data. Here we resolve all the parameters of the Zeeman and quadrupolar Hamiltonians for all cobalt sites in the unit cell and report the temperature dependencies of the NMR shift and spin lattice relaxation $T_{1}$ data for these sites. We confirm that three non-magnetic Co$^{3+}$ (Co1) are in axially symmetric posi…
23Na NMR spectrum measurements in alpha'-NaV2O5 with a single- crystalline sample are reported. In the charge-ordered phase, the number of inequivalent Na sites observed is more than that expected from the low-temperature structures of space group Fmm2 reported so far. This disagreement indicates that the real structure including both atomic displacement and charge disproportionation is of lower symmetry. It is suggested that zigzag ordering is the most probable. The temperature variation of the NMR spectra near the transition temperature is incompatible with that of second-order transitions. …
MnWO4 is regarded as a canonical example of multiferroic materials, where the multiferroic activity is caused by a spin-spiral alignment. We argue that, in reality, MnWO4 has two sources of the spin-spirality, which conflict with each other. One is the Dzyaloshinskii-Moriya (DM) interactions, reflecting the P2/c symmetry of the lattice. The P2/c structure of MnWO4 has an inversion center, that connects two Mn sublattices. Therefore, from the viewpoint of DM interactions, different Mn sublattices are expected to have opposite spin chirality. Another source is competing isotropic exchange intera…
NMR, muSR, magnetization and specific heat measurements in Li(2)VOSiO(4) powders and single crystals are reported. Specific heat and magnetization measurements evidence that Li(2)VOSiO(4) is a frustrated two-dimensional S=1/2 Heisenberg antiferromagnet on a square lattice with a superexchange coupling J_1, along the sides of the square, almost equal to J_2, the one along the diagonal ($J_2/J_1=1.1\pm 0.1$ with $J_2 + J_1 = 8.2\pm 1$ K). At $T_c\simeq 2.8$ K a phase transition to a low temperature collinear order is observed. T_c and the sublattice magnetization, derived from NMR and muSR, were…
The static and dynamic properties of V^{4+} spins (S = 1/2) in the frustrated square lattice compound Pb2(VO)(PO4)2 were investigated by means of magnetic susceptibility chi and 31P nuclear magnetic resonance (NMR) shift (K) and 31P nuclear spin-lattice relaxation rate 1/T1 measurements on a single crystal. This compound exhibits long-range antiferromagnetic order below TN \simeq 3.65 K. NMR spectra above TN show two distinct lines corresponding to two inequivalent P sites present in the crystal structure. The observed asymmetry in hyperfine coupling constant for the in-plane (P1) P site direc…
$^{31}$P nuclear magnetic resonance (NMR) measurements have been carried out to investigate the magnetic properties and spin dynamics of Fe$^{3+}$ ($S$ = 5/2) spins in the two-dimensional triangular lattice (TL) compound Na$_3$Fe(PO$_4$)$_2$. The temperature ($T$) dependence of nuclear spin-lattice relaxation rates ($1/T_1$) shows a clear peak around Néel temperature, $T_{\rm N} = 10.9$~K, corresponding to an antiferromagnetic (AFM) transition. From the temparature dependence of NMR shift ($K$) above $T_{\rm N}$, an exchange coupling between Fe$^{3+}$ spins was estimated to be $J/k_{\rm B}\sim…
Non-Fermi-liquid (NFL) behavior in the f-sublattice-diluted alloy system U_{1-x}Th_xPd_2Al_3 has been studied using ^{27}Al nuclear magnetic resonance (NMR). Impurity satellites due to specific U near-neighbor configurations to ^{27}Al sites are clearly resolved in both random and field-aligned powder samples. The spatial mean Kbar and rms spread delta K of impurity satellite shifts, which are related to the mean chibar and rms spread delta chi of the inhomogeneous susceptibility, have been measured in field-aligned powders with the crystalline c axis both perpendicular and parallel to the ext…
We report a x-ray resonant diffraction study of the perovskite Pr0.6Ca0.4MnO3. At the Mn K-edge, this technique is sensitive to details of the electronic structure of the Mn atoms. We discuss the resonant x-ray spectra measured above and below the charge and orbital ordering phase transition temperature (TCOO = 232 K), and present a detailed analysis of the energy and polarization dependence of the resonant scattering. The analysis confirms that the structural transition is a transition to an orbitally ordered phase in which inequivalent Mn atoms are ordered in a CE-type pattern. The Mn atoms …
CeRh$_2$As$_2$, a non-symmorphic heavy fermion material, was recently reported to host a remarkable phase diagram with two superconducting phases. In this material, the two inequivalent Ce sites per unit cell, related by inversion symmetry, introduce a sublattice structure corresponding to an extra internal degree of freedom. Here we propose a classification of the possible superconducting states in CeRh$_2$As$_2$ from the two Ce-sites perspective. Based on the superconducting fitness analysis and the quasiclassical Eilenberger equations, we discuss two limits: Rashba spin-orbit coupling and i…
Novel Quantum Spin Liquid States in the $S = {\frac{1}{2}}$ Three-Dimensional Compound Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$
Indian Institute of Technology Bombay（印度理工学院孟买分校）；Indian Association for the Cultivation of Science（印度科学培育协会）；University of Augsburg（奥格斯堡大学）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Indian Institute of Science Education and Research, Pune（印度科学与教育研究院浦那分校）；STFC Rutherford Appleton Laboratory（STFC卢瑟福阿普尔顿实验室）
The invariant form of the hyperfine interaction between multipolar moments and the nuclear spin is derived, and applied to discuss possibilities to identify the antiferro-octupolar (AFO) moments by NMR experiments. The ordered phase of NpO$_{2}$ and the phase IV of Ce$_{1-x}$La$_{x}$B$_{6}$ are studied in detail. Recent $^{17}$O NMR for polycrystalline samples of NpO$_{2}$ are discussed theoretically from our formulation. The observed feature of the splitting of $^{17}$O NMR spectrum into a sharp line and a broad line, their intensity ratio, and the magnetic field dependence of the shift and o…
A $^{125}$Te nuclear magnetic resonance (NMR) study was carried out in the paramagnetic state of the recently discovered quasi-one-dimensional spin-1 chain compound NiTe$_2$O$_5$. We observed that the $^{125}$Te NMR spectrum splits into two in a magnetic field applied along the $c$ axis. Based on the strong temperature variation of the relative intensity ratio of the split lines, we infer that the line splitting arises from the two sublattice susceptibilities induced in opposite directions along the chains. In great support of this interpretation, a quantitative analysis of the spin-lattice re…
We report nuclear magnetic resonance (NMR) studies in the antiferromagnetic state of the quasi-two-dimensional (CuBr)LaNb2O7. The NMR spectra at zero magnetic field and 4.2 K indicate a unique Cu and Br sites with an internal field of 5.7 T (at Cu) and 16.4 T (at Br), confirming a magnetic order. For the large internal field at the Br sites to be compatible with the collinear antiferromagnetic order observed by neutron diffraction experiments (N. Oba et al., J. Phys. Soc. Jpn. 75, (2006) 113601), the Br atoms must move significantly off the center of the square of the Cu sublattice so that the…
Using one- and two-dimensional NMR spectroscopy applied to $^{13}$C spin-labeled (TMTTF)$_2$AsF$_6$ and (TMTTF)$_2$PF$_6$, we demonstrate the existence of an intermediate charge-ordered phase in the TMTTF family of charge-transfer salts. At ambient temperature, the spectra are characteristic of nuclei in equivalent environments, or molecules. Below a continuous charge-ordering transition temperature T$_{co}$, the spectra are explained by assuming there are two inequivalent molecules with unequal electron densities. The absence of an associated magnetic anomaly indicates only the charge degrees…
We present first principles calculations of the magnetic and orbital properties of Ba$_2$NaOsO$_6$ (BNOO), a 5$d^1$ Mott insulator with strong spin orbit coupling (SOC) in its low temperature emergent quantum phases. Our computational method takes into direct consideration recent NMR results that established that BNOO develops a local octahedral distortion preceding the formation of long range magnetic order. We found that the two-sublattice canted ferromagnetic ground state identified in Lu \etal, Nature Comm. {\bf 8}, 14407 (2017) is accompanied by a two-sublattice staggered orbital ordering…
Thermodynamic properties, $^{31}$P nuclear magnetic resonance (NMR) measurements, and density-functional band-structure calculations for $\varepsilon$-LiVOPO$_4$ are reported. This quantum magnet features a singlet ground state and comprises two types of alternating spin-$\frac12$ chains that manifest themselves by the double maxima in the susceptibility and magnetic specific heat, and by the two-step magnetization process with an intermediate $\frac12$-plateau. From thermodynamic data and band-structure calculations, we estimate the leading couplings of $J_1\simeq 20$ K and $J_2\simeq 60$ K a…
The crystal structure and magnetic property of the single crystalline hexagonal rare-earth indium oxides GdInO$_3$ have been studied by combing experiments and model calculations. The two inequivalent Gd$^{3+}$ ions form the centered honeycomb lattice, which consists of honeycomb and triangular sublattices. The dc magnetic susceptibility and specific heat measurements suggest two antiferromagnetic phase transitions at $T_\textrm{N1}$ = 2.3 K and $T_\textrm{N2}$ = 1.02 K. An inflection point is observed in the isothermal magnetization curve, which implies an up-up-down phase with a 1/3 magnetiz…
Understanding the nature of the mysterious pseudogap phenomenon is one of the most important issues associated with cuprate high-$T_c$ superconductors. Here, we report $^{17}$O nuclear magnetic resonance (NMR) studies on two planar oxygen sites in stoichiometric cuprate YBa$_2$Cu$_4$O$_8$ to investigate the symmetry breaking inside the pseudogap phase. We observe that the Knight shifts of the two oxygen sites are identical at high temperatures but different below $T_{\rm nem} \sim$ 185 K, which is close to the pseudogap temperature $T^{\ast}$. Our result provides a microscopic evidence for int…
We report $^{23}$Na and $^{59}$Co nuclear magnetic (NMR) and quadrupolar resonance (NQR) studies for the $x=2/3$ phase of the lamellar oxide Na$_{x}$CoO$_{2}$, which allowed us to establish reliably the atomic order of the Na layers and their stacking between the CoO$_{2}$ slabs. We evidence that the Na$^{+}$ order stabilizes filled non magnetic Co$^{3+}$ ions on 25% of the cobalt sites arranged in a triangular sublattice. The transferred holes are delocalized on the 75% complementary cobalt sites which unexpectedly display a planar cobalt kagomé structure. These experimental results resolve a…
We have studied the C14 hexagonal Laves phase of YbAg$_2$ at normal conditions and under external pressure up to 19 GPa by the time-differential perturbed angular $γ-γ$ correlation spectroscopy (TDPAC) using $^{111}$Cd probe nuclei. Under pressure the valence of Yb undergoes a two stage transition from 2.8 to 3. The two stage scenario is characterized by two distinct quadrupole frequencies of $^{111}$Cd probes in silver sublattice, monotonically increasing with pressure and saturating at 8 and 16 GPa. Our experimental data are compared with the density functional studies of the electron band s…
The quantum spin systems Cu$_2$M'BO$_5$ (M' = Al, Ga) with the ludwigite crystal structure consist of a structurally ordered Cu$^{2+}$ sublattice in the form of three-leg ladders, interpenetrated by a structurally disordered sublattice with a statistically random site occupation by magnetic Cu$^{2+}$ and nonmagnetic Ga$^{3+}$ or Al$^{3+}$ ions. A microscopic analysis based on density-functional-theory calculations for Cu$_2$GaBO$_5$ reveals a frustrated quasi-two-dimensional spin model featuring five inequivalent antiferromagnetic exchanges. A broad low-temperature $^{11}$B nuclear magnetic re…
We have been able to resolve two long-standing issues that are central to the theory of high Tc superconductivity: (1) How is the physics of the doped region connected to that of the Mott insulator? (2) What is the origin of the two-dimensionality of the normal state? Specifically, based on the t-J model, we derive a renormalized Hamiltonian to describe the properties of underdoped cuprates. The theory is constrained to agree with the behavior at half filling, which is well described by the bosonic RVB state of Arovas and Auerbach. Moving holes are assumed to destroy long-range magnetic order,…
