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We report the local (NMR) and bulk (magnetization and heat capacity) properties of the vanadium-based S=1/2 uniform spin chain compound Bi6V3O16(Bi4V2O10.66). In the low-temperature {\alpha} phase, the magnetic ions (V4+) are arranged in one-dimensional chains. The magnetic susceptibility shows a broad maximum around 50 K signifying a short-range magnetic order. Heat capacity measurements also reveal low-dimensional magnetism. The 51V magic angle spinning nuclear magnetic resonance measurements clearly show that the magnetic V4+ and nonmagnetic V5+ species are located on different crystallographic sites with no mixed occupation. The spin susceptibility calculated from the shift of the 51V NMR spectra reproduces the behavior observed in magnetic susceptibility and agrees well with the S=1/2 uniform spin chain model with J=113(5) K., Comment: 9 pages, 11 figures

We present measurements of the thermal and the thermal-Hall conductivity as a function of temperature and magnetic field in the twodimensional dimer spin system SrCu2(BO3)2. The thermal conductivity in zero magnetic field shows a pronounced peak around 4 K which is ascribed to a spin-gap opening. The low-temperature maximum is strongly suppressed by the application of magnetic field. This result implies that the majority of heat is conducted by phonons which interact with the magnetic excitations. Furthermore, a theoretical study predicted a strong thermal Hall signature due to anisotropies originating from the Dzyaloshinskii-Moriya interactions which lead to a topological character of triplon excitations [1]. Our detailed experimental investigation did not reveal such effect disproving the existence of topological transitions in the triplon band structure.

Physical review / B 97(1), 014509 (2018). doi:10.1103/PhysRevB.97.014509, Published by The American Institute of Physics, Woodbury, NY

We have studied carbon-doped magnesium diboride nanoparticles using 13C and 11B NMR in the normal and superconducting states. Measurements of the line shape reveal the role of carbon as a flux-pinning center and, combined with Knight shift measurements, suggest the doping procedure favors the chemical substitution scenario. We perform ab initio calculations on a structure with a single carbon-boron substitution which yield results that match the experimental data. The 13C and 11B Knight shift data are used to extract the spin susceptibility, which indicates a BCS pairing mechanism; however, we do not observe the Hebel-Slichter coherence peak from 1/T1 data, which we hypothesize is due to a pair-breaking mechanism present in the boron planes.

Pulsed magnets generate the highest magnetic fields as brief transients during which the observation of NMR is difficult, however, this is the only route to unique insight into material properties up to the regime of 100 T. Here, it is shown how rather broad NMR spectra can be assembled in a pulsed magnet during a single field pulse by using the inherent time dependence of the field for the recording of field-stepped free induction decays that cover a broad frequency range. The technique is then applied to 11B NMR of the spin-dimer system SrCu2(BO3)2, a magnetic insulator known to undergo a series of field-driven changes of the magnetic ground state. At peak fields of about 54 T at the Dresden High Magnetic Field Laboratory, 11B NMR spectra spanning a total of about 9 MHz width are reconstructed. The results are in good accordance with a change from a high-temperature paramagnetic state to a low-temperature commensurate superstructure of field-induced spin-dimer triplets.

Isotropic and anisotropic magnetic behavior of the frustrated spin chain compound $��$-TeVO$_4$ is reported. Three magnetic transitions observed in zero magnetic field are tracked in fields applied along different crystallographic directions using magnetization, heat capacity, and magnetostriction measurements. Qualitatively different temperature-field diagrams are obtained below 10 T for the field applied along $a$ or $b$ and along $c$, respectively. In contrast, a nearly isotropic high-field phase emerges above 18 T and persists up to the saturation that occurs around 22.5 T. Upon cooling in low fields, the transitions at $T_{\rm N1}$ and $T_{\rm N2}$ toward the spin-density-wave and stripe phases are of the second order, whereas the transition at $T_{\rm N3}$ toward the helical state is of the first order and entails a lattice component. Our microscopic analysis identifies frustrated $J_1-J_2$ spin chains with a sizable antiferromagnetic interchain coupling in the $bc$ plane and ferromagnetic couplings along the $a$ direction. The competition between these ferromagnetic interchain couplings and the helical order within the chain underlies the incommensurate order along the $a$-direction, as observed experimentally. Although a helical state is triggered by the competition between $J_1$ and $J_2$ within the chain, the plane of the helix is not uniquely defined because of competing magnetic anisotropies. Using high-resolution synchrotron diffraction and $^{125}$Te nuclear magnetic resonance, we also demonstrate that the crystal structure of $��$-TeVO$_4$ does not change down to 10 K, and the orbital state of V$^{4+}$ is preserved., 13 pages, 14 figures, 3 tables (published version)

SrCu2(BO3)2 is a prominent realization of the Shastry-Sutherland lattice model [1]. In this quasi-two-dimensional compound, Cu2+ ions form orthogonal spin-singlet dimers with strong geometrical frustration of the next-nearest and nearest neighbor exchange interactions. SrCu2(BO3)2 has been studied extensively using a variety of techniques, such as nuclear magnetic resonance (NMR) spectroscopy, or recent magnetization measurements up to 118 T. These experiments reveal a complex sequence of magnetization plateaus with differing commensurate magnetic superstructure, stemming from a stripe type order of triplet states [2-4]. Due to its highly sensitive local probe character, NMR can provide deep insight into the spin-coupling mechanisms and excitations at highest magnetic fields. We present 11B NMR spectra measured in pulsed magnetic fields up to 56 T, and compare those with prior results obtained in highest static magnetic fields. Herewith, we prove the feasibility and efficacy of this new technique, yielding the capability for extended studies at highest magnetic fields up to the 100 T regime that determine the spin structure in the 1/3 magnetization plateau and beyond.

SrCu2(BO3)2 is a quasi-two-dimensional spin system consisting of Cu2+ ions which form orthogonal spin-singlet dimers, also known as the Shastry-Sutherland lattice. This system has been studied extensively using a variety of techniques to probe the spin-triplet excitations, including recent magnetization measurements over 100 T. Spectroscopic techniques, such as nuclear magnetic resonance (NMR), can provide further insight into the spin-coupling mechanisms and excitations. We present 11B NMR spectra measured in pulsed magnetic fields up to 54 T, and compare those with prior results obtained in static magnetic fields at 41 T. Herewith, we prove the feasibility and efficacy of this technique, yielding the capability for extended studies at highest magnetic fields up to the 100 T regime that determine the spin structure in the 1/3 magnetization plateau and beyond.

Han purple (BaCuSi2O6) is not only an ancient pigment, but also a valuable model material for studying Bose-Einstein condensation of magnons in high magnetic fields. Using precise low-temperature structural data and extensive density-functional calculations, we elucidate magnetic couplings in this compound. The resulting magnetic model comprises two types of nonequivalent spin dimers, in excellent agreement with the Cu63,65 nuclear magnetic resonance data. We further argue that leading interdimer couplings connect the upper site of one dimer to the bottom site of the contiguous dimer, and not the upper-to-upper and bottom-to-bottom sites, as assumed previously. This finding is verified by inelastic neutron scattering data and implies the lack of frustration between the layers of spin dimers in BaCuSi2O6, thus challenging existing theories of the two-dimensional-like Bose-Einstein condensation of magnons in this compound. © 2014 American Physical Society.

The low-temperature crystal structure of BaCuSi2O6 has been investigated with high-resolution synchrotron x-ray and neutron powder diffraction techniques and has been found to be on average (ignoring the incommensurate modulation) orthorhombic, with the most probable space group Ibam. The Cu-Cu dimers in this material are forming two types of layers with distinctly different interatomic distances. Subtle changes also modify the partially frustrated interlayer Cu-Cu exchange paths. The present results corroborate the interpretation of low-temperature nuclear magnetic resonance and inelastic neutron scattering data in terms of distinct dimer layers.

BaCuSi2O6 can be regarded as an almost ideal realization of an S = 1/2 system of weakly interacting spin dimers with spin-singlet ground state and gapped excitation spectrum. We argue that the fine structure observed in low-temperature EPR spectra of BaCuSi2O6 is a fingerprint of triplet excitations (excitons). Analyzing the angular dependence of the exciton modes allows us to precisely calculate the zero-field splitting within the triplet states and, correspondingly, the anisotropy parameter, D = 0.07cm-1. The proposed procedure can be applied for studying anisotropy effects in a large number of S = 1/2 gapped quantum antiferromagnets with dimerized or alternating spin structure.

BaCuSi$_2$O$_6$, a $S=1/2$ quantum antiferromagnet with a double-layer structure of Cu$^{2+}$ ions in a distorted planar-rectangular coordination and with a dimerized spin singlet ground state, is studied by means of the electron paramagnetic resonance technique. It is argued that multiple absorptions observed at low temperatures are intimately related to a thermally-activated spin-triplet exciton superstructure. Analysis of the angular dependence of exciton modes in BaCuSi$_2$O$_6$ allows us to accurately estimate anisotropy parameters. In addition, the temperature dependence of EPR intensity and linewidth is discussed., Submitted to Phys. Rev. B

BaCuSi2O6, a S = 1/2 quantum antiferromagnet with a double-layer structure of Cu2+ ions in a distorted planar-rectangular coordination and with a dimerized spin singlet ground state, has been studied by means of the electron paramagnetic resonance technique. It is argued that multiple absorptions observed at low temperatures are intimately related to a thermally activated spin-triplet exciton superstructure, which appears to be a characteristic feature of low-dimensional anisotropic spin- 1/2 systems with the dimerized spin-singlet ground state. We showed that analysis of the angular dependence of exciton modes could be used for accurate estimation of anisotropy parameters in BaCuSi2O6; the procedure can be applied for a large number of S = 1/2 quantum antiferromagnets. In addition, the temperature dependence of EPR intensity and linewidth in BaCuSi2O6 has been studied and discussed.

We present results of high-frequency/field Electron Spin Resonance (ESR) studies of the highly frustrated spin system SrCu2(BO3)2,which can be regarded as to the best known realization of the Shastry-Sutherland model for two-dimensional Heisenberg antiferromagnets. The frequency-field diagram of magnetic excitations has been studied in a frequency range of 150-700 GHz, employing unable-frequency ESR technique. Two gapped odes were observed in the excitation spectrum. The size of the quantum spin gaps determined directly is: 708 GHz and 764 GHz (34 K and 36.7 K). The observation of excitations from the ground state (which are normally forbidden) and a double-gap structure of the ESR excitation spectrum in SrCu2(BO3)2 suggest and essential role of the Dzyaloshinski-Moriya interaction. The results are compared with those obtained by Nojiri et al. [J. Phys. Soc. Jpn. 68, 2906 (1999); J.Phys. Soc. Jpn. 72, 3243 (2003)]. The temperature behavior of excited-state transitions in SrCu2(BO3)2 (ESR linewidth and intensity) is presented and discussed.

Besides being an ancient pigment, BaCuSi$_2$O$_6$ is a quasi-2D magnetic insulator with a gapped spin dimer ground state. The application of strong magnetic fields closes this gap creating a gas of bosonic spin triplet excitations called triplons. The topology of the spin lattice makes BaCuSi$_2$O$_6$ an ideal candidate for studying the Bose-Einstein condensation of triplons as a function of the external magnetic field, which acts as a chemical potential. In agreement with quantum Monte Carlo numerical simulations, we observe a distinct lambda-anomaly in the specific heat together with a maximum in the magnetic susceptibility upon cooling down to liquid Helium temperatures., published on August 20, 2004

We report measurements of the specific heat of the quantum spin liquid system SrCu2(BO3)2 in continuous magnetic fields H of up to 33 T. The specific heat vs temperature at zero field shows an anomaly at 8 K, marking the opening of a gap in the spin singlet excitations. At fields H~12 T, we clearly see a second anomaly that shifts to lower temperatures as H is increased. We attribute its origin to single triplet excitations of the singlet dimer ground state. This conclusion is supported by calculations of the specific heat, which reproduce the experimental data, made using the finite temperature Lanczos method to solve a Shastry-Sutherland Hamiltonian including nearest and next-nearest neighbor Dzyaloshinsky-Moriya interactions. The parameters used to fit the data are the exchange constants J = 74 K and J'/J = 0.62, and the Dzyaloshinsky-Moriya coupling constants |D|=6.1K, and $|D'|=2.2K., Comment: 5 pages, 4 figures in color

We report measurements of the Gaussian contribution, T_{2G}, to the plane ^{63}Cu nuclear spin--spin relaxation time in the YBa_2Cu_3O_7 and YBa_2Cu_4O_8 blocks of normal and superconducting Y_2Ba_4Cu_7O_{15}. The data confirm our previous results that adjacent CuO_2 planes have different doping levels and that these planes are strongly coupled. -- The static spin susceptibility at the anti-ferromagnetic wave vector exhibits a Curie--Weiss like temperature dependence in the normal state. -- The Y_2Ba_4Cu_7O_{15} data are incompatible with a phase diagram based on a single CuO_2 plane theory and suggest that the appearance of a spin gap implies interplane coupling. Additional data for YBa_2Cu_4O_8 and YBa_2Cu_3O_{6.982} are in accord with the single plane theory. -- The temperature dependence of T_{2G,ind} below T_c excludes isotropic s-wave superconductivity in all three compounds., Comment: 7 pages, REVTEX 3.0, 5 figures available upon request

Isotropic and anisotropic magnetic behavior of the frustrated spin-chain compound beta-TeVO4 is reported. Three magnetic transitions observed in zero magnetic field are tracked in fields applied along different crystallographic directions using magnetization, heat capacity, and magnetostriction measurements. Qualitatively different temperature-field diagrams are obtained below 10 T for the field applied along a or b and along c, respectively. In contrast, a nearly isotropic high-field phase emerges above 18 T and persists up to the saturation that occurs around 22.5 T. Upon cooling in low fields, the transitions at T-N1 and T-N2 toward the spin-density-wave and stripe phases are of the second order, whereas the transition at T-N3 toward the helical state is of the first order and entails a lattice component. Our microscopic analysis identifies frustrated J(1)-J(2) spin chains with a sizable antiferromagnetic interchain coupling in the bc plane and ferromagnetic couplings along the a direction. The competition between these ferromagnetic interchain couplings and the helical order within the chain underlies the incommensurate order along the a direction, as observed experimentally. While a helical state is triggered by the competition between J(1) and J(2) within the chain, the plane of the helix is not uniquely defined because of competing magnetic anisotropies. Using high-resolution synchrotron diffraction and Te-125 nuclear magnetic resonance, we also demonstrate that the crystal structure of beta-TeVO4 does not change down to 10 K, and the orbital state of V4+ is preserved.