Spin Correlations and Short-Range Magnetic Order in the Honeycomb-Layered Na2Ni2TeO6

An experimental study of long-range magnetic order formation mechanisms in a layered structure with a honeycomb arrangement of the magnetic atoms Na2Ni2TeO6 is conducted. For the first time, the strong spin correlations are directly observed above the Neel temperature T-N that is manifested in the presence of broad diffuse peaks on neutron diffraction patterns obtained with the XYZ polarization analysis. Due to the possibility of separating the magnetic, nuclear incoherent, and nuclear coherent contributions to the total neutron scattering cross section, it is unequivocally established that the observed diffuse scattering has magnetic nature. The spin-pair correlation function is reconstructed by modeling diffuse neutron scattering on Na2Ni2TeO6 with reverse Monte Carlo method. The obtained results indicate 2D nature of the magnetic correlations, and moreover, the symmetry of short-range magnetic state corresponds to long-range zigzag-type magnetic order in the honeycomb net, which is established earlier based on the theoretical calculations.

Long-range magnetic ordering in Li2MnGeO4 and precursor short-range spin correlations

Artem Korshunov, Irina Safiulina

Long-range magnetic ordering and short-range spin correlations in layered noncentrosymmetric orthogermanate Li2MnGeO4 were studied by means of polarized and unpolarized neutron scattering. The combined Rietveld refinement of synchrotron and neutron powder diffraction data at room temperature within the Pmn2(1) space group allowed us to specify the details of the crystal structure. According to the additional Bragg peaks in low-temperature neutron diffraction patterns a long-range antiferromagnetic ordering with the propagation vector k = (1/2 1/2 1/2) has been found below T-N approximate to 8 K. Symmetry analysis revealed the model of the ground state spin structure within the C(a)c (no. 9.41) magnetic space group. It is represented by the noncollinear ordering of manganese atoms with a refined magnetic moment of 4.9 mu(B)/Mn2+ at 1.7 K, which corresponds to the saturated value for the high-spin configuration S = 5/2. Diffuse magnetic scattering was detected on the neutron diffraction patterns at temperatures just above T-N. Its temperature evolution was investigated in detail by polarized neutron scattering with the following XYZ-polarization analysis. Reverse Monte Carlo simulation of diffuse scattering data showed the development of short-range ordering in Li2MnGeO4, which is symmetry consistent on a small scale with the long-range magnetic state below T-N. The reconstructed radial spin-pair correlation function S(0)S(r) displayed the predominant role of antiferromagnetic correlations. It was found that spin correlations are significant only for the nearest magnetic neighbors and almost disappear at r approximate to 12 angstrom at 10 K. Temperature dependence of the diffuse scattering implies short-range ordering long before the magnetic phase transition. Besides, the spin arrangement was found to be similar in both cases above and below T-N. As a result, an exhaustive picture of the gradual formation of magnetic ordering in Li2MnGeO4 is presented.

2020

Neutron spectroscopy in the layered quantum magnet SrCu₂(BO₃)₂ and in transition metal phosphorus trisulfides (MPS₃)

Diane Virginie Marie Lançon

Collective magnetic excitations are a fascinating aspect of condensed matter physics, where neutron scattering can provide valuable insight into the magnetic properties of physical realisations of model systems. This thesis focuses on the excitation spectra of layered quantum magnets in the case of the frustrated quantum magnet SrCu

_2

(BO

_3

)

_2

and the family of quasi-2D antiferromagnets MPS

_3

, with M a transition metal. \begin{itemize}[topsep=2pt,itemsep=-0.7ex] \item SrCu

_2

(BO

_3

)

_2

is a physical realisation of the two-dimensional Shastry-Sutherland theoretical model, constructed as orthogonal dimers with the product of singlets on the strong antiferromagnetic

J

bond as an exact ground state. The spin interactions for such a particular geometry induces strong frustration which leads to unconventional magnetism and exotic phases of matter. This work is concerned with a series of aspects of the magnetic excitations in this compound. The excitation spectra as a function of field, temperature and pressure are measured using neutron time-of-flight spectroscopy. The experimental results show that correlations, bound magnons and finite temperature properties are highly unconventional and these results are compared with existing theories on frustrated model systems. In addition, predicted topological properties of SrCu

_2

(BO

_3

)

_2

in an applied field are confirmed experimentally. \item The transition metal phosphorus trisulfides (MPS

_3

) are a family of quasi two-dimensional materials on a honeycomb lattice with weakly bound magnetic planes. This work focuses mainly on the exchange interactions and critical properties of FePS

_3

, which is largely anisotropic with the S=2 Fe

^{2+}

moments pointing normal to the

(a,b)

plane. Inelastic neutron scattering on single crystals is used to measure the spin wave dispersion, providing new insight on the strength of the coupling interactions and anisotropies and showing that FePS

_3

is a good two-dimensional model antiferromagnet. Similar experiments on powdered samples of NiPS

_3

show low-Q dispersive spin waves with a small spin-gap. Critical properties of FePS

_3

close to the Néel temperature are further discussed, as the magnetic nature of the measured quasi-elastic scattering is confirmed. Based on magnetization measurements in high pulsed fields, a possible tricritical point in the 40-50T range is proposed. \end{itemize} The work presented in this thesis has been carried out in a collaboration between the Institut Laue Langevin in Grenoble and the Laboratory for Quantum Magnetism of the EPFL.

EPFL2017

Glassy low-energy spin fluctuations and anisotropy gap in La1.88Sr0.12CuO4

Johan Juul Chang, Joël Mesot, Henrik Moodysson Rønnow

We present high-resolution triple-axis neutron scattering studies of the high-temperature superconductor La1.88Sr0.12CuO4 (Tc=27 K). The temperature dependence of the low-energy incommensurate magnetic fluctuations reveals distinctly glassy features. The glassiness is confirmed by the difference between the ordering temperature TN≃Tc inferred from elastic neutron scattering and the freezing temperature Tf≃11 K obtained from muon spin rotation studies. The magnetic field independence of the observed excitation spectrum as well as the observation of a partial suppression of magnetic spectral weight below 0.75 meV for temperatures smaller than Tf, indicate that the stripe frozen state is capable of supporting a spin anisotropy gap, of a magnitude similar to that observed in the spin and charge stripe-ordered ground state of La1.875Ba0.125CuO4. The difference between TN and Tf implies that the significant enhancement in a magnetic field of nominally elastic incommensurate scattering is caused by strictly inelastic scattering—at least in the temperature range between Tf and Tc—which is not resolved in the present experiment. Combining the results obtained from our study of La1.88Sr0.12CuO4 with a critical reappraisal of published neutron scattering work on samples with chemical composition close to p=0.12, where local probes indicate a sharp maximum in Tf(p), we arrive at the view that the low-energy fluctuations are strongly dependent on composition in this regime, with anisotropy gaps dominating only sufficiently close to p=0.12 and superconducting spin gaps dominating elsewhere.

American Physical Society2013