Magnetic model in multiferroic NdFe3(BO3)(4) investigated by inelastic neutron scattering

We performed inelastic neutron scattering measurements on single crystals of NdFe3((BO3)-B-11)(4) to explore the magnetic excitations, to establish the underlying Hamiltonian, and to reveal the detailed nature of hybridization between the 4f and 3d magnetism. The observed spectra exhibiting a couple of key features, i.e., anticrossing of Nd and Fe excitations and anisotropy gap at the antiferromagnetic zone center, are explained by the magnetic model including spin interaction in the framework of weakly coupled Fe3+ chains, interaction between the Fe3+ and Nd3+ moments, and single-ion anisotropy derived from the Nd3+ crystal field. The combination of the measurements and calculations reveals that the hybridization between 4f and 3d magnetism propagates the local magnetic anisotropy of the Nd3+ moment to the Fe3+ network, leading to the determination of the bulk structure of both electric polarization and magnetic moment in the multiferroics of the spin-dependent metal-ligand hybridization type.

Order and dynamics in Kagome like compound Cu2OSO4 and other quantum magnets

Virgile Yves Favre

This thesis presents results of studies of novel compounds modeling complex fundamental physics phenomena. Cu2OSO4 is a copper based magnetic Mott Insulator system, where spin half magnetic moments form a new type of lattice. These intrinsically quantum pins are exhibiting atypical magnetic order and spin dynamics. The recent success in the growth of large single crystals of Cu2OSO4 enabled to perform measurements probing its static and fluctuating properties. The peculiarity of this sample is that its atoms are forming layers, with a geometry close to the intensively studied Kagomé lattice, but with a third of its spins replaced by dimers. This quantum magnetism system has been probed in its bulk, by the means of heat capacity and DC-susceptibility measurements, revealing a transition to a magnetically long range ordered state upon cooling, the details of which are revealed by neutron scattering. Single crystal inelastic neutron scattering shed light on the spin-dynamics in the system, with clear spin waves appearing as fluctuations around the peculiar ground state of the system: a 120 degrees spin configuration where the magnetic moment of the spin-dimer causes the sample to be globally ferrimagnetic. The presented results indicate that Cu2OSO4 represents a new type of model lattice with frustrated interactions where interplay between magnetic order, thermal and quantum fluctuations can be explored. The magnetic excitations of the compound can be modeled by a yet-to-be-understood internal effective mean-field that no simple magnetic coupling seems to reproduce. K2Ni2(SO4)3 is another compound that allows for the existence of non-trivial topological phases. This thesis presents results of the study of the unusual magnetic behavior of K2Ni2(SO4)3. No clear sign of well-established magnetic long range order has been observed down to dilution temperatures. Neutron scattering reveals the details of the competition between frustration and fluctuations that prevent order from settling in. Low temperature spin excitations take the form of a continuum at 500 mK, but also of broad, energy independent continua at higher temperatures. Bulk and neutron scattering measurements are put in perspective and linked together with a view to building up a better understanding of how quantum spin liquids can be stabilized in general, and in particular in this model compound. Finally, the last contribution of this thesis to the field of condensed matter physics regards the establishment of a state-of-the-art technique to fit heat capacity and unit cell volume of samples to try and make the extraction of magnetic information from specific heat measurements more robust. This newly-developed technique consists in modeling lattice contributions with better accuracy by using data from multiple experimentally accessible quantities to consolidate the fitting scheme. This method has been cautiously applied to several compounds at the forefront of research in experimental physics.

EPFL2021

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

Magnetism of Single Adatoms and Small Adsorbed Clusters Investigated by Means of Low-Temperature STM

Quentin Dubout

This thesis works reports on the magnetic properties of single transition metal atoms and hydrogenated compounds adsorbed on crystal surfaces. It is an experimental study, based on scanning tunneling microscopy (STM), initiated by the project of demonstrating the existence of magnetic remanence for single adsorbed atoms (adatoms). All the measurements have been performed with a scanning tunneling microscope operating at 0.4 K and equipped with 8.5 T superconducting coils. The investigated systems are cobalt atoms, pure and hydrogenated (cobalt hydrides), adsorbed on Pt(111) and graphene on Pt(111) surfaces. In the first case, we have immediately been confronted to the presence of cobalt hydrides on the surface. Three types of hydrides (CoH, CoH2, and CoH3) have been identified, quite different from the clean adatoms, and readily distinguished by their tunnel spectrum (STS). Twoofthesehydridesdisplaylow-energyvibrationalmodes(1−30meV),identifiedbytheir absence of response to a magnetic field, the effect of an isotopic substitution, and by comparison with known systems. The three hydrides can be deprotonated applying a sufficient voltage between tip and sample. CoH2 on Pt(111) presents a Kondo resonance, due to a half-integer spin (S = 3/2) and a peculiar magnetic anisotropy. This system corresponds to the first demonstration of the appearance of the Kondo effect upon hydrogen adsorption. The results of several attempts to observe remanence for single cobalt adatoms on Pt(111) with spin-polarized scanning tunneling microscopy (SP-STM) are also presented and discussed. The second system differs from the first one in the presence of a graphene layer on the Pt surface. The first experimental determination of the magnetic moment and magnetic anisotropy of adatoms on graphene is reported in this thesis. A magnetic moment of (2.2 ± 0.4) μB was measured by spin-excitation spectroscopy (SES), as well as a hard magnetization axis with an anisotropy energy of 8.1 ± 0.4 meV. This value, comparable to the record value of single cobalt atoms on Pt(111), has been mainly attributed to the strong hybridization between cobalt and graphene. Ab initio calculations confirmed our observations. Graphene thus represents an extremely promising substrate for future applications in nanoscale magnetism and spintronics. This system also exhibits three different cobalt hydrides in addition to the clean atoms. Their respective chemical composition, CoH, CoH2, and CoH3, was determined by direct comparison between high resolution STM images and simulated images obtained from ab initio calculated atomic structures. A controlled deprotonation method is presented. CoH3 is the only hydride to display spin excitations. Its magnetic moment is comparable to that of clean cobalt, it presents a hard magnetization axis as well, however, its magnetic anisotropy energy is sensibly lower, 1.7 ± 0.05 meV. The other two hydrides display vibrational excitations only. The effect of hydrogen on the magnetic properties of metal adatoms is therefore very strong in this system as well, and must be taken into account in future studies, hydrogen being a very common contaminant in ultra-high vacuum set-ups. Finally, a detailed study of the structure graphene mono- and bilayers on Ru(0001) was realized. Two different stackings, AB and AA, have been identified for the bilayers, the last one not observed to date for this system. The moiré structure of monolayer graphene and of this last type of bilayer has been determined: (11.57×11.57)R4.3◦ and (10.54×10.54)R4.7◦, respectively. Moreover, C-C bond distortions of more than 10%, observed in the STM images, have been studied in detail. A quantitative comparison with ab initio calculations allowed to identify their origin as the tilt of the graphene π-orbitals. These distortions are therefore purely artificial. This is an important result for future scanning tunneling microscopy studies of graphene.

EPFL2013