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

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.

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

Two-dimensional square-lattice S=1/2 antiferromagnet Cu(pz)(2)(ClO4)(2)

Henrik Moodysson Rønnow, Nikolay Tsyrulin

We present an experimental study of the two-dimensional S=1/2 square-lattice antiferromagnet Cu(pz)(2)(ClO4)(2) (pz denotes pyrazine-C4H4N2) using specific-heat measurements, neutron diffraction, and cold-neutron spectroscopy. The magnetic field dependence of the magnetic ordering temperature was determined from specific-heat measurements for fields perpendicular and parallel to the square-lattice planes, showing identical field-temperature phase diagrams. This suggest that spin anisotropies in Cu(pz)(2)(ClO4)(2) are small. The ordered antiferromagnetic structure is a collinear arrangement with the magnetic moments along either the crystallographic b or c axis. The estimated ordered magnetic moment at zero field is m(0)=0.47 (5)mu(B) and thus much smaller than the available single-ion magnetic moment. This is evidence for strong quantum fluctuations in the ordered magnetic phase of Cu(pz)(2)(ClO4)(2). Magnetic fields applied perpendicular to the square-lattice planes lead to an increase in the antiferromagnetically ordered moment to m(0)=0.93 (5)mu(B) at mu H-0= 13.5 T evidence that magnetic fields quench quantum fluctuations. Neutron spectroscopy reveals the presence of a gapped spin excitations at the antiferromagnetic zone center and it can be explained with a slightly anisotropic nearest-neighbor exchange coupling described by J(xy)(1)= 1.563 (13) meV and J(z)(1) = 0.9979(2)J(1)(xy).

2010

Classical and Quantum Critical Phenomena in the Dipolar Antiferromagnet LiErF4

Neda Nikseresht Ghanepour

The collective behavior of systems consisting of interacting dipoles is a subject of considerable studies. The anisotropic nature of such interactions opens an arena to explore fundamental questions in correlated electron physics, ranging from quantum entanglement, phase transitions, spin glass states to disorder and fluctuations. LiHoF4 is a textbook example of a ferromagnetic Ising-dipolar model, offering a simple and well-understood Hamiltonian. The system undergoes a quantum phase transition (QPT) in a field transverse to the easy axis, which induces quantum fluctuations between the ground state doublet. Dilution of Ho sites with non-magnetic Yttrium ions lowers only the transition temperature (Tc), and eventually lead to spin-glass state. While Tc decreases in a linear fashion, as expected from simple mean-field (MF) calculation, critical field decreases much faster. The behavior upon dilution has been pointed out to be related to randomness and off-diagonal dipolar interactions. In chapter 5 of this thesis I quantify the deviation of experimental results from neutron scattering studies from MF prediction, with the aim that this analysis can be used in future theoretical efforts towards a quantitative description. The aim of this thesis, however, deals with LiErF4 which is an unexplored planar dipolar antiferromagnetic member of LiReF4 family, with TN ≃ 370 mK. The system undergoes a QPT in an applied field H∥c = 4.0±0.1 kOe, confirmed by a softening of the characteristic excitations at Hc. A combined neutron scattering, specific heat, and magnetic susceptibility study reveals a novel non-MF critical scaling of the classical phase transition, belonging to the 2DXY /h4 universality class. In accord with this, the quantum phase transition at Hc exhibits a three-dimensional classical behavior. The effective dimensional reduction may be a consequence of the intrinsic anisotropic nature of the dipolar interaction. Four-fold anisotropy and degeneracy breaking could be due to the "order-by-disorder" phenomena, which could open a gap in dispersion of the magnetic excitations.