Electron spin resonance studies of frustrated quantum spin systems

Since the last few decades frustrated spin systems have attracted much interest. These studies are motivated by the rich variety of their unusual magnetic properties and potential applications. In this thesis, excitation spectra of the weakly coupled dimer system Ba3Cr2O8, the spin-1/2 chain material with distorted diamond structure Cu3(CO3)2(OH)2 (natural mineral azurite), and the quasi-twodimensional antiferromagnet with triangle spin structure Cs2CuBr4 have been studied by means of high-field electron spin resonance. Two pairs of gapped modes corresponding to transitions from a spin-singlet ground state to the first excited triplet state with zero-field energy gaps, of 19.1 and 27 K were observed in Ba3Cr2O8. The observation of ground-state excitations clearly indicates the presence of a non-secular term allowing these transitions. Our findings are of crucial importance for the interpretation of the field-induced transitions in this material (with critical fields Hc1 = 12.5 T and Hc2 = 23.6 T) in terms of the magnon Bose-Einstein condensation. The natural mineral azurite, Cu3(CO3)2(OH)2, has been studied in magnetic fields up to 50 T, revealing several modes not observed previously. Based on the obtained data, all three critical fields were identified. A substantial zero-field energy gap, Δ = 9.6 K, has been observed in Cs2CuBr4 above the ordering temperature. It is argued that contrary to the case for the isostructural Cs2CuCl4, the size of the gap can not be explained solely by the uniform Dzyaloshinskii-Moriya interaction, but it is rather the result of the geometrical frustration stabilizing the spin-disordered state in Cs2CuBr4 in the close vicinity of the quantum phase transition between a spiral magnetically ordered state and a 2D quantum spin liquid

Spin excitations of magnetoelectric LiNiPO4_4 in multiple magnetic phases

Spin excitations of magnetoelectric LiNiPO$_4$ are studied by infrared absorption spectroscopy in the THz spectral range as a function of magnetic field through various commensurate and incommensurate magnetically ordered phases up to 33\,T. Six spin resonances and a strong two-magnon continuum are observed in zero magnetic field. Our systematic polarization study reveals that some of the excitations are usual magnetic-dipole active magnon modes, while others are either electromagnons, electric-dipole active, or magnetoelectric, both electric- and magnetic-dipole active spin excitations. Field-induced shifts of the modes for all three orientations of the field along the orthorhombic axes allow us to refine the values of the relevant exchange couplings, single-ion anisotropies, and the Dzyaloshinskii-Moriya interaction on the level of a four-sublattice mean-field spin model. This model also reproduces the spectral shape of the two-magnon absorption continuum, found to be electric-dipole active in the experiment

Magnetization reversal through an antiferromagnetic state

Magnetization reversal in ferro- and ferrimagnets is a well-known archetype of non-equilibrium processes, where the volume fractions of the oppositely magnetized domains vary and perfectly compensate each other at the coercive magnetic field. Here, we report on a fundamentally new pathway for magnetization reversal that is mediated by an antiferromagnetic state. Consequently, an atomic-scale compensation of the magnetization is realized at the coercive field, instead of the mesoscopic or macroscopic domain cancellation in canonical reversal processes. We demonstrate this unusual magnetization reversal on the Zn-doped polar magnet Fe2Mo3O8. Hidden behind the conventional ferrimagnetic hysteresis loop, the surprising emergence of the antiferromagnetic phase at the coercive fields is disclosed by a sharp peak in the field-dependence of the electric polarization. In addition, at the magnetization reversal our THz spectroscopy studies reveal the reappearance of the magnon mode that is only present in the pristine antiferromagnetic state. According to our microscopic calculations, this unusual process is governed by the dominant intralayer coupling, strong easy-axis anisotropy and spin fluctuations, which result in a complex interplay between the ferrimagnetic and antiferromagnetic phases. Such antiferro-state-mediated reversal processes offer novel concepts for magnetization control, and may also emerge for other ferroic orders.</p

From confined spinons to emergent fermions: Observation of elementary magnetic excitations in a transverse-field Ising chain

We report on spectroscopy study of elementary magnetic excitations in an Ising-like antiferromagnetic chain compound SrCo$_2$V$_2$O$_8$ as a function of temperature and applied transverse magnetic field up to 25 T. An optical as well as an acoustic branch of confined spinons, the elementary excitations at zero field, are identified in the antiferromagnetic phase below the N\'{e}el temperature of 5 K and described by a one-dimensional Schr\"{o}dinger equation. The confinement can be suppressed by an applied transverse field and a quantum disordered phase is induced at 7 T. In this disordered paramagnetic phase, we observe three emergent fermionic excitations with different transverse-field dependencies. The nature of these modes is clarified by studying spin dynamic structure factor of a 1D transverse-field Heisenberg-Ising (XXZ) model using the method of infinite time evolving block decimation. Our work reveals emergent quantum phenomena and provides a concrete system for testifying theoretical predications of one-dimension quantum spin models.Comment: 8 pages and 6 figure

Experimental observation of Bethe strings

Almost a century ago, string states-complex bound states of magnetic excitations-were predicted to exist in one-dimensional quantum magnets(1). However, despite many theoretical studies(2-11), the experimental realization and identification of string states in a condensed-matter system have yet to be achieved. Here we use high-resolution terahertz spectroscopy to resolve string states in the antiferromagnetic Heisenberg-Ising chain SrCo2V2O8 in strong longitudinal magnetic fields. In the field-induced quantum-critical regime, we identify strings and fractional magnetic excitations that are accurately described by the Bethe ansatz(1,3,4). Close to quantum criticality, the string excitations govern the quantum spin dynamics, whereas the fractional excitations, which are dominant at low energies, reflect the antiferromagnetic quantum fluctuations. Today, Bethe's result(1) is important not only in the field of quantum magnetism but also more broadly, including in the study of cold atoms and in string theory; hence, we anticipate that our work will shed light on the study of complex many-body systems in general

Electron spin resonance studies of frustrated quantum spin systems

Since the last few decades frustrated spin systems have attracted much interest. These studies are motivated by the rich variety of their unusual magnetic properties and potential applications. In this thesis, excitation spectra of the weakly coupled dimer system Ba3Cr2O8, the spin-1/2 chain material with distorted diamond structure Cu3(CO3)2(OH)2 (natural mineral azurite), and the quasi-twodimensional antiferromagnet with triangle spin structure Cs2CuBr4 have been studied by means of high-field electron spin resonance. Two pairs of gapped modes corresponding to transitions from a spin-singlet ground state to the first excited triplet state with zero-field energy gaps, of 19.1 and 27 K were observed in Ba3Cr2O8. The observation of ground-state excitations clearly indicates the presence of a non-secular term allowing these transitions. Our findings are of crucial importance for the interpretation of the field-induced transitions in this material (with critical fields Hc1 = 12.5 T and Hc2 = 23.6 T) in terms of the magnon Bose-Einstein condensation. The natural mineral azurite, Cu3(CO3)2(OH)2, has been studied in magnetic fields up to 50 T, revealing several modes not observed previously. Based on the obtained data, all three critical fields were identified. A substantial zero-field energy gap, Δ = 9.6 K, has been observed in Cs2CuBr4 above the ordering temperature. It is argued that contrary to the case for the isostructural Cs2CuCl4, the size of the gap can not be explained solely by the uniform Dzyaloshinskii-Moriya interaction, but it is rather the result of the geometrical frustration stabilizing the spin-disordered state in Cs2CuBr4 in the close vicinity of the quantum phase transition between a spiral magnetically ordered state and a 2D quantum spin liquid