Leonie Woodland

Abstract:

The Ising chain realizes the fundamental paradigm of spin fractionalization, where locally flipping a spin creates two domain walls (spinons) that can separate apart at no energy cost. In a quasi-one-dimensional system, the mean-field effects of the weak three-dimensional couplings confine the spinons into a Zeeman ladder of two-spinon bound states. Here, we experimentally tune the confinement potential between spinons in the quasi-one-dimensional Ising ferromagnet CoNb2O6 by means of an applied magnetic field with a large component along the Ising direction. Using high-resolution single crystal inelastic neutron scattering, we directly observe how the spectrum evolves from the limit of very weak confinement at low field (with many closely spaced bound states with energies scaling as the field strength to the power 2/3) to very strong confinement at high field (where it consists of a magnon and a dispersive two-magnon bound state, with a linear field dependence). At intermediate fields, we explore how the higher-order bound states disappear from the spectrum as they move to higher energies and overlap with the two-particle continuum. By performing a global fit to the observed spectrum in zero field and high field applied along two orthogonal directions, combined with a quantitative parametrization of the interchain couplings, we propose a refined single-chain and interchain Hamiltonian that quantitatively reproduces the dispersions of all observed modes and their field dependence.

Abstract:

We present experimental and theoretical evidence of novel bound state formation in the low transverse field ordered phase of the quasi-one-dimensional Ising-like material CoNb2O6. High-resolution single-crystal inelastic neutron scattering measurements observe that small transverse fields lead to a breakup of the spectrum into three parts, each evolving very differently upon increasing field. This can be naturally understood starting from the excitations of the ordered phase of the transverse field Ising model, domain wall quasiparticles (solitons). Here, the transverse field and a staggered off-diagonal exchange create one-soliton hopping terms with opposite signs. We show that this leads to a rich spectrum and a special field, when the strengths of the off-diagonal exchange and transverse field match, at which solitons become localized; the highest field investigated is very close to this special regime. We solve this case analytically and find three two-soliton continua, along with three novel bound states. Perturbing away from this novel localized limit, we find very good qualitative agreement with the experimental data. We also present calculations using exact diagonalization of a recently refined Hamiltonian model for CoNb2O6 and using diagonalization of the two-soliton subspace, both of which provide a quantitative agreement with the observed spectrum. The theoretical models qualitatively and quantitatively capture a variety of nontrivial features in the observed spectrum, providing insight into the underlying physics of bound state formation.

Abstract:

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular-lattice Ising-like antiferromagnet Na2BaCo(PO4)2 in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field BC, we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in a polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below BC, we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering the field and, at 0.25 T and zero field, it dominates the entire spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal P3¯m1 space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the CoO6 octahedra around the c axis, which lowers the symmetry to P3¯.

Abstract:

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular-lattice Ising-like antiferromagnet ${\mathrm{Na}}_2\mathrm{BaCo}{\left({\mathrm{PO}}_4\right)}_2$ in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field $B_{\mathrm{C}}$ , we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in a polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below $B_{\mathrm{C}}$ , we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering the field and, at 0.25 T and zero field, it dominates the entire spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal $P\overline{3}m1$ space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the ${\mathrm{CoO}}_6$ octahedra around the $c$ axis, which lowers the symmetry to $P\overline{3}$ .