Field-induced quasi-bound state within the two-magnon continuum of a square-lattice Heisenberg antiferromagnet

Abstract

Quantum magnets in two dimensions display strong quantum interaction effects even when magnetically ordered. Using the metal-organic framework material CuF$_2$(D$_2$O)$_2$(pyz), we investigate the field-dependent spin dynamics of the $S = 1/2$ square-lattice Heisenberg antiferromagnet by high-resolution inelastic neutron scattering to applied fields beyond one third of saturation. We discover an anomalously sharp, dispersive ``shadow mode'' residing within the two-magnon continuum, which shadows the dispersion of the transverse one-magnon branches across the Brillouin zone at an offset equal to the Larmor energy. We perform cylinder matrix-product-state (MPS) calculations that reproduce the field-induced spectrum quantitatively and apply a spectrally consistent $1/S$ spin-wave theory to deduce that the ``Larmor-shadow mode'' is a composite two-magnon resonance: a dispersing magnon at wavevector ${\bf Q}$ couples to the uniform Larmor precession at $\Gamma$, its small intrinsic linewidth indicating a non-perturbative effect of attractive magnon-magnon interactions. Another quantum-fluctuation phenomenon, the zero-field $(\pi,0)$ anomaly, is lost at increasing fields, which tighten the spectral weight into the one-magnon and Larmor-shadow modes. To our knowledge, these results constitute the first observation of a sharp quasi-bound state embedded in the continuum of a gapless two-dimensional antiferromagnet.