Violation of detailed balance in non-equilibrium magnons observed by inelastic neutron scattering

Traditional inelastic neutron scattering (INS) characterizes excitations—such as phonons and magnons—in condensed matter systems at thermodynamic equilibrium. However, the most intriguing and puzzling many-body effects in open quantum systems often emerge from dissipative dynamics that are inherently out of equilibrium. Here, we use a combination of laser pumping and INS to experimentally observe long-lived nonequilibrium magnons in a two-dimensional (2D) square-lattice Heisenberg antiferromagnet. These nonequilibrium magnons manifest themselves as a violation of detailed balance in the dynamic structure factor and reach steady states under periodic driving, analogous to nonequilibrium steady states in driven dissipative systems. Furthermore, we show that the violation of detailed balance reflects the quantum-mechanical nature of the underlying dynamical system, where out-of-time-ordered correlations of creation and annihilation operators do not satisfy commutation relations. The in operando INS technique developed here provides a new approach to studying nonequilibrium magnons in prototypical 2D quantum magnets and can be extended to other systems, including one-dimensional spin chains and topological many-body spin systems, where nonequilibrium effects are widespread and rich in discovery potential.