Terahertz field-driven magnon upconversion in an antiferromagnet

Tailored light excitation and nonlinear control of lattice vibrations have emerged as powerful strategies to manipulate the properties of quantum materials out of equilibrium. Generalizing the use of coherent phonon-phonon interactions to nonlinear couplings among other types of collective modes would open unprecedented opportunities in the design of novel dynamic functionalities in solids. For example, the collective excitations of magnetic order -- magnons -- can carry information with little energy dissipation, and their coherent and nonlinear control would provide an attractive route to achieve collective-mode-based information processing and storage in forthcoming spintronics and magnonics. Here, we discover that intense terahertz (THz) fields can initiate processes of magnon upconversion mediated by an intermediate magnetic resonance. By using a suite of advanced spectroscopic tools, including a newly demonstrated two-dimensional (2D) THz polarimetry technique enabled by single-shot detection, we unveil the unidirectional nature of coupling between distinct magnon modes of a canted antiferromagnet. Calculations of spin dynamics further suggest that this coupling is a universal feature of antiferromagnets with canted magnetic moments. These results demonstrate a route to inducing desirable energy transfer pathways and THz-induced coupling between coherent magnons in solids and pave the way for a new era in the development of ultrafast control of magnetism.