Resonant ultrafast excitation of infrared-active phonons is a powerful technique with which to control the electronic properties of materials that leads to remarkable phenomena such as the light-induced enhancement of superconductivity^1,2, switching of ferroelectric polarization^3,4 and ultrafast insulator-to-metal transitions⁵. Here, we show that light-driven phonons can be utilized to coherently manipulate macroscopic magnetic states. Intense mid-infrared electric field pulses tuned to resonance with a phonon mode of the archetypical antiferromagnet DyFeO₃ induce ultrafast and long-living changes of the fundamental exchange interaction between rare-earth orbitals and transition metal spins. Non-thermal lattice control of the magnetic exchange, which defines the stability of the macroscopic magnetic state, allows us to perform picosecond coherent switching between competing antiferromagnetic and weakly ferromagnetic spin orders. Our discovery emphasizes the potential of resonant phonon excitation for the manipulation of ferroic order on ultrafast timescales⁶.

Magnonics is a research field complementary to spintronics, in which the quanta of spin waves (magnons) replace electrons as information carriers, promising lower dissipation^1–3. The development of ultrafast, nanoscale magnonic logic circuits calls for new tools and materials to generate coherent spin waves with frequencies as high and wavelengths as short as possible^4,5. Antiferromagnets can host spin waves at terahertz frequencies and are therefore seen as a future platform for the fastest and least dissipative transfer of information^6–11. However, the generation of short-wavelength coherent propagating magnons in antiferromagnets has so far remained elusive. Here we report the efficient emission and detection of a nanometre-scale wavepacket of coherent propagating magnons in the antiferromagnetic oxide dysprosium orthoferrite using ultrashort pulses of light. The subwavelength confinement of the laser field due to large absorption creates a strongly non-uniform spin excitation profile, enabling the propagation of a broadband continuum of coherent terahertz spin waves. The wavepacket contains magnons with a shortest detected wavelength of 125 nm that propagate into the material with supersonic velocities of more than 13 km s^–1. This source of coherent short-wavelength spin carriers opens up new prospects for terahertz antiferromagnetic magnonics and coherence-mediated logic devices at terahertz frequencies.

The microscopic origin of ultrafast modification of the ratio between the symmetric (J) and antisymmetric (D) exchange interaction in antiferromagnetic iron oxides is revealed, using femtosecond laser excitation as a pump and terahertz emission spectroscopy as a probe. By tuning the photon energy of the laser pump pulse we show that the effect of light on the D/J ratio in two archetypical iron oxides FeBO3 and ErFeO3 is maximized when the photon energy is in resonance with a spin and parity forbidden d-d transition between the crystal-field split states of Fe3+ ions. The experimental findings are supported by a multielectron model, which accounts for the resonant absorption of photons by Fe3+ ions. Our results reveal the importance of the parity and spin-change forbidden, and therefore often underestimated, d-d transitions in ultrafast optical control of magnetism.