Dynamical Nonrelativistic Spin Splitting via THz Nonlinear Phononics

Abstract

Nonrelativistic spin splitting (NRSS) in collinear antiferromagnets offers a route to high-frequency spintronics immune to stray fields, but its dynamic control has remained elusive. We demonstrate, using density functional theory (DFT) and nonlinear phononics, that THz laser pulses can achieve ultrafast, reversible control of NRSS on picosecond timescales in antiferromagnets. We derive two symmetry criteria, accounting for phonon and magnetic wavevector compatibility and order-parameter parity, to identify which Raman-active phonon modes can activate or amplify NRSS. Applying these rules to NiO and LaFeO$_3$, we show that resonant driving of an infrared-active mode at 11.08 THz transiently converts spin-degenerate NiO into an NRSS state via biquadratic anharmonic coupling, generating a time-averaged spin splitting of $\sim$40 meV. In LaFeO$_3$, selective excitation amplifies the existing NRSS by about 100%. In both cases, the induced spin splitting is accompanied by a transient SOC-induced net moment detectable via the magneto-optical Kerr effect. This framework establishes nonlinear phononics as a general route for ultrafast manipulation of spin-split antiferromagnetic phases well beyond the reach of static strain.