Modeling the Ultrafast Response of Two-Magnon Raman Excitations in Antiferromagnets on the Femtosecond Timescale

Illuminating a magnetic material with femtosecond laser pulses induces complex ultrafast dynamical processes. The resulting optically detectable response usually contains contributions from both the optical properties and the magnetic degrees of freedom. Disentangling all the different components concurring to the generation of the total signal is a major challenge of contemporary experimental solid-state physics. Here, this problem is tackled, addressing the purely optical, nonmagnetic artifacts on the time resolved two-magnon stimulated Raman spectrum of an antiferromagnet, rationalizing the recent observation on the exchange energy modification upon photo-excitation. It is demonstrated how the genuine dynamics of the magnetic eigenmode can be disentangled from the nonlinear optical effects, generated by cross phase modulation, on the femtosecond timescale. The introduced approach can be extended for the investigation of <100 fs dynamic processes by means of coherent Raman scattering.