Blueprint for deterministic all-optical switching of magnetization

We resolve a significant controversy about how to understand and engineer single-shot all-optical switching of magnetization in ferrimagnets using femto- or picosecond-long heat pulses. By realistically modelling a generic ferrimagnet as two coupled macrospins, we comprehensively show that the net magnetization can be reversed via different pathways, using a heat pulse with duration spanning all relevant timescales within the non-adiabatic limit. This conceptual understanding is fully validated by experiments studying the material and optical limits at which the switching process in GdFeCo alloys loses its reliability. Our interpretation and results constitute a blueprint for understanding how deterministic all-optical switching can be achieved in alternative ferrimagnets using short thermal pulses.