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A new approach to all-optical detection and control of the coupling betweenelectric and magnetic order on ultrafast timescales is achieved usingtime-resolved second harmonic generation (SHG) to study a ferroelectric(FE)/ferromagnet (FM) oxide heterostructure. We use femtosecond optical pulsesto modify the spin alignment in aBa$_{0.1}$Sr$_{0.9}$TiO$_{3}$(BSTO)/La$_{0.7}$Ca$_{0.3}$MnO$_{3}$ (LCMO)heterostructure and selectively probe the ferroelectric response using SHG. Inthis heterostructure, the pump pulses photoexcite non-equilibriumquasiparticles in LCMO, which rapidly interact with phonons before undergoingspin-lattice relaxation on a timescale of tens of picoseconds. This reduces thespin-spin interactions in LCMO, applying stress on BSTO throughmagnetostriction. This then modifies the FE polarization through thepiezoelectric effect, on a timescale much faster than laser-induced heatdiffusion from LCMO to BSTO. We have thus demonstrated an ultrafast indirectmagnetoelectric effect in a FE/FM heterostructure mediated through elasticcoupling, with a timescale primarily governed by spin-lattice relaxation in theFM layer.

Using ultrashort optical pulses to couple ferroelectric and ferromagnetic order in an oxide heterostructure