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

TL;DR

This paper demonstrates an ultrafast all-optical method to control and detect the coupling between ferroelectric and ferromagnetic orders in an oxide heterostructure using femtosecond pulses and second harmonic generation.

Contribution

It introduces a novel ultrafast optical approach to induce and measure magnetoelectric coupling mediated by elastic interactions in a FE/FM heterostructure.

Findings

Ultrafast optical pulses modify spin alignment in the ferromagnetic layer.

The ferroelectric response is selectively probed using second harmonic generation.

The magnetoelectric effect occurs on a timescale governed by spin-lattice relaxation.

Abstract

A new approach to all-optical detection and control of the coupling between electric and magnetic order on ultrafast timescales is achieved using time-resolved second harmonic generation (SHG) to study a ferroelectric (FE)/ferromagnet (FM) oxide heterostructure. We use femtosecond optical pulses to modify the spin alignment in a Ba$_{0.1}$Sr$_{0.9}$TiO$_{3}$(BSTO)/La$_{0.7}$Ca$_{0.3}$MnO$_{3}$ (LCMO) heterostructure and selectively probe the ferroelectric response using SHG. In this heterostructure, the pump pulses photoexcite non-equilibrium quasiparticles in LCMO, which rapidly interact with phonons before undergoing spin-lattice relaxation on a timescale of tens of picoseconds. This reduces the spin-spin interactions in LCMO, applying stress on BSTO through magnetostriction. This then modifies the FE polarization through the piezoelectric effect, on a timescale much faster than laser-induced heat diffusion from LCMO to BSTO. We have thus demonstrated an ultrafast indirect magnetoelectric effect in a FE/FM heterostructure mediated through elastic coupling, with a timescale primarily governed by spin-lattice relaxation in the FM layer.