Electric-field-enhanced second-harmonic domain contrast and nonreciprocity in a van der Waals antiferromagnet

Abstract Imaging antiferromagnetic 180° domains with actively controlled visibility is vital for both fundamental science and sophisticated applications. While optical second-harmonic generation (SHG) is a well-known technique for distinguishing such domains in non-centrosymmetric antiferromagnets, a general material-based strategy to control domain contrast remains elusive. Using van der Waals antiferromagnet MnPS3 as a proof of concept, we demonstrate the tuning of nonreciprocity-induced domain contrast in SHG through applying an in-plane electric field that transforms the magnetic point group to its unitary subgroup. The interference among intrinsic electric-dipole, magnetic-dipole, and field-induced electric-dipole transitions, each carrying distinct characters under space-inversion ( $${{\mathcal{P}}}$$ P ) and time-reversal ( $${{\mathcal{T}}}$$ T ) operations, enables large tuning of domain contrast and nonreciprocity in a broad spectral range. This strategy, generically applicable to systems characterized by $${{\mathcal{P}}}{{\mathcal{T}}}$$ P T -symmetric magnetic groups with a polar unitary subgroup, offers a path to fast electrical modulation of nonlinear nonreciprocal photonic behaviors using antiferromagnets.