Electrically switchable chiral nonlinear optics in an achiral ferroelectric 2D van der Waals halide perovskite.

Abstract

Two-dimensional (2D) van der Waals (vdW) semiconductors play a key role in developing nanoscale nonlinear optical devices. 2D Ruddlesden-Popper lead halide perovskites (RPPs) expand the potential of using 2D vdW semiconductors in nonlinear optical applications because they exhibit electrically switchable and chiral second-order optical nonlinearity originating from the emergence of ferroelectricity and chirality. However, electrically switchable chiral nonlinear optics has not yet been realized because of the difficulty in electrically manipulating chiral structures. Here, we demonstrate that chiral second-harmonic generation (SHG) can be electrically induced and switched in an achiral biaxial ferroelectric 2D RPP. We observe reversible and continuous electrical switching of SHG circular dichroism and large nonlinear chiroptical activity. Polarization-resolved SHG imaging reveals that electrical poling induces the ferroelectric multidomain structure arising from the biaxial nature of the material, and the planar chirality appears. Our findings show a simple electrical control of the nonlinear chiroptical responses and establish chiral nonlinear optics based on ferroelectric 2D RPPs.