Optical anisotropy enables both linear and nonlinear optical properties, enabling applications such as polarizing optics, frequency upconversion, and electro-optic (EO) modulation. EO modulation relies on optical anisotropy and the changes to it that occur under electric fields. Optical anisotropy originates from a lack of symmetry in the material's structure: when a material lacks inversion symmetry, second-order nonlinear optical effects can occur. The linear EO effect, or Pockels effect, is of use in optical modulation for network interconnection and telecommunications.Silicon photonics offers the possibility of condensing optical interconnects to intra-/interchip length scales. However, silicon-based EO modulators that exploit the plasma dispersion effect suffer from significant energy losses incurred in changing the carrier density; and they also require large device footprints, in light of a weak index change, that stand in the way of high-speed operation. [1] The integration of high-performance nonlinear optical materials within photonic waveguides is therefore desired. The inorganic nonlinear crystals such as lithium niobate (LNO) and barium titanate (BTO) possess high phase transition temperatures (above 120 °C) [2,3] and large coercive field strengths (greater than 10 5 V m −1 ); [2] however, the integration of inorganic nonlinear crystals relies on costly and complicated bonding or deposition processes (heterogeneous integration). [4,5] Organic nonlinear optical molecules can be solution processed, and therefore offer convenient integration with on-chip photonic structures. [6][7][8] However, such organic molecules, which (individually) have impressively high EO coefficients, lose performance when they depole in light of thermodynamic instabilities in ordered films of organic molecules. [9,10] The past decade has seen the rapid development of metal halide perovskite optoelectronics, including solar cells, light emitting diodes, lasers, and detectors. These materials are highly crystalline and can be solution processed, enabling integration with photonic structures. The most widely studied metal halide perovskites, which features the chemical structure APbX 3
Rapid and efficient conversion of electrical signals to optical signals is needed in telecommunications and data network interconnection. The linear electro-optic (EO) effect in noncentrosymmetric materials offers a pathway to such conversion. Conventional inorganic EO materials make on-chipintegration challenging, while organic nonlinear molecules suffer from thermodynamic molecular disordering that decreases the EO coefficient of the material. It has been posited that hybrid metal halide perovskites could potentially combine the advantages of inorganic materials (stable crystal orientation) with those of organic materials (solution processing). Here, layered metal halide perovskites are reported and investigated for in-plane birefringence and linear electro-optic response. Phenylmethylammonium lead chloride (PMA 2 PbCl 4 ) crystals are grown that...