Telecom-band Chiral Light Detection through Hidden Giant Third-Order Nonlinear Circular Dichroism in Two-dimensional Halide Perovskite

Abstract

Chiral nonlinear optical (NLO) responses enable efficient discrimination of circularly polarized light (CPL) and are attracting increasing interest for optical and optoelectronic technologies. However, studies on NLO properties in chiral materials have largely focused on second-order NLO processes, while the role of chirality in third-order NLO processes remains poorly explored. Here, we demonstrate telecom-band CPL detection by third harmonic generation circular dichroism (THG-CD) in the chiral two-dimensional perovskite (R/S-MBACl)2PbI4 and uncover a giant hidden THG-CD anisotropy that is accessible via polarization-resolved detection. Polarization-resolved THG measurements reveal that opposite chiral NLO responses emerge in orthogonal THG polarization channels. Therefore, these chiral anisotropic contributions largely cancel each other in the total-THG signal detection, leading to underestimation of the THG-CD dissymmetry in conventional evaluations based on total-THG intensity. By separating these hidden chiral contributions, we observe exceptionally large dissymmetry factors exceeding 1.9 and achieve selective extraction of chiral NLO responses with opposite handedness, without any structural chiral inversion. These findings highlight the importance of polarization-resolved analysis for evaluating more accurate chiral NLO responses inherent to the material and provide a promising platform for optical information processing, encryption, and anti-counterfeiting technologies at technologically relevant telecommunication wavelengths.