AI 中文总结
研究通过手性二维钙钛矿中三次谐波产生圆二色性检测电信波段圆偏振光,发现隐藏的巨大各向异性,经偏振分辨分析分离手性贡献,实现不对称因子超1.9及相反手性响应提取,为相关技术提供平台。
AI 中文摘要
手性非线性光学(NLO)响应能够有效区分圆偏振光(CPL),在光学和光电子技术中备受关注。然而,手性材料的NLO性质研究主要集中在二阶NLO过程,三阶NLO过程中手性的作用仍未充分探索。本文通过手性二维钙钛矿(R/S-MBACl)2PbI4中的三次谐波产生圆二色性(THG-CD)演示了电信波段CPL检测,并发现了通过偏振分辨检测可获得的巨大隐藏THG-CD各向异性。偏振分辨THG测量表明,在正交THG偏振通道中出现相反的手性NLO响应。因此,这些手性各向异性贡献在总THG信号检测中相互抵消,导致基于总THG强度的传统评估中THG-CD不对称性被低估。通过分离这些隐藏的手性贡献,我们观察到异常大的不对称因子超过1.9,并实现了具有相反手性的手性NLO响应的选择性提取,而无需任何结构手性反转。这些发现突出了偏振分辨分析对于评估材料固有更准确手性NLO响应的重要性,并为电信相关波长的光学信息处理、加密和防伪技术提供了一个有前景的平台。
英文摘要
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.