Giant Birefringence and Strong Third-Order Nonlinear Optical Response in a Hybrid Crystal Templated by a Push–Pull π-Conjugated System

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-07-31 DOI:10.1021/acsmaterialslett.5c00786

Sivasubramani Vediyappan, Zilong Chen, Xu Die, Zhihua Yang, Luyong Zhang, Xueling Hou*, Fangfang Zhang*, Senthil Pandian Muthu and P. Ramasamy*,

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Abstract

High-performance birefringent and third-order nonlinear optical (NLO) crystals are indispensable components of advanced photonic devices owing to their excellent ability to precisely modulate light polarization. The conventional hybrid organic–inorganic (HOI) crystals often suffer from intrinsic limitations that hinder their performance. In contrast, our novel strategy employs a distinctive π-conjugated organic functional unit with an optimized push–pull configuration further integrated into a robust metal-halide framework. The novel crystal, namely, (C₅H₅N₃O₂)₂ZnCl₂ (2A5NPZC), represents a novel paradigm in HOI design and exhibits remarkable properties, including bulk crystal (15 × 7 × 4 mm³), giant refractive index difference (0.40 at 514 nm (exp)), a high third-order NLO susceptibility (χ⁽³⁾ = 4.442 × 10^–9 esu), excellent optical transmittance range (415–1400 nm), and superior optical limiting capability (6.3 mW/cm² at 532 nm). Our findings highlight the broader potential of push–pull-type π-conjugated units as a versatile platform for the rational design of high-performance materials well-suited for advanced photonic technologies.

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推拉π共轭体系模板化杂化晶体的巨大双折射和强三阶非线性光学响应

高性能双折射和三阶非线性光学晶体具有精确调制光偏振的优异性能，是先进光子器件不可缺少的组成部分。传统的有机-无机杂化晶体（HOI）往往受到固有的限制，阻碍了它们的性能。相比之下，我们的新策略采用了独特的π共轭有机功能单元，其优化的推拉结构进一步集成到坚固的金属卤化物框架中。新型晶体（C5H5N3O2）2ZnCl2 （2A5NPZC）代表了HOI设计的新范例，具有显著的性能，包括体积晶体（15 × 7 × 4 mm3），巨大的折射率差（514 nm处0.40 (exp)），高三阶NLO敏感性（χ(3) = 4.442 × 10-9 esu），优异的光学透过率范围（415-1400 nm）和优越的光学限制能力（532 nm处6.3 mW/cm2）。我们的研究结果突出了推拉型π共轭单元作为合理设计高性能材料的通用平台的广阔潜力，这些材料非常适合先进的光子技术。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.