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<p>A high-quality non-centrosymmetric coordination single crystal of bis(5,5′-((butane-1,4-diylbis(azanylylidene))bis(methanylylidene))bis(3-(ethoxycarbonyl)-2,4-dimethylpyrrol-1-idok<sup>4</sup>N,N′,N′′,N′′′)copper(II) (BAMEMC), C<sub>24</sub>H<sub>32</sub>CuN<sub>4</sub>O<sub>4</sub>, was successfully grown by an optimized slow evaporation solution growth method using an ethanol–THF mixed solvent system under controlled crystallization conditions. The crystal was comprehensively characterized by single-crystal X-ray diffraction, UV–visible spectroscopy, laser damage threshold (LDT), particle size-dependent second-harmonic generation (SHG), temperature-dependent SHG with differential scanning calorimetry (DSC), and terahertz time-domain spectroscopy (THz-TDS) to establish the correlation between its crystal structure and multifunctional photonic properties. Although the crystal structure of BAMEMC has been previously reported, its integrated nonlinear optical, thermally switchable, and terahertz photonic characteristics have not been investigated. Single-crystal X-ray diffraction confirmed crystallization in the polar non-centrosymmetric monoclinic Cc space group. The crystal exhibited an optical cut-off wavelength of 316&#xa0;nm, approximately 77% visible-region transmittance, and a laser damage threshold of 1.296 GW&#xa0;cm⁻<sup>2</sup>, demonstrating good optical quality and resistance to high-power laser irradiation. Kurtz–Perry measurements revealed a relative SHG efficiency of 3.27 times that of KDP, while temperature-dependent SHG measurements supported by DSC confirmed a reversible thermally induced nonlinear optical switching process associated with a reversible thermal transition. THz-TDS further demonstrated coherent broadband terahertz emission under femtosecond optical excitation. These results establish, for the first time, an experimental correlation between the polar coordination framework of BAMEMC and its nonlinear optical conversion efficiency, reversible thermal switching, laser damage resistance, and ultrafast terahertz response, thereby significantly extending the functional importance of this previously reported coordination SDG&#xa0;crystal for advanced nonlinear optical, terahertz photonic, and optoelectronic applications.</p>

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Engineering a terahertz-active polar BAMEMC sustainable single crystal for reversible nonlinear optical switching and enhanced frequency conversion

  • 期刊论文

  • 发表日期：

    2026年7月31日

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  • P. Vivek

摘要

A high-quality non-centrosymmetric coordination single crystal of bis(5,5′-((butane-1,4-diylbis(azanylylidene))bis(methanylylidene))bis(3-(ethoxycarbonyl)-2,4-dimethylpyrrol-1-idok4N,N′,N′′,N′′′)copper(II) (BAMEMC), C24H32CuN4O4, was successfully grown by an optimized slow evaporation solution growth method using an ethanol–THF mixed solvent system under controlled crystallization conditions. The crystal was comprehensively characterized by single-crystal X-ray diffraction, UV–visible spectroscopy, laser damage threshold (LDT), particle size-dependent second-harmonic generation (SHG), temperature-dependent SHG with differential scanning calorimetry (DSC), and terahertz time-domain spectroscopy (THz-TDS) to establish the correlation between its crystal structure and multifunctional photonic properties. Although the crystal structure of BAMEMC has been previously reported, its integrated nonlinear optical, thermally switchable, and terahertz photonic characteristics have not been investigated. Single-crystal X-ray diffraction confirmed crystallization in the polar non-centrosymmetric monoclinic Cc space group. The crystal exhibited an optical cut-off wavelength of 316 nm, approximately 77% visible-region transmittance, and a laser damage threshold of 1.296 GW cm⁻2, demonstrating good optical quality and resistance to high-power laser irradiation. Kurtz–Perry measurements revealed a relative SHG efficiency of 3.27 times that of KDP, while temperature-dependent SHG measurements supported by DSC confirmed a reversible thermally induced nonlinear optical switching process associated with a reversible thermal transition. THz-TDS further demonstrated coherent broadband terahertz emission under femtosecond optical excitation. These results establish, for the first time, an experimental correlation between the polar coordination framework of BAMEMC and its nonlinear optical conversion efficiency, reversible thermal switching, laser damage resistance, and ultrafast terahertz response, thereby significantly extending the functional importance of this previously reported coordination SDG crystal for advanced nonlinear optical, terahertz photonic, and optoelectronic applications.