具有强二次谐波活性和 Er3+ 近红外发光的非中心对称镧系 MOF 材料：在非线性光学测温中的应用,ACS Applied Materials & Interfaces

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具有强二次谐波活性和 Er3+ 近红外发光的非中心对称镧系 MOF 材料：在非线性光学测温中的应用
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-01-05 , DOI: 10.1021/acsami.2c22571
Marcin Runowski _{1,

2} , Dawid Marcinkowski ₂ , Kevin Soler-Carracedo ₁ , Adam Gorczyński ₂ , Ernest Ewert ₂ , Przemysław Woźny ₂ , Inocencio R Martín ₁

Affiliation

基于镧系离子的光学活性发光材料因其独特的光谱特性、非线性光学活性以及作为非接触式传感器应用的可能性而备受关注。具有强二次谐波产生 (SHG) 并且在 NIR 区域具有光学活性的镧系金属有机框架 (Ln-MOF) 出人意料地不足。此外，此类 Ln-MOF 需要手性配体和/或需要多步合成程序。^{在这里，我们展示了非中心对称、同构 Ln-MOF 材料（MOF-Er 3+} (1) 和共掺杂 MOF-Yb ³⁺ /Er ³⁺ ）的 NIR 脉冲激光照射(2)) 由简单的非手性有机底物通过一步法构建而成，可产生强大且可调谐的 SHG 活性。可以轻松收集 SHG 信号，在 ≈800 至 1500 nm 的宽 NIR 光谱范围内激发材料，从而在整个可见光谱区域观察到强烈的发射颜色。此外，在 ≈900 至 1025 nm 范围内激发时，该材料还表现出以 ≈1550 nm 为中心的 Er ^{3+离子的 NIR 发光。}使用 975 nm 脉冲激发可以同时观察 Er ^{3+的常规 NIR 发射}和 SHG 信号，完全由 Ln-MOF 材料的成分调整。利用上述效应的不同热响应优势，我们开发了一种基于镧系元素-MOF 材料的非线性光学温度计。在该系统中，SHG 信号随温度升高而降低，而 Er ³⁺的 NIR 发射带略微变宽，允许比率（Er ³⁺ NIR 1550 nm/SHG 488 nm）温度监测。我们的研究为合理设计具有所需光学和电子特性的现成和自监测 NLO 活性 Ln-MOFs 提供了基础。

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Noncentrosymmetric Lanthanide-Based MOF Materials Exhibiting Strong SHG Activity and NIR Luminescence of Er3+: Application in Nonlinear Optical Thermometry

Optically active luminescent materials based on lanthanide ions attract significant attention due to their unique spectroscopic properties, nonlinear optical activity, and the possibility of application as contactless sensors. Lanthanide metal-organic frameworks (Ln-MOFs) that exhibit strong second-harmonic generation (SHG) and are optically active in the NIR region are unexpectedly underrepresented. Moreover, such Ln-MOFs require ligands that are chiral and/or need multistep synthetic procedures. Here, we show that the NIR pulsed laser irradiation of the noncentrosymmetric, isostructural Ln-MOF materials (MOF-Er³⁺ (1) and codoped MOF-Yb³⁺/Er³⁺ (2)) that are constructed from simple, achiral organic substrates in a one-step procedure results in strong and tunable SHG activity. The SHG signals could be easily collected, exciting the materials in a broad NIR spectral range, from ≈800 to 1500 nm, resulting in the intense color of emission, observed in the entire visible spectral region. Moreover, upon excitation in the range of ≈900 to 1025 nm, the materials also exhibit the NIR luminescence of Er³⁺ ions, centered at ≈1550 nm. The use of a 975 nm pulse excitation allows simultaneous observations of the conventional NIR emission of Er³⁺ and the SHG signal, altogether tuned by the composition of the Ln-MOF materials. Taking the benefits of different thermal responses of the mentioned effects, we have developed a nonlinear optical thermometer based on lanthanide-MOF materials. In this system, the SHG signal decreases with temperature, whereas the NIR emission band of Er³⁺ slightly broadens, allowing ratiometric (Er³⁺ NIR 1550 nm/SHG 488 nm) temperature monitoring. Our study provides a groundwork for the rational design of readily available and self-monitoring NLO-active Ln-MOFs with the desired optical and electronic properties.

更新日期：2023-01-05

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