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配体环境化学计量对钐、镨和钕离子配位化合物近红外发光效率的影响

Influence of Ligand Environment Stoichiometry on NIR-Luminescence Efficiency of Sm, Pr and Nd Ions Coordination Compounds.

作者信息

Polikovskiy Trofim, Korshunov Vladislav, Metlin Mikhail, Gontcharenko Viktoria, Metlina Darya, Datskevich Nikolay, Kiskin Mikhail, Belousov Yury, Tsorieva Alisia, Taydakov Ilya

机构信息

P. N. Lebedev Physical Institute of the Russian Academy of Sciences, 53 Leninskiy 1. Prospect, 119991 Moscow, Russia.

Faculty of Chemistry, National Research University Higher School of Economics, 20 Miasnitskaya Str., 101000 Moscow, Russia.

出版信息

Molecules. 2023 Aug 5;28(15):5892. doi: 10.3390/molecules28155892.

DOI:10.3390/molecules28155892
PMID:37570861
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10421502/
Abstract

Six new complexes of the ligand HQ (-4-(cyclohexanecarbonyl)-5-methyl-2-phenyl-2,4-dihydro-3H-pyrazol-3-one) and Ln ions with emission in the near-infrared (Nd) or visible and near-infrared (Sm, Pr) spectral regions were synthesized and characterized using various methods, including single crystal X-ray diffraction. The study demonstrated that both tris complexes [LnQ(HO)(EtOH)] and tetrakis-acids [HO][LnQ] can be synthesized by varying the synthetic conditions. The photochemical properties of the complexes were investigated experimentally and theoretically using various molecular spectroscopy techniques and Judd-Ofelt theory. The objective was to quantitatively and qualitatively disclose the influence of complex stoichiometry on its luminescence properties. The study showed that the addition of an extra ligand molecule (in the tetrakis species) increased molar extinction by up to 2 times, affected the shape of photoluminescence spectra, especially of the Pr complex, and increased the quantum yield of the Sm complex by up to 2 times. The results obtained from this study provide insights into the luminescent properties of lanthanide coordination compounds, which are crucial for the design and development of novel photonic materials with tailored photophysical properties.

摘要

合成了六种新的配体HQ（-4-（环己烷羰基）-5-甲基-2-苯基-2,4-二氢-3H-吡唑-3-酮）与镧系离子形成的配合物，其在近红外（钕）或可见光和近红外（钐、镨）光谱区域有发射，并使用包括单晶X射线衍射在内的各种方法对其进行了表征。研究表明，通过改变合成条件，可以合成三配位配合物[LnQ(HO)(EtOH)]和四配位酸[HO][LnQ]。使用各种分子光谱技术和贾德-奥费尔特理论，对配合物的光化学性质进行了实验和理论研究。目的是定量和定性地揭示配合物化学计量比对其发光性质的影响。研究表明，额外添加一个配体分子（在四配位物种中）使摩尔消光系数增加了两倍，影响了光致发光光谱的形状，特别是镨配合物的光谱形状，并使钐配合物的量子产率提高了两倍。这项研究所得结果为镧系配位化合物的发光性质提供了见解，这对于设计和开发具有定制光物理性质的新型光子材料至关重要。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/ab8e3e4daded/molecules-28-05892-g012.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/ab8e3e4daded/molecules-28-05892-g012.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/f25cef8b6488/molecules-28-05892-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/f63117aca517/molecules-28-05892-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/1f3446b83695/molecules-28-05892-g002.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c261/10421502/ab8e3e4daded/molecules-28-05892-g012.jpg

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