Two chiral EuIII and SmIII enantiomeric pairs with enantiopure N-donor ligands: showing strong third-harmonic generation and photoluminescence properties†

IF 2.6 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY CrystEngComm Pub Date : 2024-11-01 DOI:10.1039/D4CE01052C

Jinliang Zhang, Zhiqiang Zhang, Congli Gao and Xi-Li Li

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Abstract

The reaction of the precursors Eu(dbm)₃(H₂O) and Sm(dbm)₃(H₂O) with enantiopure monobidentate N-donor ligands (L_R/L_S), respectively, afforded two chiral Eu^III and Sm^III enantiomeric pairs, namely Ln(dbm)₃(L_R)/Ln(dbm)₃(L_S) (Ln = Eu^III, D-1/L-1 and Ln = Sm^III, D-2/L-2), where dbm⁻ = dibenzoylmethanate and L_R/L_S = (−)/(+)-4,5-pinenepyridyl-2-pyrazine. Compared with their precursors, D-1 and D-2 display highly enhanced photophysical properties under excitation with visible light. A study of nonlinear optical (NLO) response reveals that Eu(dbm)₃(H₂O) and Sm(dbm)₃(H₂O) only show moderate second-harmonic generation (SHG) responses, while D-1/L-1 and D-2/L-2 only exhibit strong third-harmonic generation (THG) responses. The THG intensities of D-1/L-1 and D-2/L-2 are 62/59 and 56/58 × α-SiO₂, respectively. These findings clearly indicate that introducing L_R and L_S into Eu(dbm)₃(H₂O) and Sm(dbm)₃(H₂O) can not only highly boost the photophysical performances but also lead to the switching of the NLO responses from SHG to THG.

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具有对映不纯n给体的两个手性EuIII和SmIII对映体：表现出强三次谐波生成和光致发光特性

前体Eu(dbm)3（H2O）和Sm(dbm)3（H2O）分别与对映纯单齿n给体（LR/LS）反应，得到两个手性EuIII和SmIII对映体，即Ln(dbm)3(LR)/Ln(dbm)3(LS) (Ln = EuIII， D-1/L-1和Ln = SmIII, D-2/L-2)，其中dbm−=二苯甲酰甲烷，LR/LS =(−)/(+)-4,5-蒎烯吡啶-2-吡嗪。与前驱体相比，D-1和D-2在可见光激发下表现出高度增强的光物理性质。非线性光学（NLO）响应研究表明，Eu(dbm)3（H2O）和Sm(dbm)3（H2O）仅表现出中等的二次谐波（SHG）响应，而D-1/L-1和D-2/L-2仅表现出强烈的三次谐波（THG）响应。D-1/L-1和D-2/L-2的THG强度分别为62/59和56/58 × α-SiO2。这些结果清楚地表明，在Eu(dbm)3（H2O）和Sm(dbm)3（H2O）中引入LR和LS不仅可以显著提高光物理性能，而且可以导致NLO响应从SHG转换为THG。

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