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首页> 外文期刊>Journal of the American Chemical Society >Length-Dependent Convergence and Saturation Behavior of Electrochemical, Linear Optical, Quadratic Nonlinear Optical, and Cubic Nonlinear Optical Properties of Dipolar Alkynylruthenium Complexes with Oligo(phenyleneethynylene) Bridges
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Length-Dependent Convergence and Saturation Behavior of Electrochemical, Linear Optical, Quadratic Nonlinear Optical, and Cubic Nonlinear Optical Properties of Dipolar Alkynylruthenium Complexes with Oligo(phenyleneethynylene) Bridges

机译：带有寡（亚苯基亚乙炔基）桥的偶极炔钌络合物的电化学，线性光学，二次非线性光学和立方非线性光学性质的长度依赖性收敛和饱和行为

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摘要

The syntheses of frans-[Ru{4,4'-C-CC_6H_2[2>5-(OEt)_2]C=CC_6H_4NO_2}CI(dppm)_2] (19), trans-[Ru{4,4',4"-C=CC_6H_4C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_4NO_2}CI(dppm)_2](20), trans-[Ru{4,4',4",4'"-C=CC_6H_(4~-) C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_4NO_2}CI(dppe)_2](21), frans-[Ru{4,4',4",4'"-C=CC_6H_(4~-) C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_4NO_2}CI(dppm)_2](22), frans-[Ru{4,4',4",4'"-C=CC_6H_4C= CC_6H_4C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_4NO_2}CI(dppm)_2] (23), and frans-[Ru{4,4',4",4'",4""-C=CC_6H_(4~-) C=CC_6H_4C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_2[2,5-(OEt)_2]C=CC_6H_4NO_2}CI(dppm)_2] (24) are reported, together with those of precursor alkynes, complexes with the donor-π-bridge-acceptor formulation that affords efficient quadratic and cubic NLO compounds; the identity of 19 was confirmed by a structural study. The electrochemical properties of 19-24 and related complexes with shorter π-bridge ligands were assessed by cyclic voltammetry, and the linear optical, quadratic nonlinear optical, and cubic nonlinear optical properties were assayed by UV-vis-NIR spectroscopy, hyper-Rayleigh scattering studies at 1064 and 1300 nm, and broad spectral range femtosecond Z-scan studies, respectively. The Ru~(II/III) oxidation potentials and wavelengths of the optical absorption maxima decrease on jr-bridge lengthening, until the tri(phenylene-ethynylene) complex is reached, further chain lengthening leaving these parameters invariant; theoretical studies employing time-dependent density functional theory have shed light on this behavior. The quadratic nonlinearity β_(1064) and two-photon absorption cross-section reach maximal values at this same π-bridge length, a similar saturation behavior that may reflect a common importance of ruthenium-to-alkynyl ligand charge transfer in electronic and optical behavior in these molecules.
机译：反式-[Ru {4,4'-C-CC_6H_2 [2> 5-（OEt）_2] C = CC_6H_4NO_2} CI（dppm）_2]（19），反式-[Ru {4,4'， 4“ -C = CC_6H_4C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_4NO_2} CI（dppm）_2]（20），反式[Ru {4,4'，4”，4'“-C = CC_6H_（4〜-）C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_4NO_2} CI（dppe）_2]（21），frans- [ Ru {4,4'，4“，4'”-C = CC_6H_（4〜-）C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_4NO_2} CI（dppm）_2]（22），法兰-[Ru {4,4'，4“，4'”-C = CC_6H_4C = CC_6H_4C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_4NO_2} CI（dppm）_2]（23），以及法兰形-[Ru {4,4'，4“，4'”，4“”-C = CC_6H_（4〜-）C = CC_6H_4C = CC_6H_2 [2,5-据报道（OEt）_2] C = CC_6H_2 [2,5-（OEt）_2] C = CC_6H_4NO_2} CI（dppm）_2]（24）与前体炔烃一起与施主-π-桥复合。受体配方可提供有效的二次和立方NLO化合物；通过结构研究证实了19的身份；通过循环伏安法评估了19-24和具有较短π桥配体的相关配合物的电化学性能，以及线性，二次光学ñ分别通过UV-vis-NIR光谱，1064和1300 nm处的超瑞利散射研究以及宽光谱范围的飞秒Z扫描研究了线性光学和立方非线性光学性质。 Ru-（II / III）氧化电位和光吸收最大值的波长随着jr-桥的加长而减小，直到达到三苯撑-乙炔基络合物为止，进一步的链延长使这些参数不变。使用时变密度泛函理论的理论研究阐明了这种行为。二次非线性β_（1064）和双光子吸收截面在相同的π桥长度处达到最大值，相似的饱和行为可能反映了钌到炔基配体电荷转移在电子和光学行为中的共同重要性在这些分子中。

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  • 来源
    《Journal of the American Chemical Society》 |2009年第29期|10293-10307|共15页
  • 作者

    Bandar Babgi; Luca Rigamonti; Marie P. Cifuentes; T. Christopher Corkery; Michael D. Randiest; Torsten Schwich; Simon Petrie; Robert Stranger; Ayele Teshome; Inge Asselberghs; Koen Clays; Marek Samoc; Mark G. Humphrey;

  • 作者单位

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia Dipartimento di Chimica Inorganica, Metallorganica e Analitica 'Lamberto Malatesta', Universita degli Studi di Milano, Via Venezian 21, 20133 Milano, Italy;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

    Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium, Laser Physics Centre, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200, Australia;

    Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium, Laser Physics Centre, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200, Australia;

    Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium, Laser Physics Centre, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200, Australia;

    Department of Chemistry, University of Leuven, Celestijnenlaan 200D, B-3001 Leuven, Belgium, Laser Physics Centre, Research School of Physics and Engineering, Australian National University, Canberra, ACT 0200, Australia Institute of Physical and Theoretical Chemistry, Wroclaw University of Technology, 50-370 Wroclaw, Poland;

    Research School of Chemistry, Australian National University, Canberra, ACT 0200, Australia;

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