2016
DOI: 10.1021/acs.jpcc.6b04434
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High Second-Order NLO Response Exhibited by the First Example of Polymeric Film Incorporating a Diimine–Dithiolate Square-Planar Complex: The [Ni(o-phen)(bdt)]

Abstract: A novel square-planar diimine−dithiolate nonlinear optical (NLO) chromophore, the complex [Ni(ophen)(bdt)] (1), is reported in this paper (o-phen = dianion of 1,2-phenylendiamina; bdt =1,2-benzenedithiolate). This compound has been fully characterized by single-crystal X-ray diffraction, UV−vis−NIR spectroscopy, cyclic voltammetry, DFT, and TD-DFT calculations. 1 crystallizes in the P 21 space group and shows an almost planar molecule. The cyclic voltammetry measurements present an irreversible anodic peak at … Show more

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Cited by 2 publications
(3 citation statements)
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“…[3][4][5] Square-planar heteroleptic d 8 -metal-dithiolene complexes, have been shown to work as tunable second-order NLO chromophores. [6][7][8][9][10][11] The requirement to obtain this property is achieved with the presence of two ligands occurring in formally different oxidation states, one reducing (dianionic = dithiolate, electron Donor = D), and the other oxidizing (neutral = dithione or diimine, electron Acceptor = A), with the metal (M) acting as a -bridge. These noncentrosymmetric molecules (D-M-A), exhibit an absorption peak in the visible spectral region, which is tunable with the HOMO-LUMO energy gap.…”
Section: Introductionmentioning
confidence: 99%
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“…[3][4][5] Square-planar heteroleptic d 8 -metal-dithiolene complexes, have been shown to work as tunable second-order NLO chromophores. [6][7][8][9][10][11] The requirement to obtain this property is achieved with the presence of two ligands occurring in formally different oxidation states, one reducing (dianionic = dithiolate, electron Donor = D), and the other oxidizing (neutral = dithione or diimine, electron Acceptor = A), with the metal (M) acting as a -bridge. These noncentrosymmetric molecules (D-M-A), exhibit an absorption peak in the visible spectral region, which is tunable with the HOMO-LUMO energy gap.…”
Section: Introductionmentioning
confidence: 99%
“…To overcome this drawback, NLO chromophores are embedded into polymeric poled films. 11,14,42 To obtain a sufficiently stable second-harmonic generation (SHG) signal of thin films, chromophores are required to possess suitable properties (good solubility, thermal stability, no aggregation for stacking) to be incorporated homogeneously in the host matrix of poled film and remain so within the time. To meet these requirements, we are investigating square-planar heteroleptic d 8 -metaldithiolene 6,[12][13][14][15] characterized by remarkable high negative molecular first hyperpolarizability both at the molecular level and in the bulk.…”
Section: Introductionmentioning
confidence: 99%
“…Metal dithiolates are highly tunable , and have a wide range of applications and properties, including catalysis in water splitting and olefin transformations, proton-coupled electron transfer, nonlinear optical responses, and molecular conductivity and magnetization. We examine the oxidation series of bis­(ethylene-1,2-dithiolato) nickel or [Ni­(edt) 2 ] (−2,–1,0) , where edt is ethylene dithiolate ligand (Figure ), which is paradigmatic of other more substituted nickel dithiolate complexes. , …”
Section: Introductionmentioning
confidence: 99%