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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Optimizing simultaneous two-photon absorption and transient triplet-triplet absorption in platinum acetylide chromophores
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Optimizing simultaneous two-photon absorption and transient triplet-triplet absorption in platinum acetylide chromophores

机译：优化乙炔铂生色团的同时双光子吸收和瞬态三重态-三重态吸收

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A series of platinum-containing organometallic dimer complexes has been synthesized and the photophysical properties have been investigated under one- and two-photon (2PA) absorption conditions. The complexes have the general structure [DPAF-C - C-Pt(PBu_3)_2-C≡C-Ar-C≡C- Pt(PBu_3)_2-C≡C-DPAF], where Ar is a π-conjugated unit, Bu = n-butyl, and DPAF = diphenylamino-2,7-fluorenylene. The core Ar units include 1,4-phenylene, 2,5-thienylene, 5,5′-(2,2′-bithienylene), 2,5-(3,4-ethylenedioxythiophene, 2,1,3-benzothiadiazole, and 4,7-dithien-2-yl-2,1,3-benzothiadiazole. Absorption and photoluminescence spectroscopy indicates that the complexes feature low-lying excited states based on both the core [-Pt(PBu_3)_2-C≡C-Ar-C≡C- Pt(PBu_3)_2-] chromophore as well as the DPAF units. Photoexcitation of the complexes produces a singlet state excited state, which rapidly undergos intersystem crossing to afford a triplet state that has a lifetime in the microsecond time domain. In most cases, the lowest energy triplet state is localized on the core chromophore. Femtosecond 2PA spectra are measured along with triplet-triplet absorption spectra and nanosecond intensity-dependent transmission for solutions of the complexes. Each of the complexes features a 2PA absorption band in the near-infrared region (λ ≈ 700-750 nm) with a cross section 50-200 GM that is ascribed to the DPAF chromophore. The complexes also feature broad triplet-triplet absorption throughout the visible and near-infrared regions (λ ≈ 500-800 nm, ∈_(TT) ≈ 5-10 ×10~4 M~(-1) cm ~(-1)). Each of the complexes exhibits efficient nonlinear absorption of nanosecond pulses in the near-infrared region (600-800 nm), and we demonstrate that effect is most efficient in the chromophores where the 2PA cross section maxima coincides spectrally with the excited triplet state absorption.
机译：合成了一系列含铂的有机金属二聚体配合物，并在单光子和双光子（2PA）吸收条件下研究了光物理性质。配合物具有一般结构[DPAF-C-C-Pt（PBu_3）_2-C≡C-Ar-C≡C-Pt（PBu_3）_2-C≡C-DPAF]，其中Ar是π共轭单元，Bu ＝正丁基，和DPAF ＝二苯基氨基-2，7-亚芴基。核心Ar单元包括1,4-亚苯基，2,5-亚噻吩基，5,5'-（2,2'-亚噻吩基），2,5-（3,4-乙撑二氧噻吩，2,1,3-苯并噻二唑，和4,7-二噻吩-2-基-2,1,3-苯并噻二唑。吸收和光致发光光谱表明，该络合物基于两个核心[-Pt（PBu_3）_2-C≡C- Ar-C≡C-Pt（PBu_3）_2-]生色团和DPAF单元的光激发产生单重态激发态，该态迅速经历系统间交叉，从而获得具有微秒寿命的三重态。在大多数情况下，最低能量的三重态处于核心生色团上，飞秒2PA光谱与三重态-三重态吸收光谱和纳秒强度相关的透射率一起用于复合物的溶液测量，每个复合物均具有2PA吸收归因于DPAF色度的横截面为50-200 GM的近红外区域（λ≈700-750 nm） phor配合物在可见光和近红外区域（λ≈500-800 nm，ε_（TT）≈5-10×10〜4 M〜（-1）cm〜（-1）处具有广泛的三重态三重态三重吸收。 ）。每个配合物在近红外区（600-800 nm）处均表现出纳秒脉冲的有效非线性吸收，并且我们证明了在2PA截面最大值与激发三重态吸收光谱符合的发色团中，该效应最为有效。

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