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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >The Early Picosecond Photophysics of Ru(II)Polypyridyl Complexes:A Tale of Two Timescales
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The Early Picosecond Photophysics of Ru(II)Polypyridyl Complexes:A Tale of Two Timescales

机译：Ru（II）多吡啶配合物的早期皮秒光物理：两个时标的故事

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摘要

The early picosecond time scale excited-state dynamics of the paradigm tris(2,2'-bipyridyl)Ruthenium(II)([Ru(bpy)3]~(2+))and related complexes have been examined by picosecond Kerr-gated time-resolved resonance Raman(ps-TR3)spectroscopy.The evolution of the signature Raman bands of the lowest thermally equilibrated excited(THEXI)state under two-color pump/probe conditions show that this state is not fully populated within several hundred femtoseconds as proposed previously but rather only within the first 20 ps following excitation.In addition to an emission observed within the instrument rise time(TAU<3 ps),the early picosecond dynamics are characterized by a rise in the intensity of the Raman marker bands of the THEXI-~3MLCT state,a rise time which,within experimental uncertainty,is not influenced by either partial or complete ligand deuteriation or the presence of ligands other than bpy,as in the heteroleptic complexes[Ru(bpy)2(Ll)]~+and[Ru(bpy)2(Hdcb)]~+(where H2dcb is 4,4'-dicarboxy-2,2'-bipyridine and LI is 2,-(5'-phenyl-4'-[l,2,4]triazole-3'-yl)pyridine).Overall,although the results obtained in the present study are consistent with those obtained from examination of this paradigm complex on the femtosecond timescale,regarding initial formation of the vibrationally hot ~3MLCT state by ISC from the singlet Franck-Condon state,the observation that the THEXI-~3MLCT state reaches thermal equilibration over a much longer time period than previously suggested warrants a re-examination of views concerning the rapidity with which thermal equilibration of transition metal complex excited states takes place.
机译：皮秒三（2,2'-联吡啶基）钌（II）（[Ru（bpy）3]〜（2+））及其相关配合物的皮秒时间尺度激发态动力学时间分辨共振拉曼（ps-TR3）光谱。在双色泵浦/探针条件下最低热平衡激发（THEXI）状态的特征拉曼谱带的演化表明，该状态在几百飞秒内并未完全填充之前提出的，但仅在激发后的前20 ps内。除了在仪器上升时间内观察到的发射（TAU <3 ps）外，早期皮秒动力学的特征是拉曼标记带的强度增加。 THEXI-〜3MLCT状态，一种上升时间，在实验不确定性内，不受杂配物[Ru（bpy）2（Ll）]〜中部分或完全氘代配体氘或除bpy以外配体的存在的影响+和[Ru（bpy）2（Hdcb）]〜+（其中H2dcb是4,4'-双曲线xy-2,2'-联吡啶和L1为2，-（5'-苯基-4'-[1,2,4]三唑-3'-基）吡啶）。尽管本研究获得了总体结果与在飞秒时间尺度上检查这种范式复杂性所获得的结果一致，关于ISC由单重态Franck-Condon状态最初形成的振动热〜3MLCT状态，观察到THEXI-〜3MLCT状态在一个比以前所建议的更长的时间，需要重新考虑有关过渡金属络合物激发态热平衡发生速度的观点。

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