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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Isolated Building Blocks of Photonic Materials: High-Resolution Excited-State Photoelectron Spectroscopy of Jet-Cooled Tetramethylethylene and 1,1'-Bicyclohexylidene
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Isolated Building Blocks of Photonic Materials: High-Resolution Excited-State Photoelectron Spectroscopy of Jet-Cooled Tetramethylethylene and 1,1'-Bicyclohexylidene

机译：孤立的光子材料构建基块：喷射冷却的四甲基亚乙基和1,1'-双环己叉基的高分辨率激发态光电子能谱

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摘要

The spectroscopy and photophysics of tetramethylethylene and 1,1'-bicyclohexylidene have been investigated using excited-state photoelectron spectroscopy in combination with multiphoton excitation. Vibronic coupling within the full manifold of the excited singlet states has been shown to play a dominant role in determining the spectroscopic properties of these compounds. Although this vibronic coupling inhibits the determination of excited state excitation energies by excitation spectroscopy, it enables at the same time their observation in the photoelectron spectra. As a result, a large number of previously unobserved Rydberg states could be located and assigned. For both molecules ionization from the Rydberg states is observed to be heavily perturbed by ionization from the underlying quasi-continuum of the (π, π~*) valence state. The photoelectron spectra of 1,1'-bicyclohexylidene reveal that the state around 55000 cm~(-1) (6.82 eV), which has previously been assigned as a second valence state, does not show the ionization pattern expected on the basis of previous suggestions made for the character of this state. On the basis of this observation, configuration mixing between the (π, π~*) valence state and the (π, 3d) Rydberg manifold is offered as a possible explanation.
机译：结合激发态光电子能谱和多光子激发，研究了四甲基乙烯和1,1'-双环己叉基的光谱和光物理性质。已证明在激发单重态的完整流形内的振动耦合在确定这些化合物的光谱性质中起主要作用。尽管这种电声耦合抑制了通过激发光谱法确定激发态激发能，但是它同时使它们能够在光电子光谱中进行观察。结果，可以找到并分配大量以前未观察到的里德堡状态。对于这两种分子，观察到来自里德堡态的电离被来自（π，π〜*）价态的下准连续体的电离严重地干扰。 1,1'-双环己叉基的光电子光谱表明，先前被指定为第二价态的55000 cm〜（-1）（6.82 eV）附近的状态未显示出基于先前的电离模式针对这种状态的性质提出了一些建议。基于此观察结果，提供了（π，π〜*）价态与（π，3d）Rydberg流形之间的构型混合作为可能的解释。

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