Anion resonances of para-benzoquinone probed by frequency-resolved photoelectron imaging.

Anion resonances of para-benzoquinone probed by frequency-resolved photoelectron imaging.
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通过频率分辨光电子成像探测对苯醌的阴离子共振。

DOI:
10.1021/jp509102p
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发表时间:
2014
期刊:
The journal of physical chemistry. A
影响因子:
--
通讯作者:
J. Verlet
J. Verlet
中科院分区:
--
文献类型:
--
作者:
C. W. West;J. Bull;Erkki Antonkov;J. Verlet

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自由电子在封闭壳中性分子上的共振附着,以及随后的电子分离和电子弛豫通道之间的相互作用,代表了整个化学和生化系统中一个基本但常见的过程。详细介绍了阴离子频率分辨光电子成像的新方法,并用于绘制气相对苯醌的分子激发态动力学,对苯醌是许多生物电子转移链中的电子接受部分。激发能、电子动能和电子弹射各向异性的三维谱显示了激发态和中间态动力学的清晰指纹。结果表明,许多激发态是强耦合的,为形成基态自由基阴离子提供了一条途径,尽管事实上电子在激发态中是正式不受束缚的。讨论了我们的方法与电子冲击附着研究的关系和主要优势,包括扩展到时间分辨动力学和更大的分子系统。
The resonant attachment of a free electron to a closed shell neutral molecule and the interplay between the following electron detachment and electronic relaxation channels represents a fundamental but common process throughout chemical and biochemical systems. The new methodology of anion frequency-resolved photoelectron imaging is detailed and used to map out molecular excited state dynamics of gas-phase para-benzoquinone, which is the electron accepting moiety in many biological electron-transfer chains. Three-dimensional spectra of excitation energy, electron kinetic energy, and electron ejection anisotropy reveal clear fingerprints of excited and intermediate state dynamics. The results show that many of the excited states are strongly coupled, providing a route to forming the ground state radical anion, despite the fact that the electron is formally unbound in the excited states. The relation of our method to electron impact attachment studies and the key advantages, including the extension to time-resolved dynamics and to larger molecular systems, are discussed.
DOI: 10.1039/c1cp22237f
发表时间: 2011-01-01
影响因子: 3.3
作者:
Horke, Daniel A.;Verlet, Jan R. R.
通讯作者: Verlet, Jan R. R.
DOI: 10.1039/c2cp43275g
发表时间: 2012-11
期刊: Physical chemistry chemical physics : PCCP
影响因子: --
作者:
A. Chatterley;D. Horke;J. Verlet
通讯作者: A. Chatterley;D. Horke;J. Verlet