Unravelling the electronic structure and dynamics of an isolated molecular rotary motor in the gas-phase.
Unravelling the electronic structure and dynamics of an isolated molecular rotary motor in the gas-phase.
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DOI：
10.1039/c7sc01997a
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发表时间：
2017-09-01
期刊：
影响因子：
8.4
通讯作者：
Fielding HH
中科院分区：
文献类型：
--
作者：
Beekmeyer R;Parkes MA;Ridgwell L;Riley JW;Chen J;Feringa BL;Kerridge A;Fielding HH
利用负离子光电子能谱和量子化学计算方法研究了气相中单向分子旋转马达负离子的电子结构和动力学。光驱动的分子马达是一类重要的化合物，它是由手性拥挤烯烃衍生而来的，其中连续的光化学和热重排导致分子的一部分相对于另一部分单向旋转。在这里，我们采用阴离子光电子能谱探测的电子结构和动力学的单向分子旋转电机阴离子在气相和量子化学计算，以指导我们的结果的解释。我们发现，光激发后的第一个电子激发态，分子绕其轴旋转，一些人口仍然在激发势能面和一些人口进行内部转换回到电子基态。这些观察结果与溶液中旋转分子马达的时间分辨测量中观察到的结果相似。这项工作证明了阴离子光电子能谱在研究气相分子马达的电子结构和动力学方面的潜力，为理论提供了重要的基准，并提高了我们对光激活分子旋转马达的基本理解，这可用于通知新的光激活纳米级器件的设计。
Anion photoelectron spectroscopy and quantum chemistry calculations are employed to probe the electronic structure and dynamics of a unidirectional molecular rotary motor anion in the gas-phase. Light-driven molecular motors derived from chiral overcrowded alkenes are an important class of compounds in which sequential photochemical and thermal rearrangements result in unidirectional rotation of one part of the molecule with respect to another. Here, we employ anion photoelectron spectroscopy to probe the electronic structure and dynamics of a unidirectional molecular rotary motor anion in the gas-phase and quantum chemistry calculations to guide the interpretation of our results. We find that following photoexcitation of the first electronically excited state, the molecule rotates around its axle and some population remains on the excited potential energy surface and some population undergoes internal conversion back to the electronic ground state. These observations are similar to those observed in time-resolved measurements of rotary molecular motors in solution. This work demonstrates the potential of anion photoelectron spectroscopy for studying the electronic structure and dynamics of molecular motors in the gas-phase, provides important benchmarks for theory and improves our fundamental understanding of light-activated molecular rotary motors, which can be used to inform the design of new photoactivated nanoscale devices.
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影响因子：
8.4
作者：
Bochenkova AV;Mooney CRS;Parkes MA;Woodhouse JL;Zhang L;Lewin R;Ward JM;Hailes HC;Andersen LH;Fielding HH
通讯作者：
Fielding HH
影响因子：
4.4
作者：
BECKE, AD
通讯作者：
BECKE, AD
影响因子：
2.9
作者：
Amirjalayer, Saeed;Cnossen, Arjen;Browne, Wesley R.;Feringa, Ben L.;Buma, Wybren J.;Woutersen, Sander
通讯作者：
Woutersen, Sander
影响因子：
3.3
作者：
Karlström, G;Lindh, R;Seijo, L
通讯作者：
Seijo, L
影响因子：
5.5
作者：
Kazaryan, Andranik;Lan, Zhenggang;Filatov, Michael
通讯作者：
Filatov, Michael