Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses.

Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses.
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DOI:
10.1063/1.4944344
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发表时间:
2016-07
期刊:
Structural dynamics (Melville, N.Y.)
影响因子:
--
通讯作者:
Rudenko A
Rudenko A
中科院分区:
其他
文献类型:
--
作者:
Boll R;Erk B;Coffee R;Trippel S;Kierspel T;Bomme C;Bozek JD;Burkett M;Carron S;Ferguson KR;Foucar L;Küpper J;Marchenko T;Miron C;Patanen M;Osipov T;Schorb S;Simon M;Swiggers M;Techert S;Ueda K;Bostedt C;Rolles D;Rudenko A

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利用紫外泵浦、x射线探针方案,在直线相干光源自由电子激光器上研究了碘甲烷和氟甲烷解离分子中的超快电子转移。讨论了这两种分子的紫外激发性质和不同的化学性质。观察到这两种物质的分子内长距离电荷转移特征,并对其在碘甲烷中的距离依赖进行了定量分析,其电荷态高达I21+。重建的电子转移临界距离与经典的过势垒模型和早期使用近红外泵浦脉冲的实验结果一致。
Ultrafast electron transfer in dissociating iodomethane and fluoromethane molecules was studied at the Linac Coherent Light Source free-electron laser using an ultraviolet-pump, X-ray-probe scheme. The results for both molecules are discussed with respect to the nature of their UV excitation and different chemical properties. Signatures of long-distance intramolecular charge transfer are observed for both species, and a quantitative analysis of its distance dependence in iodomethane is carried out for charge states up to I21+. The reconstructed critical distances for electron transfer are in good agreement with a classical over-the-barrier model and with an earlier experiment employing a near-infrared pump pulse.