Photodissociation of aligned CH(3)I and C(6)H(3)F(2)I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization.

Photodissociation of aligned CH(3)I and C(6)H(3)F(2)I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization.
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对齐的CH(3)I和C(6)H(3)F(3)F(2)I分子的光解离,该分子用位点选择性的极端紫外线离子化探测了时间分辨的库仑爆炸成像。

DOI:
10.1063/1.4998648
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发表时间:
2018-01
期刊:
Structural dynamics (Melville, N.Y.)
影响因子:
--
通讯作者:
Boll R
Boll R
中科院分区:
其他
文献类型:
--
作者:
Amini K;Savelyev E;Brauße F;Berrah N;Bomme C;Brouard M;Burt M;Christensen L;Düsterer S;Erk B;Höppner H;Kierspel T;Krecinic F;Lauer A;Lee JWL;Müller M;Müller E;Mullins T;Redlin H;Schirmel N;Thøgersen J;Techert S;Toleikis S;Treusch R;Trippel S;Ulmer A;Vallance C;Wiese J;Johnsson P;Küpper J;Rudenko A;Rouzée A;Stapelfeldt H;Rolles D;Boll R

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我们研究了由自由电子激光产生的强、极紫外(XUV)飞秒脉冲引起的时间分辨库仑爆炸,作为一种成像碘甲烷和2,6-二氟碘苯两个分子的光诱导分子动力学的方法。在267 nm的激发波长下,两种分子的主要反应途径都是碳碘键断裂的中性解离。这使得研究分子环境对强飞秒XUV脉冲的吸收以及随后的库仑爆炸过程的影响成为可能。我们发现,XUV探测脉冲在解离的碘甲烷中诱导了碘原子的局域内壳层电离,而不是在二氟碘苯中诱导了所有光碎片的非选择性电离。结果揭示了电子从甲基和苯基转移到多电荷碘离子的证据。此外,还发现了苯基上超快电荷重排的迹象,这表明时间分辨库仑爆炸成像对扩展分子中电荷的局域化很敏感。
We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon–iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.
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