Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

被引:44
作者
Brasse, Felix [1 ]
Goldsztejn, Gildas [1 ]
Amini, Kasra [2 ]
Boll, Rebecca [3 ]
Bari, Sadia [3 ]
Bomme, Cedric [3 ]
Brouard, Mark [2 ]
Burt, Michael [2 ]
de Miranda, Barbara Cunha [4 ]
Duesterer, Stefan [3 ]
Erk, Benjamin [3 ]
Geleoc, Marie [5 ]
Geneaux, Romain [5 ]
Gentleman, Alexander S. [6 ]
Guillemin, Renaud [4 ]
Ismail, Iyas [4 ]
Johnsson, Per [7 ]
Journel, Loic [4 ]
Kierspel, Thomas [8 ,9 ]
Kockert, Hansjochen [2 ]
Kuepper, Jochen [8 ,9 ,10 ]
Lablanquie, Pascal [4 ]
Lahl, Jan [7 ]
Lee, Jason W. L. [6 ]
Mackenzie, Stuart R. [6 ]
Maclot, Sylvain [7 ]
Manschwetus, Bastian [3 ]
Mereshchenko, Andrey S. [11 ]
Mullins, Terence [8 ]
Olshin, Pavel K. [11 ]
Palaudoux, Jerome [4 ]
Patchkovskii, Serguei [1 ]
Penent, Francis [4 ,12 ]
Piancastelli, Maria Novella [4 ,12 ]
Rompotis, Dimitrios [3 ]
Ruchon, Thierry [5 ]
Rudenko, Artem [13 ]
Savelyev, Evgeny [3 ]
Schirmel, Nora [3 ]
Techert, Simone [3 ,14 ,15 ]
Travnikova, Oksana [4 ]
Trippel, Sebastian [8 ,9 ]
Underwood, Jonathan G. [16 ]
Vallance, Claire [2 ]
Wiese, Joss [8 ]
Simon, Marc [4 ]
Holland, David M. P. [17 ]
Marchenko, Tatiana [4 ]
Rouzee, Arnaud [1 ]
Rolles, Daniel [13 ]
机构
[1] Max Born Inst Nichtlineare Opt & Kurzzeitspektros, D-12489 Berlin, Germany
[2] Univ Oxford, Dept Chem, Chem Res Lab, Oxford OX1 3TA, England
[3] DESY, D-22607 Hamburg, Germany
[4] Sorbonne Univ, CNRS, LCPMR, F-75005 Paris, France
[5] Univ Paris Saclay, CEA Saclay, CNRS, LIDYL,CEA, F-91191 Gif Sur Yvette, France
[6] Univ Oxford, Dept Chem, Phys & Theoret Chem Lab, Oxford OX1 3QZ, England
[7] Lund Univ, Dept Phys, S-22100 Lund, Sweden
[8] DESY, Ctr Free Electron Laser Sci CFEL, D-22607 Hamburg, Germany
[9] Univ Hamburg, Ctr Ultrafast Imaging, D-22761 Hamburg, Germany
[10] Univ Hamburg, Dept Phys, D-22761 Hamburg, Germany
[11] St Petersburg State Univ, 7-9 Univ Skaya Nab, St Petersburg 199034, Russia
[12] Uppsala Univ, Dept Phys & Astron, POB 516, Uppsala, Sweden
[13] Kansas State Univ, Dept Phys, JR Macdonald Lab, Cardwell Hall, Manhattan, KS 66506 USA
[14] Max Planck Inst Biophys Chem, D-33077 Gottingen, Germany
[15] Gottingen Univ, Inst Xray Phys, D-33077 Gottingen, Germany
[16] UCL, Dept Phys & Astron, London WC1E 6BT, England
[17] Daresbury Lab, Warrington WA4 4AD, Cheshire, England
基金
英国工程与自然科学研究理事会; 瑞典研究理事会;
关键词
METHYL-IODIDE; DYNAMICS; PHOTOIONIZATION; ENERGY; FIELD; PHOTODISSOCIATION; PHOTOABSORPTION; SPECTRA;
D O I
10.1103/PhysRevA.97.043429
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I) is investigated by ionization above the iodine 4d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.
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页数:10
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