Ultrafast isomerization initiated by X-ray core ionization

被引:92
|
作者
Liekhus-Schmaltz, Chelsea E. [1 ,2 ]
Tenney, Ian [1 ,2 ]
Osipov, Timur [3 ]
Sanchez-Gonzalez, Alvaro [4 ]
Berrah, Nora [3 ]
Boll, Rebecca [5 ,6 ]
Bomme, Cedric [5 ]
Bostedt, Christoph [7 ]
Bozek, John D. [7 ]
Carron, Sebastian [7 ]
Coffee, Ryan [7 ]
Devin, Julien [1 ,2 ]
Erk, Benjamin [5 ]
Ferguson, Ken R. [7 ,8 ]
Field, Robert W. [9 ]
Foucar, Lutz [10 ]
Frasinski, Leszek J. [4 ]
Glownia, James M. [7 ]
Guehr, Markus [2 ]
Kamalov, Andrei [1 ,2 ]
Krzywinski, Jacek [7 ]
Li, Heng [2 ,7 ]
Marangos, Jonathan P. [4 ]
Martinez, Todd J. [2 ,11 ]
McFarland, Brian K. [2 ]
Miyabe, Shungo [2 ,11 ]
Murphy, Brendan [3 ]
Natan, Adi [2 ]
Rolles, Daniel [5 ]
Rudenko, Artem [12 ]
Siano, Marco [4 ]
Simpson, Emma R. [4 ]
Spector, Limor [1 ,2 ]
Swiggers, Michele [7 ]
Walke, Daniel [4 ]
Wang, Song [1 ,2 ]
Weber, Thorsten [13 ]
Bucksbaum, Philip H. [1 ,2 ,8 ]
Petrovic, Vladimir S. [1 ,2 ]
机构
[1] Stanford Univ, Dept Phys, Stanford, CA 94305 USA
[2] PULSE Inst Ultrafast Energy Sci, Menlo Pk, CA 94025 USA
[3] Univ Connecticut, Dept Phys, Storrs, CT 06269 USA
[4] Univ London Imperial Coll Sci Technol & Med, Dept Phys, London SW7 2AZ, England
[5] DESY, D-22607 Hamburg, Germany
[6] Max Planck Inst Nucl Phys, D-69117 Heidelberg, Germany
[7] Linac Coherent Light Source, Menlo Pk, CA 94025 USA
[8] Stanford Univ, Dept Appl Phys, Stanford, CA 94305 USA
[9] MIT, Dept Chem, Cambridge, MA 02139 USA
[10] Max Planck Inst Med Res, D-69120 Heidelberg, Germany
[11] Stanford Univ, Dept Chem, Stanford, CA 94305 USA
[12] Kansas State Univ, Dept Phys, JR Macdonald Lab, Manhattan, KS 66506 USA
[13] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA
来源
NATURE COMMUNICATIONS | 2015年 / 6卷
基金
美国国家科学基金会; 英国工程与自然科学研究理事会;
关键词
MEMBRANE-PROTEIN STRUCTURE; ACETYLENE; DISSOCIATION; SPECTROSCOPY; VINYLIDENE; DYNAMICS; PULSES; LASERS; C2H2;
D O I
10.1038/ncomms9199
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Rapid proton migration is a key process in hydrocarbon photochemistry. Charge migration and subsequent proton motion can mitigate radiation damage when heavier atoms absorb X-rays. If rapid enough, this can improve the fidelity of diffract-before-destroy measurements of biomolecular structure at X-ray-free electron lasers. Here we study X-ray-initiated isomerization of acetylene, a model for proton dynamics in hydrocarbons. Our time-resolved measurements capture the transient motion of protons following X-ray ionization of carbon K-shell electrons. We Coulomb-explode the molecule with a second precisely delayed X-ray pulse and then record all the fragment momenta. These snapshots at different delays are combined into a 'molecular movie' of the evolving molecule, which shows substantial proton redistribution within the first 12 fs. We conclude that significant proton motion occurs on a timescale comparable to the Auger relaxation that refills the K-shell vacancy.
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页数:7
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