Ultrafast isomerization initiated by X-ray core ionization

被引：93

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.

引用

页数：7

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