Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

被引:71
作者
Ferre, A. [1 ]
Boguslavskiy, A. E. [2 ,3 ]
Dagan, M. [4 ]
Blanchet, V. [1 ]
Bruner, B. D. [4 ]
Burgy, F. [1 ]
Camper, A. [5 ]
Descamps, D. [1 ]
Fabre, B. [1 ]
Fedorov, N. [1 ]
Gaudin, J. [1 ]
Geoffroy, G. [1 ]
Mikosch, J. [2 ,6 ]
Patchkovskii, S. [2 ,6 ]
Petit, S. [1 ]
Ruchon, T. [5 ]
Soifer, H. [4 ]
Staedter, D. [7 ]
Wilkinson, I.
Stolow, A. [2 ,3 ,8 ]
Dudovich, N. [4 ]
Mairesse, Y. [1 ]
机构
[1] Univ Bordeaux, CNRS, CEA, CELIA,UMR5107, F-33405 Talence, France
[2] Natl Res Council Canada, Ottawa, ON K1A 0R6, Canada
[3] Univ Ottawa, Dept Phys, Ottawa, ON K1N 6N5, Canada
[4] Weizmann Inst Sci, Dept Phys Complex Syst, IL-76100 Rehovot, Israel
[5] CEA Saclay, CEA, IRAMIS, Interact & Dynam Lab LIDyL, F-91191 Gif Sur Yvette, France
[6] Max Born Inst, D-12489 Berlin, Germany
[7] Univ Toulouse, CNRS, LCAR IRSAMC, F-31062 Toulouse, France
[8] Univ Ottawa, Dept Chem, Ottawa, ON K1N 6N5, Canada
基金
加拿大自然科学与工程研究理事会; 欧洲研究理事会;
关键词
FIELD; IONIZATION; PHOTOELECTRON; SPECTROSCOPY; REFLECTION; ATOMS; ION;
D O I
10.1038/ncomms6952
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
High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20-26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.
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收藏
页数:10
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