State-resolved attosecond reversible and irreversible dynamics in strong optical fields

被引:0
|
作者
Sabbar, Mazyar [1 ]
Timmers, Henry [1 ]
Chen, Yi-Jen [2 ,3 ]
Pymer, Allison K. [4 ]
Loh, Zhi-Heng [5 ,6 ,7 ]
Sayres, Scott G. [8 ,9 ]
Pabst, Stefan [10 ,11 ]
Santra, Robin [2 ,3 ]
Leone, Stephen R. [1 ,12 ,13 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] DESY, Ctr Free Electron Laser Sci, D-22607 Hamburg, Germany
[3] Univ Hamburg, Dept Phys, D-20355 Hamburg, Germany
[4] Eastman Chem Co, Kingsport, TN 37660 USA
[5] Nanyang Technol Univ, Div Chem & Biol Chem, Singapore 639798, Singapore
[6] Nanyang Technol Univ, Div Phys & Appl Phys, Sch Phys & Math Sci, Singapore 639798, Singapore
[7] Nanyang Technol Univ, Ctr Opt Fibre Technol, Photon Inst, Singapore 639798, Singapore
[8] Arizona State Univ, Sch Mol Sci, Tempe, AZ 85287 USA
[9] Arizona State Univ, Biodesign Ctr Appl Struct Discovery, Tempe, AZ 85287 USA
[10] Harvard Smithsonian Ctr Astrophys, ITAMP, 60 Garden St, Cambridge, MA 02138 USA
[11] Harvard Univ, Dept Phys, Cambridge, MA 02138 USA
[12] Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA
[13] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA
基金
美国国家科学基金会;
关键词
REAL-TIME OBSERVATION; TUNNEL IONIZATION; CHARGE MIGRATION; LASER; COULOMB; CYCLE; XE;
D O I
10.1038/NPHYS4027
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Strong-field ionization (SFI) is a key process for accessing real-time quantum dynamics of electrons on the attosecond timescale. The theoretical foundation of SFI was pioneered in the 1960s, and later refined by various analytical models. While asymptotic ionization rates predicted by these models have been tested to be in reasonable agreement for a wide range of laser parameters, predictions for SFI on the sub-laser-cycle timescale are either beyond the scope of the models or show strong qualitative deviations from full quantum-mechanical simulations. Here, using the unprecedented state specificity of attosecond transient absorption spectroscopy, we follow the real-time SFI process of the two valence spin-orbit states of xenon. The results reveal that the irreversible tunnelling contribution is accompanied by a reversible electronic population that exhibits an observable spin-orbit-dependent phase delay. A detailed theoretical analysis attributes this observation to transient ground-state polarization, an unexpected facet of SFI that cannot be captured by existing analytical models that focus exclusively on the production of asymptotic electron/ion yields.
引用
收藏
页码:472 / 478
页数:7
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