Attosecond Time-Domain Measurement of Core-Level-Exciton Decay in Magnesium Oxide

被引:59
作者
Geneaux, Romain [1 ]
Kaplan, Christopher J. [1 ]
Yue, Lun [2 ]
Ross, Andrew D. [1 ]
Baekhoj, Jens E. [2 ]
Kraus, Peter M. [1 ]
Chang, Hung-Tzu [1 ]
Guggenmos, Alexander [1 ]
Huang, Mi-Ying [1 ]
Zurch, Michael [1 ]
Schafer, Kenneth J. [2 ]
Neumark, Daniel M. [1 ,3 ]
Gaarde, Mette B. [2 ]
Leone, Stephen R. [1 ,3 ,4 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Louisiana State Univ, Dept Phys & Astron, Baton Rouge, LA 70803 USA
[3] Lawrence Berkeley Natl Lab, Chem Sci Div, Berkeley, CA 94720 USA
[4] Univ Calif Berkeley, Dept Phys, Berkeley, CA 94720 USA
关键词
X-RAY-EMISSION; VIBRATIONAL STRUCTURE; PHONON RELAXATION; LINE-SHAPES; PHOTOEMISSION; DYNAMICS; SPECTRA; STATES; MGO;
D O I
10.1103/PhysRevLett.124.207401
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
Excitation of ionic solids with extreme ultraviolet pulses creates localized core-level excitons, which in some cases couple strongly to the lattice. Here, core-level-exciton states of magnesium oxide are studied in the time domain at the Mg L-2,L-3 edge with attosecond transient reflectivity spectroscopy. Attosecond pulses trigger the excitation of these short-lived quasiparticles, whose decay is perturbed by time-delayed near-infrared pulses. Combined with a few-state theoretical model, this reveals that the infrared pulse shifts the energy of bright (dipole-allowed) core-level-exciton states as well as induces features arising from dark core-level excitons. We report coherence lifetimes for the two lowest core-level excitons of 2.3 +/- 0.2 and 1.6 +/- 0.5 fs and show that these are primarily a consequence of strong exciton-phonon coupling, disclosing the drastic influence of structural effects in this ultrafast relaxation process.
引用
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页数:6
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