Channel Coupling Dynamics of Deep-Lying Orbitals in Molecular High-Harmonic Generation.
Channel Coupling Dynamics of Deep-Lying Orbitals in Molecular High-Harmonic Generation.
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DOI：
10.1103/physrevlett.128.183202
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发表时间：
2022-05
影响因子：
8.6
通讯作者：
Zheng Shu;Hongjing Liang;Yichen Wang;Shi-lin Hu;Shi Chen;Haifeng Xu;R. Ma;D. Ding;Jingjing Chen
中科院分区：
文献类型：
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作者：
Zheng Shu;Hongjing Liang;Yichen Wang;Shi-lin Hu;Shi Chen;Haifeng Xu;R. Ma;D. Ding;Jingjing Chen
对高次谐波光谱结构的研究为强激光作用下的分子结构和动力学提供了丰富的信息，在此基础上发展了分子超快动力学成像技术。结合从头计算和对CO2分子高次谐波光谱的实验测量，我们在高次谐波光谱的低能区发现了一种新的DIP结构，它被认为是深层分子轨道参与这一过程的指纹，并破译了潜在的阿秒多通道耦合动力学。我们的工作为强激光场中分子的超快动力学提供了新的线索。
Investigation on structures in the high-harmonic spectrum has provided profuse information of molecular structure and dynamics in intense laser fields, based on which techniques of molecular ultrafast dynamics imaging have been developed. Combining ab initio calculations and experimental measurements on the high-harmonic spectrum of the CO_{2} molecule, we find a novel dip structure in the low-energy region of the harmonic spectrum which is identified as fingerprints of participation of deeper-lying molecular orbitals in the process and decodes the underlying attosecond multichannel coupling dynamics. Our work sheds new light on the ultrafast dynamics of molecules in intense laser fields.