超快原子间能量转移中核波包干涉的观测
Observation of Nuclear-wavepacket Interference in Ultrafast Inter-atomic Energy Transfer
AI总结：
本文通过时间分辨光离子-光离子符合光谱和量子动力学模拟，在氩二聚体超快原子间能量转移中观测到核波包量子干涉，揭示了其对动能释放谱的周期性调制，为研究复杂体系中的量子干涉效应奠定基础。
摘要：
我们报告了在低于原子间库仑衰变（ICD）阈值的氩二聚体中，驱动超快激发能量转移的核波包动力学中量子干涉的实验观测。利用时间分辨光离子-光离子符合光谱和量子动力学模拟，我们揭示了初始态中核量子动力学对电子弛豫动力学的影响：一个原子上内价层3s空穴导致另一个原子上4s或4p激发的弛豫过程受到调制，从而在符合Ar+-Ar+离子对的动能释放（KER）谱上产生深度周期性调制。此外，时间分辨KER谱显示出能量转移过程中量子干涉效应的特征指纹。我们的发现为阐明更复杂体系中超快电荷和能量转移动力学中的量子干涉效应铺平了道路。
英文摘要：
We report the experimental observation of quantum interference in the nuclear wave-packet dynamics driving ultrafast excitation-energy transfer in argon dimers below the threshold of interatomic Coulombic decay (ICD). Using time-resolved photoion-photoion coincidence spectroscopy and quantum dynamics simulations, we reveal that the electronic relaxation dynamics of the inner-valence $3s$ hole on one atom leading to a $4s$ or $4p$ excitation on the other one is influenced by nuclear quantum dynamics in the initial state, giving rise to a deep, periodic modulation on the kinetic-energy-release (KER) spectra of the coincident Ar$^+$-Ar$^+$ ion pairs. Moreover, the time-resolved KER spectra show characteristic fingerprints of quantum interference effects during the energy-transfer process. Our findings pave the way to elucidating quantum-interference effects in ultrafast charge- and energy-transfer dynamics in more complex systems.
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