Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy

Nonresonant coherent amplitude transfer in attosecond four-wave-mixing spectroscopy
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阿秒四波混频光谱中的非共振相干振幅传递

DOI:
10.1103/physreva.107.023526
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发表时间:
2023
期刊:
影响因子:
2.9
通讯作者:
Leone, Stephen R.
Leone, Stephen R.
中科院分区:
物理与天体物理2区
文献类型:
--
作者:
Gaynor, James D.;Fidler, Ashley P.;Kobayashi, Yuki;Lin, Yen-Cheng;Keenan, Clare L.;Neumark, Daniel M.;Leone, Stephen R.

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利用阿秒四波混频(FWM)光谱技术,利用一个极紫外(XUV)脉冲和两个非共线近红外(NIR)脉冲,测量了氩原子中电子被XUV激发到一系列自电离里德堡态所产生的里德堡波包动力学。从各个里德堡态发射的信号表现出振荡结构,并持续远远超过预期的发射里德堡态的寿命。这些结果反映了较长寿命的里德伯态对每个单独检测到的状态的四波混频发射信号的实质性贡献。波包分解分析表明,相干振幅转移主要发生在光激发态到非相干Rydberg态之间。实验观察再现的含时薛定谔方程模拟使用电子结构和跃迁矩计算。该理论强调了在四波混频过程中,近红外光的穿透态和暗态以非共振的方式驱动相干振幅转移到态。
Attosecond four-wave mixing (FWM) spectroscopy using an extreme ultraviolet (XUV) pulse and two noncollinear near-infrared (NIR) pulses is employed to measure Rydberg wave packet dynamics resulting from XUV excitation of aelectron in atomic argon into a series of autoionizingRydberg stateseV. The emitted signals from individual Rydberg states exhibit oscillatory structure and persist well beyond the expected lifetimes of the emitting Rydberg states. These results reflect substantial contributions of longer-lived Rydberg states to the FWM emission signals of each individually detected state. A wave packet decomposition analysis reveals that coherent amplitude transfer occurs predominantly from photoexcitedstates to the observedRydberg states. The experimental observations are reproduced by time-dependent Schrödinger equation simulations using electronic structure and transition moment calculations. The theory highlights that coherent amplitude transfer is driven nonresonantly to thestates by the NIR light throughanddark states during the FWM process.
DOI: 10.32388/pgiswd
发表时间: 2020-02
期刊: Definitions
影响因子: --
作者:
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