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陶建飞, 金鑫, 吴可非, 刘小井
cstr: 32037.14.aps.74.20250999

Revisiting near-threshold photoelectron interference in argon with a non-adiabatic semiclassical model

TAO Jianfei, JIN Xin, WU Kefei, LIU Xiaojing
cstr: 32037.14.aps.74.20250999
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  • 结合实验与理论研究, 探索了在多光子区域($ \gamma \gt 1 $)短脉冲激光作用下氩原子的光电离过程. 通过建立包含隧穿出口处电子初始纵向动量的半经典模型, 模拟了光电子动量分布. 该方法基于费曼路径积分理论框架, 为每条电子轨迹赋予动力学相位, 从而实现了对量子干涉效应的研究. 模拟结果与含时薛定谔方程(TDSE)数值解高度符合, 同时发现, 初始纵向动量的引入对于精确重现电离阈值附近观测到的光电子谱干涉结构至关重要, 并揭示出离子实极化对低能谱影响甚微. 本文的研究结果强调了超短脉冲光电离中非绝热势垒下动力学的重要性, 并提供了基于量子轨道的清晰物理图像.
    Purpose: The interaction of intense, ultrashort laser pulses with atoms gives rise to rich non-perturbative phenomena, which are encoded within the final-state photoelectron momentum distribution (PMD). A particularly enigmatic feature often observed in the multiphoton ionization regime (Keldysh parameter $ \gamma \gtrsim 1 $), is a complex, fan-like interference pattern in the near-threshold, low-energy region of the PMD. The physical origin of this structure has been a subject of extensive debate, with proposed mechanisms ranging from multipath interference in the Coulomb field to complex sub-barrier dynamics. This work aims to provide a physical explanation for this phenomenon. We hypothesize and demonstrate that this fan-like structure is not only the consequence of Coulomb focusing, but also a direct and sensitive signature of non-adiabatic dynamics occurring as an electron tunnels through the laser-dressed atomic potential barrier. Our goal is to clearly separate the key physical ingredients responsible for shaping this quantum interference. Methodology: To achieve this, we employ a synergistic three-pronged approach that combines experiment, exact numerical simulation, and a sophisticated theoretical model.1. Experiment: We perform velocity-map imaging measurements on argon atoms ionized by a 798-nm 35-fs laser pulse at a peak intensity of $ 6.3 \times 10^{13} $ W/cm2, and the experimental results clearly show the low-energy fan-like interference pattern.2. Quantum Benchmark: We solve the time-dependent Schrödinger equation (TDSE) within the single-active-electron (SAE) approximation by using a well-established model potential for argon, which accurately reproduces its ionization potential and ground-state properties. After performing a focal-volume average to simulate experimental conditions, the TDSE results show excellent qualitative agreement with the measurements, establishing the TDSE as a reliable quantum benchmark for our investigation.3. Semiclassical Model (CTMC-p): The core of our analysis relies on a custom-developed semiclassical trajectory model based on the Feynman path-integral formulation. In this framework, ionization process is divided into two steps: (i) an electron tunnels through the potential barrier at an initial time $ t_0 $ and position $ {\boldsymbol{r}}_0 $, and (ii) it propagates classically in the combined laser and ionic fields according to Newton’s equations. Crucially, each trajectory is endowed with a quantum phase accumulated along its path, $ \varPhi_k $, allowing for the coherent summation of all trajectories ending with the same final momentum, $ M_j = \displaystyle\sum\nolimits_k {\mathrm{e}}^{{\mathrm{i}}\varPhi_k} $. Our model combines two critical physical effects beyond standard treatments:Non-Adiabatic Tunneling: We introduce a non-zero initial longitudinal momentum, $ v_{0 //} =-A(t_0)\times $$ \left(\sqrt{1+\gamma_{\text{eff}}^2}-1\right) $, acquired by the electron at the tunnel exit. This term accounts for the non-instantaneous nature of the tunneling process, a key non-adiabatic effect.Core Polarization: We include an induced dipole potential, $ U_{\text{ID}} = -\alpha^{\mathrm{I}} {\boldsymbol{E}}(t) \cdot {\boldsymbol{r}}/r^3 $, to model the dynamic polarization of the Ar+ ionic core, a multi-electron effect.By selectively including or excluding these effects, we can clearly isolate their respective contributions to the final PMD. Results: Our central finding is that the non-adiabatic initial longitudinal momentum is the decisive factor for correctly describing the near-threshold interference. The benchmark TDSE calculation for a single intensity of $ 5 \times 10^{13} $ W/cm2 ($ \gamma \approx 1.6 $) reveals a distinct 6-lobe interference pattern. A traditional semiclassical simulation based on the quasi-static tunneling approximation (i.e., setting $ v_{0//} = 0 $) qualitatively fails, predicting an incorrect 8-lobe structure. However, upon including the non-zero initial longitudinal momentum ($ v_{0//} \neq 0 $), our non-adiabatic semiclassical model quantitatively reproduces the correct 6-lobe structure, showing that it is in excellent agreement with the TDSE benchmark.To understand the underlying physics, we perform a quantum-orbit decomposition. This analysis reveals that the overall fan-like structure arises from the interference of multiple trajectory types, including “direct” (Category Ⅰ), “forward-scattered” (Category Ⅱ, and “glory-scattered” (Category Ⅲ) orbits. Although the entire structure arises from the collective interference of these paths, we pinpoint the origin of the lobe-count correction. The initial longitudinal momentum contributes a phase term, $ \Delta\varPhi_{\text{initial}} \approx -{\boldsymbol{v}}_{0//} \cdot {\boldsymbol{r}}_0 $, to the total accumulated action. We find that the relative phase between the “direct” and “glory” trajectories is exquisitely sensitive to this term due to their vastly different paths and birth conditions. It is this specific and dramatic change in the Ⅰ-Ⅲ interference channel that ultimately corrects the topology of the entire pattern, reducing the lobe count from 8 to 6. In contrast, other interference pairs, such as the holographic pair Ⅱ-Ⅲ, are largely robust against this effect as their nearly identical birth conditions cause the initial phase term to cancel out in their relative phase. In parallel, our simulations show that the ionic core polarization has a negligible effect on this low-energy structure, but is essential for accurately describing higher-energy rescattering features by smoothing unphysical caustics caused by a pure Coulomb potential. Conclusion: We demonstrate clearly that the near-threshold fan-like interference pattern in the multiphoton regime is a direct manifestation of non-adiabatic dynamics during tunneling, specifically the acquisition of a longitudinal momentum component by the electron during its finite-time passage under the potential barrier. Our findings not only provide a clear, intuitive, and orbit-based physical picture for this complex quantum phenomenon but also highlight the predictive power of semiclassical methods when crucial non-adiabatic effects are properly incorporated. This understanding lays a foundation for future investigations, including the extension of this model to more complex molecular systems and its application in retrieving attosecond electron dynamics from holographic interference patterns.
      通信作者: 刘小井, liuxj@shanghaitech.edu.cn
    • 基金项目: 国家自然科学基金(批准号: 11574020)、上海市202科技创新行动计划国际科技合作项目(批准号: 22560780300)和上海科技大学“双一流”建设基金资助的课题.
      Corresponding author: LIU Xiaojing, liuxj@shanghaitech.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11574020), the STCSM Fund of Shanghai, China (Grant No. 22560780300), and the Double First-Class Initiative Fund of ShanghaiTech University, China.
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出版历程
  • 收稿日期:  2025-07-25
  • 修回日期:  2025-08-21
  • 上网日期:  2025-09-05
  • 刊出日期:  2025-11-05

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