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中国物理学会期刊

阿秒瞬态吸收光谱: 揭示电子动力学的超快光学探针

CSTR: 32037.14.aps.74.20250546

Attosecond transient absorption spectroscopy: an ultrafast optical probe for revealing electron dynamics

CSTR: 32037.14.aps.74.20250546
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  • 阿秒瞬态吸收光谱是一种全光学泵浦-探测光谱技术. 该技术利用阿秒脉冲(极紫外至软X射线区间)激发或探测应用体系, 实时追踪电子跃迁、量子态演化及能量传递等过程, 为揭示电子和核相关超快动力学机制提供了前沿研究手段. 其核心优势在于: 1)同时具备超快时间(亚飞秒级)和精细光谱(meV级)分辨能力; 2)宽谱阿秒脉冲同时激发多个量子态, 实现多能级并行探测; 3)内壳层-价态跃迁的元素与位点特异性, 使其能够解析电荷转移、自旋态变化及局域结构演化. 目前, 阿秒瞬态吸收光谱已在原子分子物理、电子相干动力学及强场物理等研究领域取得重要突破. 本文系统地阐述了阿秒瞬态吸收光谱的技术原理, 重点分析其在气相和凝聚相体系的应用进展, 展望其在超快物理化学和量子材料等领域的应用前景. 同时, 针对阿秒激光发展趋势和探测技术特点, 探讨了阿秒瞬态吸收光谱技术未来发展方向.

     

    Attosecond transient absorption spectroscopy (ATAS) is an all-optical pump-probe technique that employs attosecond pulses (from the extreme ultraviolet to soft X-ray) to excite or probe a system, enabling real-time tracking of electronic transitions, quantum state evolution, and energy transfer processes. This approach possesses some key advantages: 1) ultrafast temporal resolution (sub-femtosecond) combined with high spectral resolution (millielectronvolt level); 2) broadband excitation of multiple quantum states, allowing simultaneous detection of multiple energy levels; and 3) element- and site-specific insights provided by the measurements of inner-shell to valence transition reveal charge transfer dynamics, spin state changes, and local structural evolution. To date, significant breakthroughs have been achieved in atomic/molecular physics, electronic coherent dynamics, and strong-field physics by using ATAS. This paper systematically reviews the technical principles and theoretical models related to ATAS by using medium intensity near-infrared pulses, analyzes the recent progress of the applications in gas-phase systems and condensed-phase systems, and explores their future prospects in ultrafast physical chemistry and quantum materials. In gas-phase environments, the ATAS has demonstrated significant capabilities in probing energy level shifts and population transfers in atomic systems, as well as capturing nonadiabatic dynamics and charge migration in diatomic and polyatomic molecules. While in condensed-phase systems, this technique has been effectively used to study the ultrafast dynamics of carriers in semiconductors and to examine the interaction dynamics of localized electrons in insulators and transition metals. Given the rapid evolution of attosecond laser technologies and the unique advantages of the ATAS detection method, this paper also outlines potential future directions. These prospects are expected to further expand the frontiers of ultrafast spectroscopy and drive advancements in a range of disciplines in basic research and technological applications.

     

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