论文标题

通过几秒芯级瞬态吸收光谱法在激光加热镍中的电子热化和松弛

Electron Thermalization and Relaxation in Laser-Heated Nickel by Few-Femtosecond Core-Level Transient Absorption Spectroscopy

论文作者

Chang, Hung-Tzu, Guggenmos, Alexander, Cushing, Scott K., Cui, Yang, Din, Naseem Ud, Acharya, Shree Ram, Porter, Ilana J., Kleineberg, Ulf, Turkowski, Volodymyr, Rahman, Talat S., Neumark, Daniel M., Leone, Stephen R.

论文摘要

镍中光激发载体动力学的直接测量是使用镍M $ _ {2,3} $ edge上的几秒钟极端紫外线(XUV)瞬态吸收光谱制成的。可以观察到,可以通过高斯宽扩展($σ$)和基态吸收光谱的红位宽($σ$)和红移($ω_{s} $)来描述光激发镍的核心水平吸收线条。理论预测,实验结果验证了在初始快速载体热化后,电子温度升高($ΔT$)与高斯扩张因子$σ$线性成正比,从而提供了电子温度放松的定量实时跟踪。测量结果显示了50 nm厚的多晶镍膜的电子冷却时间为640 $ \ pm $ 80 fs。使用热热载体,光谱红移表现出与电子温度变化$ω_{s} \proptoδt^{1.5} $的变化的幂律关系。通过载流子散射的快速电子热化伴随并遵循标称的4 FS光激发脉冲,直到载体达到准热平衡为止。与<6 fs仪器响应函数纠缠在一起,从在不同泵浦的情况下获取的实验数据估计的载体热化时间范围从34 fs到13 fs,并且可以观察到,电子热化时间随着泵的增加而减小。该研究提供了一个初始示例,即用XUV光实时测量金属中的电子温度和热化,并为在具有核心水平吸收光谱的金属中进一步研究光诱导的相变和载体传输的基础。

Direct measurements of photoexcited carrier dynamics in nickel are made using few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy at the nickel M$_{2,3}$ edge. It is observed that the core-level absorption lineshape of photoexcited nickel can be described by a Gaussian broadening ($σ$) and a red shift ($ω_{s}$) of the ground state absorption spectrum. Theory predicts, and the experimental results verify that after initial rapid carrier thermalization, the electron temperature increase ($ΔT$) is linearly proportional to the Gaussian broadening factor $σ$, providing quantitative real-time tracking of the relaxation of the electron temperature. Measurements reveal an electron cooling time for 50 nm thick polycrystalline nickel films of 640$\pm$80 fs. With hot thermalized carriers, the spectral red shift exhibits a power-law relationship with the change in electron temperature of $ω_{s}\proptoΔT^{1.5}$. Rapid electron thermalization via carrier-carrier scattering accompanies and follows the nominal 4 fs photoexcitation pulse until the carriers reach a quasi-thermal equilibrium. Entwined with a <6 fs instrument response function, carrier thermalization times ranging from 34 fs to 13 fs are estimated from experimental data acquired at different pump fluences and it is observed that the electron thermalization time decreases with increasing pump fluence. The study provides an initial example of measuring electron temperature and thermalization in metals in real time with XUV light, and it lays a foundation for further investigation of photoinduced phase transitions and carrier transport in metals with core-level absorption spectroscopy.

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