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中国物理学会期刊

太赫兹光谱揭示拓扑半金属Co2MnAl薄膜中光载流子驱动的正负光电导转换

The conversion of positive-negative photoconductivity driven by photoexcited carriers in topological semimetal Co2MnAl thin films revealed with Terahertz Spectroscopy

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  • 本研究采用光泵浦-太赫兹探测光谱技术,对比研究了拓扑半金属 Co2MnAl与传统Fe薄膜的超快太赫兹光电导特性,观测到Co2MnAl薄膜中光载流子驱动的正负光电导转换现象。利用磁场调制分离信号,结合Tinkham模型定量分析光电导动力学,发现Fe薄膜仅表现电子散射主导的负光电导,弛豫过程不受泵浦能量密度影响。Co2MnAl薄膜因自旋分辨的金属/半导体复合能带结构,初始正光电导源于少数自旋半导体通道光生载流子增加,后续快速转为负光电导则由动态极化子形成导致载流子迁移率降低引起,其光电导峰值受泵浦能量密度调控。本研究阐明了Co2MnAl薄膜超快光电特性及正负光电导转换的物理机制,实现了对其不同自旋电子动力学行为的光谱学区分,为优化钴基哈斯勒合金太赫兹辐射性能、研发新型超快自旋电子器件提供了核心实验与物理依据。

    In this study, we employ the time-resolved optical pump-terahertz probe (OPTP) spectroscopy based on a femtosecond laser system with a central wavelength of 800 nm, pulse duration of 120 fs, and repetition rate of 1 kHz to systematically explore the ultrafast terahertz photoconductive characteristics and terahertz emission properties of topological ferromagnetic Heusler semimetal Co2MnAl thin films, with conventional ferromagnetic Fe thin films as a reference sample. By introducing magnetic field modulation to fully separate terahertz emission signals from pump-induced transmission signals, and quantitatively analyzing the transient photoconductivity dynamics using the Tinkham thin-film approximation model, we directly observe a distinct photoexcited carrier-driven positive-negative photoconductivity conversion behavior in Co2MnAl thin films under femtosecond laser excitation. In sharp comparison, Fe thin films only display negative photoconductivity governed by electron-electron scattering, and its relaxation processes show negligible dependence on pump laser fluence. Originating from the characteristic spin-resolved metallic/semiconducting dual band structure in Co2MnAl, the initial positive photoconductivity within sub-picoseconds is ascribed to the increased population of photogenerated carriers in the minority-spin semiconducting channel, whereas the subsequent ultrafast switching to negative photoconductivity arises from the formation of dynamic polarons that drastically suppress carrier mobility. Furthermore, the photoconductivity peak magnitude of Co2MnAl can be flexibly modulated by varying pump fluence. The peak-to-peak amplitudes of terahertz emission from both Co2MnAl and Fe thin films exhibit a linear increase with increasing pump fluence, indicating a similar optical excitation mechanism dominated by magnetic dipole and anomalous Hall effects. This work not only clarifies the intrinsic ultrafast photophysical mechanisms and spin-dependent carrier dynamics in Co2MnAl thin films, but also realizes the spectroscopic discrimination of majority-spin and minority-spin carrier behaviors, which provides critical experimental evidence and physical insights for optimizing the terahertz radiation performance of cobalt-based Heusler alloys and designing high-performance ultrafast spintronic and terahertz optoelectronic devices.

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