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arXiv 2103.09965cond-mat.mtrl-sci
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短飞秒极紫外瞬态吸收光谱研究WS $_{2}$中载流子和芯激子的耦合动力学

Coupled Valence Carrier and Core-Exciton Dynamics in WS$_{2}$ Probed by Few-Femtosecond Extreme Ultraviolet Transient Absorption Spectroscopy

Hung-Tzu Chang, Alexander Guggenmos, Christopher T. Chen, Juwon Oh, Romain Géneaux, Yi-De Chuang, Adam M. Schwartzberg, Shaul Aloni, Daniel M. Neumark, Stephen R. Leone

摘要:

用500-1000 nm超连续谱和宽带XUV脉冲(30-50 eV)进行的少飞秒极紫外(XUV)瞬态吸收光谱同时探测WS $_{2}$中W O $_3$边缘(37-45 eV)处的光激发载流子的动力学和W N $_{6,7}$边缘(32-37 eV)处的芯激子吸收的载流子诱导的修改。在半导体的同一XUV光谱区域中获得连续的芯到导带吸收特征和离散的芯激子跃迁提供了一种新颖的手段来研究载流子激发对芯激子动力学的影响。核心水平的瞬态吸收光谱,测量与脉冲到达第一探索核心水平和价载流子的动力学,揭示了核心激子跃迁的强烈影响的光激发载流子。从W-O $_{3}$边的芯-导带跃迁的XUV瞬态吸收谱中提取了$1.2\pm0.3$ ps的空穴-声子弛豫时间和$3.1\pm0.4$ ps的载流子复合时间.在W N $_{6,7}$边缘的瞬态吸收信号的全球拟合产量$\sim 10$ fs相干寿命的核心激子状态,并揭示了光激发载流子,改变电子屏蔽和带填充,是占主导地位的贡献者的核心激子的光谱修改和直接场诱导的变化发挥次要作用。这项工作提供了第一次看光激发载流子的核心激子状态的调制和推进我们的理解,在金属二硫属化物的载流子动力学。

英文摘要:

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

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