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arXiv 1704.06372cond-mat.mtrl-scicond-mat.mes-hall
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单层MoS2超快响应的光致带隙重整化

Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2

Eva A. A. Pogna, Margherita Marsili, Domenico De Fazio, Stefano Dal Conte, Cristian Manzoni, Davide Sangalli, Duhee Yoon, Antonio Lombardo, Andrea C. Ferrari, A… 展开作者

Eva A. A. Pogna, Margherita Marsili, Domenico De Fazio, Stefano Dal Conte, Cristian Manzoni, Davide Sangalli, Duhee Yoon, Antonio Lombardo, Andrea C. Ferrari, Andrea Marini, Giulio Cerullo, Deborah Prezzi

摘要:

过渡金属二硫属化合物(TMD)是一种新型的二维半导体材料,在光电和柔性器件中具有广阔的应用前景。然而,仍然缺乏对它们的微观物理学的微观解释-对于理解和优化设备操作至关重要。在这里,我们使用飞秒瞬态吸收光谱,泵浦脉冲可调谐性和宽带探测,监测弛豫动力学单层二硫化钼在整个可见光范围内,不同的激子跃迁的光激发。我们发现,无论激发光子的能量,瞬态吸收光谱显示的所有激子跃迁和相应的红移光诱导吸收带的同时漂白。超快光学响应的第一性原理建模表明,瞬态带隙重整化,所造成的光激发载流子的存在下,是主要负责所观察到的功能。我们的研究结果表明,即使在低激发密度制度的瞬态光学响应的TMD的多体效应的强烈影响。

英文摘要:

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2d) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics -- of pivotal importance for the understanding and optimization of device operation -- is still lacking. Here we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation photon energy, the transient absorption spectrum shows the simultaneous bleaching of all excitonic transitions and corresponding red-shifted photoinduced absorption bands. First-principle modeling of the ultrafast optical response reveals that a transient bandgap renormalization, caused by the presence of photo-excited carriers, is primarily responsible for the observed features. Our results demonstrate the strong impact of many-body effects in the transient optical response of TMDs even in the low-excitation-density regime.

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