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TMD单层中激子性质的合金工程

Alloy engineering of excitonic properties in TMD monolayers

Eirini Katsipoulaki, Adlen Smiri, Panagiotis Spiliotakis, Konstantinos Mourzidis, Danae Katrisioti, Takashi Taniguchi, Kenji Watanabe, Georgios Kopidakis, Zdenek Sofer, Gang Wang, Emmanuel Stratakis, George Kioseoglou, Iann C. Gerber, Xavier Marie, Ioannis Paradisanos

arXiv 2608.03347首次发表:更新:

AI 中文总结

该研究通过光谱学调控TMD单层MoS$_{2x}$Se$_{2(1-x)}$的激子性质,实现光学带隙、圆偏振度等的连续可调,证明合金工程是调控其激子性质的有效策略。

AI 中文摘要

我们利用光谱学研究了全成分范围的单层MoS$_{2x}$Se$_{2(1-x)}$合金,证明光学带隙可在约0.35 eV范围内连续调控,同时B-A激子分裂系统地减小,与密度泛函理论计算结果一致。变温测量显示,从富硒到富硫合金,平均声子能量逐渐增加,符合简约质量标度模型。偏振分辨光谱进一步表明,在78 K下,圆偏振度从MoSe$_2$中的近零单调增加到MoS$_2$中的约15%,观察到的偏振演化归因于合金诱导的电子结构改变,调控了亮暗激子混合及相关谷去极化。这些发现确立了合金工程是控制TMD单层激子性质的有效策略。

英文摘要

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.

Comments11 pages, 4 figures

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