Ultrafast Coherent Exciton Couplings and Many-Body Interactions in Monolayer WS2,Nano Letters

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Ultrafast Coherent Exciton Couplings and Many-Body Interactions in Monolayer WS2
Nano Letters ( IF 9.1 ) Pub Date : 2024-06-20 , DOI: 10.1021/acs.nanolett.4c01991
Daniel Timmer ₁ , Moritz Gittinger ₁ , Thomas Quenzel ₁ , Alisson R Cadore ₂ , Barbara L T Rosa ₂ , Wenshan Li ₂ , Giancarlo Soavi ₂ , Daniel C Lünemann ₁ , Sven Stephan ₁ , Martin Silies ₁ , Tommy Schulz ₃ , Alexander Steinhoff ₃ , Frank Jahnke ₃ , Giulio Cerullo _{4,

5} , Andrea C Ferrari ₂ , Antonietta De Sio _{1,

6} , Christoph Lienau _{1,

6}

Affiliation

Transition metal dichalcogenides (TMDs) are quantum confined systems with interesting optoelectronic properties, governed by Coulomb interactions in the monolayer (1L) limit, where strongly bound excitons provide a sensitive probe for many-body interactions. Here, we use two-dimensional electronic spectroscopy (2DES) to investigate many-body interactions and their dynamics in 1L-WS₂ at room temperature and with sub-10 fs time resolution. Our data reveal coherent interactions between the strongly detuned A and B exciton states in 1L-WS₂. Pronounced ultrafast oscillations of the transient optical response of the B exciton are the signature of a coherent 50 meV coupling and coherent population oscillations between the two exciton states. Supported by microscopic semiconductor Bloch equation simulations, these coherent dynamics are rationalized in terms of Dexter-like interactions. Our work sheds light on the role of coherent exciton couplings and many-body interactions in the ultrafast temporal evolution of spin and valley states in TMDs.

中文翻译：

单层 WS2 中的超快相干激子耦合和多体相互作用

过渡金属二硫化物 (TMD) 是具有有趣光电特性的量子限制系统，受单层 (1L) 极限中的库仑相互作用控制，其中强束缚激子为多体相互作用提供了灵敏的探针。在这里，我们使用二维电子光谱 (2DES) 在室温下以亚 10 fs 时间分辨率研究 1L-WS ₂中的多体相互作用及其动力学。我们的数据揭示了 1L-WS ₂中强烈失谐的 A 和 B 激子态之间的相干相互作用。 B 激子瞬态光学响应的显着超快振荡是两个激子态之间相干 50 meV 耦合和相干布居振荡的特征。在微观半导体布洛赫方程模拟的支持下，这些相干动力学根据类似德克斯特的相互作用被合理化。我们的工作揭示了相干激子耦合和多体相互作用在 TMD 中自旋和谷态超快时间演化中的作用。

更新日期：2024-06-20

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