Valley-dependent exciton fine structure and Autler–Townes doublets from Berry phases in monolayer MoSe2

Yong, Chaw-Keong; Utama, M. Iqbal Bakti; Ong, Chin Shen; Cao, Ting; Regan, Emma C.; Horng, Jason; Shen, Yuxia; Cai, Hui; Watanabe, Kenji; Taniguchi, Takashi; Tongay, Sefaattin; Deng, Hui; Zettl, Alex; Louie, Steven G.; Wang, Feng

doi:10.1038/s41563-019-0447-8

Title: Valley-dependent exciton fine structure and Autler–Townes doublets from Berry phases in monolayer MoSe₂

Journal Article · Mon Aug 05 00:00:00 EDT 2019 · Nature Materials

DOI:https://doi.org/10.1038/s41563-019-0447-8· OSTI ID:1605255

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^[2]; Regan, Emma C. ^[2]; Horng, Jason ^[3]; Shen, Yuxia ^[4]; Cai, Hui ^[5];

^[6]; Taniguchi, Takashi ^[6]; Tongay, Sefaattin ^[4];

^[3];

^[7];

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Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Arizona State Univ., Tempe, AZ (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
National Inst. for Materials Science, Tsukuba (Japan)
Univ. of California, Berkeley, CA (United States). Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The Berry phase of Bloch states can have profound effects on electron dynamics and lead to novel transport phenomena, such as the anomalous Hall effect and the valley Hall effect. Recently, it was predicted that the Berry phase effect can also modify the exciton states in transition metal dichalcogenide monolayers, and lift the energy degeneracy of exciton states with opposite angular momentum through an effective valley-orbital coupling. Here, we report the observation and control of the Berry phase-induced splitting of the 2p exciton states in monolayer molybdenum diselenide (MoSe₂) using the intraexciton optical Stark spectroscopy. We observe the time-reversal-symmetric analogue of the orbital Zeeman effect resulting from the valley-dependent Berry phase, which leads to energy difference of +14 (-14) meV between the 2p+ and 2p- exciton states in the K (K') valley, consistent with the ordering from our ab initio GW-Bethe–Salpeter equation results. In addition, we show that the light–matter coupling between intraexciton states is remarkably strong, leading to a prominent valley-dependent Autler–Townes doublet under resonant driving. Finally, our study opens up pathways to coherently manipulate the quantum states and excitonic excitation with infrared radiation in two-dimensional semiconductors.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOD; National Science Foundation (NSF); US Army Research Office (ARO)

Grant/Contract Number:: AC02-05CH11231; ACI-1548562

OSTI ID:: 1605255

Journal Information:: Nature Materials, Vol. 18, Issue 10; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 28 works

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Cited By (2)

Resonant optical Stark effect in monolayer WS2 Cunningham, Paul D.; Hanbicki, Aubrey T.; Reinecke, Thomas L. Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-13501-x	journal	December 2019
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Title: Valley-dependent exciton fine structure and Autler–Townes doublets from Berry phases in monolayer MoSe2

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