Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Guo, Liang; Wu, Meng; Cao, Ting; Monahan, Daniele M.; Lee, Yi-Hsien; Louie, Steven G.; Fleming, Graham R.

doi:10.1038/s41567-018-0362-y

Exchange-driven intravalley mixing of excitons in monolayer transition metal dichalcogenides

Journal Article · Sun Dec 09 23:00:00 EST 2018 · Nature Physics

DOI:https://doi.org/10.1038/s41567-018-0362-y· OSTI ID:1530822

Guo, Liang ^[1]; ^[2]; ^[2]; Monahan, Daniele M. ^[1]; ^[3]; ^[2]; Fleming, Graham R. ^[4]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Kavli Energy Nanoscience Inst. at Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
National Tsing Hua Univ., Hsinchu (Taiwan). Materials Sciences and Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Kavli Energy Nanoscience Inst. at Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Biophysics and Integrated Bioimaging Division

Monolayer transition metal dichalcogenides (TMDCs) are promising two-dimensional (2D) semiconductors for application in optoelectronics. Their optical properties are dominated by two series of photo-excited exciton states—A (XA) and B (XB)1,2—that are derived from direct interband transitions near the band extrema. These exciton states have large binding energies and strong optical absorption3,4,5,6, and form an ideal system to investigate many-body effects in low dimensions. Because spin–orbit coupling causes a large splitting between bands of opposite spins, XA and XB are usually treated as spin-polarized Ising excitons, each arising from interactions within a specific set of states induced by interband transitions between pairs of either spin-up or spin-down bands (TA or TB). Here, by using monolayer MoS2 as a prototypical system and solving the first-principles Bethe–Salpeter equations, we demonstrate a strong intravalley exchange interaction between TA and TB, indicating that XA and XB are mixed states instead of pure Ising excitons. Using 2D electronic spectroscopy, we observe that an optical excitation of the lower-energy TA induces a population of the higher-energy TB, manifesting the intravalley exchange interaction. This work elucidates the dynamics of exciton formation in monolayer TMDCs, and sheds light on many-body effects in 2D materials.

Research Organization:: LBNL Materials Project

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

DOE Contract Number:: AC02-05CH11231

OSTI ID:: 1530822

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 3 Vol. 15; ISSN 1745-2473

Country of Publication:: United States

Language:: English

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