4.8 Article

Direct Determination of Band-Gap Renormalization in the Photoexcited Monolayer MoS2

Journal

PHYSICAL REVIEW LETTERS
Volume 122, Issue 24, Pages -

Publisher

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.122.246803

Keywords

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Funding

  1. National Science Foundation (NSF) [DMR-1608437]
  2. NSF [DMR-1809680]
  3. Center for Precision Assembly of Superstratic and Superatomic Solids, a Materials Science and Engineering Research Center (MRSEC) through NSF [DMR-142063]
  4. Vannevar Bush Faculty Fellowship through Office of Naval Research Research Grant [N00014-18-1-2080]
  5. Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Solar Energy Technologies Office
  6. DOE [DE-SC00014664]

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A key feature of monolayer semiconductors, such as transition-metal dichalcogenides, is the poorly screened Coulomb potential, which leads to a large exciton binding energy (E-b) and strong renormalization of the quasiparticle band gap (E-g) by carriers. The latter has been difficult to determine due to a cancellation in changes of E-b and E-g, resulting in little change in optical transition energy at different carrier densities. Here, we quantify band-gap renormalization in macroscopic single crystal MoS2 monolayers on SiO2 using time and angle-resolved photoemission spectroscopy. At an excitation density above the Mott threshold, E-g decreases by as much as 360 meV. We compare the carrier density-dependent E-g with previous theoretical calculations and show the necessity of knowing both doping and excitation densities in quantifying the band gap.

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