Nonlocal dielectric function and nested dark excitons in MoS2

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Andreas Koitzsch - , Leibniz Institute for Solid State and Materials Research Dresden (First author)
  • Anna-Sophie Pawlik - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Carsten Habenicht - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Tom Klaproth - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Roman Schuster - , Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Bernd Buchner - , Chair of Experimental Solid State Physics, Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Martin Knupfer - , Leibniz Institute for Solid State and Materials Research Dresden (Last author)

Abstract

Their exceptional optical properties are a driving force for the persistent interest in atomically thin transition metal dichalcogenides such as MoS2. The optical response is dominated by excitons. Apart from the bright excitons, which directly couple to light, it has been realized that dark excitons, where photon absorption or emission is inhibited by the spin state or momentum mismatch, are decisive for many optical properties. However, in particular the momentum dependence is difficult to assess experimentally and often remains elusive or is investigated by indirect means. Here we study the momentum dependent electronic structure experimentally and theoretically. We use angle-resolved photoemission as a one-particle probe of the occupied valence band structure and electron energy loss spectroscopy as a two-particle probe of electronic transitions across the gap to benchmark a single-particle model of the dielectric function epsilon(q, omega) against momentum dependent experimental measurements. This ansatz captures key aspects of the data surprisingly well. In particular, the energy region where substantial nesting occurs, which is at the origin of the strong light-matter interaction of thin transition metal dichalcogenides and crucial for the prominent C-exciton, is described well and spans a more complex exciton landscape than previously anticipated. Its local maxima in (q not equal 0, omega) space can be considered as dark excitons and might be relevant for higher order optical processes. Our study may lead to a more complete understanding of the optical properties of atomically thin transition metal dichalcogenides.

Details

Original languageEnglish
Number of pages9
Journalnpj 2D materials and applications
Volume3
Issue number41
Publication statusPublished - 1 Nov 2019
Peer-reviewedYes

External IDs

Scopus 85074365382

Keywords

Keywords

  • Monolayer, Absorption, Thickness