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  • Letter

External screening and lifetime of exciton population in single-layer ReSe2 probed by time- and angle-resolved photoemission spectroscopy

Klara Volckaert1, Byoung Ki Choi2,3, Hyuk Jin Kim2, Deepnarayan Biswas1, Denny Puntel4, Simone Peli5, Fulvio Parmigiani4,5, Federico Cilento5, Young Jun Chang2,6 et al.

Søren Ulstrup1,*

  • 1Department of Physics and Astronomy, Interdisciplinary Nanoscience Center, Aarhus University, 8000 Aarhus C, Denmark
  • 2Department of Physics, University of Seoul, Seoul 02504, Republic of Korea
  • 3Advanced Light Source, E. O. Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 4Dipartimento di Fisica, Università degli Studi di Trieste, 34127 Trieste, Italy
  • 5Elettra-Sincrotrone Trieste S.C.P.A., 34149 Basovizza, Trieste, Italy
  • 6Department of Smart Cities, University of Seoul, Seoul 02504, Republic of Korea

  • *ulstrup@phys.au.dk

Phys. Rev. Materials 7, L041001 – Published 25 April, 2023

DOI: https://doi.org/10.1103/PhysRevMaterials.7.L041001

Abstract

The semiconductor ReSe2 is characterized by a strongly anisotropic optical absorption and is therefore promising as an optically active component in two-dimensional heterostructures. However, the underlying femtosecond dynamics of photoinduced excitations in such materials has not been sufficiently explored. Here, we apply an infrared optical excitation to single-layer ReSe2 grown on a bilayer graphene substrate and monitor the temporal evolution of the excited state signal using time- and angle-resolved photoemission spectroscopy. We measure an optical gap of (1.53±0.02)eV, consistent with resonant excitation of the lowest exciton state. The exciton distribution is tunable via the linear polarization of the pump pulse and exhibits a biexponential decay with time constants given by τ1=(110±10) fs and τ2=(650±70) fs, facilitated by interlayer charge transfer to the underlying bilayer graphene and recombination via an in-gap state that is pinned at the Fermi level. By extracting the momentum-resolved exciton distribution we estimate its real-space radial extent to be greater than (17±1) Å, implying significant spatial broadening of the distribution due to screening from the bilayer graphene substrate.

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