Probing the upper band gap of atomic rhenium disulfide layers

Krishna P. Dhakal, Hyunmin Kim, Seonwoo Lee, Youngjae Kim, Jae Dong Lee, Jong Hyun Ahn

Research output: Contribution to journalArticlepeer-review

20 Citations (Scopus)


Here, we investigate the ultrafast carrier dynamics and electronic states of exfoliated ReS2 films using time-resolved second harmonic generation (TSHG) microscopy and density functional theory (DFT) calculations. The second harmonic generation (SHG) of layers with various thicknesses is probed using a 1.19-eV beam. Up to ~13 nm, a gradual increment is observed, followed by a decrease caused by bulk interferometric light absorption. The addition of a pump pulse tuned to the exciton band gap (1.57 eV) creates a decay-to-rise TSHG profile as a function of the probe delay. The power and thickness dependencies indicate that the electron–hole recombination is mediated by defects and surfaces. The two photon absorptions of 2.38 eV in the excited state that are induced by pumping from 1.57 to 1.72 eV are restricted because these transitions highly correlate with the forbidden d–d intrasubshell orbital transitions. However, the combined usage of a frequency-doubled pump (2.38 eV) with wavelength-variant SHG probes (2.60–2.82 eV) allows us to vividly monitor the variations in TSHG profiles from decay-to-rise to rise-to-decay, which imply the existence of an additional electron absorption state (s-orbital) at an approximate distance of 5.05 eV from the highest occupied molecular orbital states. This observation was critically examined by considering the allowance of each electronic transition and a small upper band gap (~0.5 eV) using modified DFT calculations.

Original languageEnglish
Article number98
JournalLight: Science and Applications
Issue number1
Publication statusPublished - 2018 Dec 1

Bibliographical note

Publisher Copyright:
© 2018, The Author(s).

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Atomic and Molecular Physics, and Optics


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