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Probing the Upper Band Gap of Atomic Rhenium Disulfide Layers

Probing the Upper Band Gap of Atomic Rhenium Disulfide Layers
Dhakal, Krishna PrasadKim, HyunminLee, SeonwooKim, YoungjaeLee, JaeDongAhn, Jong-Hyun
DGIST Authors
Kim, HyunminLee, JaeDong
Issue Date
Light: Science and Applications, 7(1)
Article Type
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. © 2018, The Author(s).
Nature Publishing Group
Related Researcher
  • Author Lee, JaeDong Light and Matter Theory Laboratory
  • Research Interests Theoretical Condensed Matter Physics; Ultrafast Dynamics and Optics; Nonequilibrium Phenomena
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Companion Diagnostics and Medical Technology Research Group1. Journal Articles
Department of Emerging Materials ScienceLight and Matter Theory Laboratory1. Journal Articles

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