Probing the upper band gap of atomic rhenium disulfide layers

Krishna P. Dhakal; Hyunmin Kim; Seonwoo Lee; Youngjae Kim; JaeDong Lee; Jong-Hyun Ahn

doi:10.1038/s41377-018-0100-3

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Probing the upper band gap of atomic rhenium disulfide layers

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- Probing the upper band gap of atomic rhenium disulfide layers
- Probing the upper band gap of atomic rhenium disulfide layers
- 光：科学与应用 2018年7卷第6期页码：945-955
- Affiliations：
  
  1.School of Electrical and Electronic Engineering, Yonsei University, Seoul, 03722, Republic of Korea
  2.Companion Diagnostics & Medical Technology Research Group, DGIST, Daegu, 42988, Republic of Korea
  3.Department of Emerging Materials Science, DGIST, Daegu, 42988, Republic of Korea
- Author bio：
  
  Hyunmin Kim (hyunmin.kim@dgist.ac.kr)
  JaeDong Lee (jdlee@dgist.ac.kr)
  J-H. Ahn (ahnj@yonsei.ac.kr)
- Funds：
- DOI：10.1038/s41377-018-0100-3
  中图分类号：
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Krishna P. Dhakal, Hyunmin Kim, Seonwoo Lee, 等. Probing the upper band gap of atomic rhenium disulfide layers[J]. 光：科学与应用, 2018,7(6):945-955.

Dhakal, K. P. et al. Probing the upper band gap of atomic rhenium disulfide layers. Light: Science & Applications, 7, 945-955 (2018).
Krishna P. Dhakal, Hyunmin Kim, Seonwoo Lee, 等. Probing the upper band gap of atomic rhenium disulfide layers[J]. 光：科学与应用, 2018,7(6):945-955. DOI： 10.1038/s41377-018-0100-3.

Dhakal, K. P. et al. Probing the upper band gap of atomic rhenium disulfide layers. Light: Science & Applications, 7, 945-955 (2018). DOI： 10.1038/s41377-018-0100-3.

摘要

Abstract

Here, we investigate the ultrafast carrier dynamics and electronic states of exfoliated ReS,2, 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.

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references

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