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Probing the upper band gap of atomic rhenium disulphide layers

Title	Probing the upper band gap of atomic rhenium disulphide layers
Authors	Krishna P. Dhakal, Hyunmin Kim, Seonwoo Lee, Youngjae Kim, JaeDong Lee, Jong-Hyun Ahn
Magazine	Light, Science & Applications
Date	11/28/2018
DOI	10.1038/s41377-018-0100-3
Introduction	This study focuses on 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. We observed the second harmonic generation (SHG) of various thicknesses using a 1.19-eV beam. An increment was noted up to approximately 13 nm, followed by a reduction due to bulk interferometric light absorption. A pump pulse adjusted to the exciton band gap (1.57 eV) resulted in a decay-to-rise TSHG profile based on the probe delay. The electron–hole recombination is influenced by defects and surfaces, with two photon absorptions of 2.38 eV in the excited state being restricted due to the correlation with forbidden d–d intrasubshell orbital transitions. Using a frequency-doubled pump (2.38 eV) alongside wavelength-variant SHG probes (2.60–2.82 eV), we detected variations in TSHG profiles from decay-to-rise to rise-to-decay, suggesting an additional electron absorption state (s-orbital) approximately 5.05 eV from the highest occupied molecular orbital states. This finding was critically evaluated considering the electronic transitions and a small upper band gap (~0.5 eV) using modified DFT calculations.
Quote	Krishna P. Dhakal, Hyunmin Kim and Seonwoo Lee et al. Probing the upper band gap of atomic rhenium disulphide layers. 2018. DOI: 10.1038/s41377-018-0100-3
Materials	Chemical Compounds

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