Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopies

Yadong Wang*, Fadil Iyikanat, Habib Rostami, Xueyin Bai, Xuerong Hu, Susobhan Das, Yunyun Dai, Luojun Du, Yi Zhang, Shisheng Li, Harri Lipsanen, F. Javier García de Abajo, Zhipei Sun

*Corresponding author for this work

Research output: Contribution to journalArticleScientificpeer-review

Abstract

Electronic states and their dynamics are of critical importance for electronic and optoelectronic applications. Here, various relevant electronic states in monolayer MoS2, such as multiple excitonic Rydberg states and free-particle energy bands are probed with a high relative contrast of up to >= 200 via broadband (from approximate to 1.79 to 3.10 eV) static third-harmonic spectroscopy (THS), which is further supported by theoretical calculations. Moreover, transient THS is introduced to demonstrate that third-harmonic generation can be all-optically modulated with a modulation depth exceeding approximate to 94% at approximate to 2.18 eV, providing direct evidence of dominant carrier relaxation processes associated with carrier-exciton and carrier-phonon interactions. The results indicate that static and transient THS are not only promising techniques for the characterization of monolayer semiconductors and their heterostructures, but also a potential platform for disruptive photonic and optoelectronic applications, including all-optical modulation and imaging.

Original languageEnglish
Article number2107104
Number of pages7
JournalAdvanced Materials
Volume34
Issue number3
Early online date23 Nov 2021
DOIs
Publication statusPublished - 20 Jan 2022
MoE publication typeA1 Journal article-refereed

Keywords

  • electronic states
  • monolayer transition metal dichalcogenides
  • static third-harmonic spectroscopy
  • third-harmonic generation
  • transient third-harmonic spectroscopy

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