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

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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
Issue number3
Early online date23 Nov 2021
Publication statusPublished - 20 Jan 2022
MoE publication typeA1 Journal article-refereed


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


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