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Probing Electronic States in Monolayer Semiconductors through Static and Transient Third-Harmonic Spectroscopies
Stockholm University, Nordic Institute for Theoretical Physics (Nordita).ORCID iD: 0000-0002-9521-1008
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Number of Authors: 132022 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 34, no 3, article id 2107104Article in journal (Refereed) Published
Abstract [en]

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 ≈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 ≈94% at ≈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.

Place, publisher, year, edition, pages
2022. Vol. 34, no 3, article id 2107104
Keywords [en]
electronic states, monolayer transition metal dichalcogenides, static third-harmonic spectroscopy, third-harmonic generation, transient third-harmonic spectroscopy
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:su:diva-199505DOI: 10.1002/adma.202107104ISI: 000721484000001PubMedID: 34743375Scopus ID: 2-s2.0-85119667671OAI: oai:DiVA.org:su-199505DiVA, id: diva2:1619352
Available from: 2021-12-13 Created: 2021-12-13 Last updated: 2022-10-25Bibliographically approved

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Rostami, Habib

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