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 ≈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.
| Original language | English |
|---|---|
| Article number | 2107104 |
| Pages (from-to) | e2107104 |
| Journal | Advanced Materials |
| Volume | 34 |
| Issue number | 3 |
| Early online date | 23 Nov 2021 |
| DOIs | |
| Publication status | Published - 20 Jan 2022 |
Bibliographical note
Publisher Copyright:© 2021 Wiley-VCH GmbH
Funding
Y.W. and F.I. contributed equally to this work. The authors acknowledge the financial support from Aalto Centre for Quantum Engineering, Academy of Finland (grants: 314810, 333982, 336144, and 336818), Academy of Finland Flagship Programme (320167, PREIN), the European Union's Horizon 2020 Research and Innovation Program (grant agreement no. 820423,S2QUIP; 965124, FEMTOCHIP), the EU H2020‐MSCA‐RISE‐872049 (IPN‐Bio), Foundation for Aalto University Science and Technology and Finnish Foundation for Technology Promotion (grant: 8216), the EU H2020‐MSCA‐RISE‐872049 (IPN‐Bio), ERC (834742 and 789104‐eNANO), the Spanish MINECO (Severo Ochoa CEX2019‐000910‐S), and Fundaciós Cellex. Y.W. and F.I. contributed equally to this work. The authors acknowledge the financial support from Aalto Centre for Quantum Engineering, Academy of Finland (grants: 314810, 333982, 336144, and 336818), Academy of Finland Flagship Programme (320167, PREIN), the European Union's Horizon 2020 Research and Innovation Program (grant agreement no. 820423,S2QUIP; 965124, FEMTOCHIP), the EU H2020-MSCA-RISE-872049 (IPN-Bio), Foundation for Aalto University Science and Technology and Finnish Foundation for Technology Promotion (grant: 8216), the EU H2020-MSCA-RISE-872049 (IPN-Bio), ERC (834742 and 789104-eNANO), the Spanish MINECO (Severo Ochoa CEX2019-000910-S), Fundacio?s Cellex, and the Swedish Research Council (VR 2018-04252). Note: The acknowledgements section was updated on January 20, 2022, after initial publication online.
| Funders | Funder number |
|---|---|
| Aalto Centre for Quantum Engineering, Academy of Finland | 314810, 336144, 336818, 333982 |
| EU H2020‐MSCA‐RISE‐872049 | |
| Foundation for Aalto University Science and Technology | |
| Fundación Cellex | |
| Horizon 2020 Framework Programme | 834742, 872049 |
| European Commission | |
| European Research Council | 789104‐eNANO |
| Academy of Finland | 320167 |
| Ministerio de Economía y Empresa | |
| Vetenskapsrådet | VR 2018-04252 |
| Tekniikan Edistämissäätiö | 8216 |
| Horizon 2020 | 820423, 965124 |
ASJC Scopus subject areas
- General Materials Science
- Mechanics of Materials
- Mechanical Engineering