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Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2.

Accepted version
Peer-reviewed

Type

Article

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Authors

Pogna, Eva AA 
Marsili, Margherita 
Dal Conte, Stefano 
Manzoni, Cristian 

Abstract

Transition metal dichalcogenides (TMDs) are emerging as promising two-dimensional (2D) semiconductors for optoelectronic and flexible devices. However, a microscopic explanation of their photophysics, of pivotal importance for the understanding and optimization of device operation, is still lacking. Here, we use femtosecond transient absorption spectroscopy, with pump pulse tunability and broadband probing, to monitor the relaxation dynamics of single-layer MoS2 over the entire visible range, upon photoexcitation of different excitonic transitions. We find that, irrespective of excitation photon energy, the transient absorption spectrum shows the simultaneous bleaching of all excitonic transitions and corresponding red-shifted photoinduced absorption bands. First-principle modeling of the ultrafast optical response reveals that a transient bandgap renormalization, caused by the presence of photoexcited carriers, is primarily responsible for the observed features. Our results demonstrate the strong impact of many-body effects in the transient optical response of TMDs even in the low-excitation-density regime.

Description

Keywords

many-body perturbation theory, real-time simulations, transient absorption spectroscopy, transition metal dichalcogenides, two-dimensional materials

Journal Title

ACS Nano

Conference Name

Journal ISSN

1936-0851
1936-086X

Volume Title

10

Publisher

American Chemical Society (ACS)
Sponsorship
Engineering and Physical Sciences Research Council (EP/K01711X/1)
Engineering and Physical Sciences Research Council (EP/K017144/1)
European Commission (604391)
Engineering and Physical Sciences Research Council (EP/L016087/1)