Alloy engineering of excitonic properties in TMD monolayers

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.

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Journal
Physical Review Materials
Published
2026-10-26
DOI
https://doi.org/10.1103/m7kc-8q5v
Primary Topic
2D Materials and Applications
Type
article
Field-Weighted Citation Impact
0.00

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article

Alloy engineering of excitonic properties in TMD monolayers

Ioannis Paradisanos, Iann C. Gerber, Adlen Smiri, Georgios Kopidakis et al.
3 links
Physical Review Materials
2D Materials and Applications
article

Alloy engineering of excitonic properties in TMD monolayers

Ioannis Paradisanos, Iann C. Gerber, Adlen Smiri, Georgios Kopidakis, George Kioseoglou, E. Katsipoulaki, Konstantinos Mourzidis, Danae Katrisioti, Takashi Taniguchi, Kenji Watanabe, Zdenek Sofer, Emmanuel Stratakis, Xavier Marie, Panagiotis Spiliotakis, Gang Wang
article en

Abstract

We investigate monolayer MoS$_{2x}$Se$_{2(1-x)}$ alloys across the full composition range using optical spectroscopy. We demonstrate continuous tuning of the optical gap over $\sim$0.35 eV, accompanied by a systematic reduction of the B--A exciton splitting, in agreement with density functional theory calculations. Temperature-dependent measurements reveal a progressive increase of the average phonon energy from Se-rich to S-rich alloys that follows a simple reduced-mass scaling model. Polarization-resolved spectroscopy further shows a monotonic increase of the circular polarization from nearly zero in MoSe$_2$ to $\sim$15\% in MoS$_2$ at 78 K. The observed evolution of the polarization is attributed to alloy-induced modifications of the electronic structure that modify bright--dark exciton mixing and the associated valley depolarization. These findings establish alloy engineering as an effective strategy for controlling excitonic properties in TMD monolayers.

Physical Review MaterialsVol. 10(10)
Beijing Institute of Technology (CN), Centre National de la Recherche Scientifique (FR), University of Crete (GR), Institut Universitaire de France (FR), National Institute for Materials Science (JP), Laboratoire de Physique et Chimie des Nano-Objets (FR), Université de Toulouse (FR), Institut National des Sciences Appliquées de Lyon (FR), Foundation for Research and Technology Hellas (GR), University of Chemistry and Technology, Prague (CZ)
Centre Informatique National de l’Enseignement Supérieur, Equipex, Agence Nationale de la Recherche, Japan Science and Technology Corporation, Ministry of Education, Culture, Sports, Science and Technology, Ministerstvo Školství, Mládeže a Tělovýchovy, Dynasty Foundation, Grand Équipement National De Calcul Intensif, HORIZON EUROPE Framework Programme, Core Research for Evolutional Science and Technology
Openalex Percentile: Top 56%
2D Materials and Applications
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