Optical two-dimensional coherent spectroscopy of excitons in transition-metal dichalcogenides

doi:10.1007/s11467-023-1345-8

Front. Phys.

2024, Vol. 19

Issue (2) : 23301 https://doi.org/10.1007/s11467-023-1345-8

VIEW & PERSPECTIVE

Optical two-dimensional coherent spectroscopy of excitons in transition-metal dichalcogenides

YanZuo Chen¹, ShaoGang Yu¹(

), Tao Jiang², XiaoJun Liu¹, XinBin Cheng^2,³, Di Huang²(

)

¹. State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China
². MOE Key Laboratory of Advanced Micro-Structured Materials, Shanghai Frontiers Science Center of Digital Optics, Institute of Precision Optical Engineering, and School of Physics Science and Engineering, Tongji University, Shanghai 200092, China
³. Shanghai Institute of Intelligent Science and Technology, Tongji University, Shanghai 200092, China

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Abstract

Exciton physics in atomically thin transition-metal dichalcogenides (TMDCs) holds paramount importance for fundamental physics research and prospective applications. However, the experimental exploration of exciton physics, including excitonic coherence dynamics, exciton many-body interactions, and their optical properties, faces challenges stemming from factors such as spatial heterogeneity and intricate many-body effects. In this perspective, we elaborate upon how optical two-dimensional coherent spectroscopy (2DCS) emerges as an effective tool to tackle the challenges, and outline potential directions for gaining deeper insights into exciton physics in forthcoming experiments with the advancements in 2DCS techniques and new materials.

Keywords monolayer transition-metal dichalcogenides two-dimensional coherent spectroscopy

Corresponding Author(s): ShaoGang Yu,Di Huang

Issue Date: 13 October 2023

Cite this article:

YanZuo Chen,ShaoGang Yu,Tao Jiang, et al. Optical two-dimensional coherent spectroscopy of excitons in transition-metal dichalcogenides[J]. Front. Phys. , 2024, 19(2): 23301.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-023-1345-8
https://academic.hep.com.cn/fop/EN/Y2024/V19/I2/23301

Fig.1 Typical time orderings of the excitation pulses to generate different types of time/frequency domain 2D spectra. (a) Zero-quantum spectrum for an inhomogeneously broadened V-shape three-state system with a ground state and two mutually dipole-forbidden excited states. (b) One-quantum spectrum for an inhomogeneously broadened three-state V system. (c) Double-quantum spectrum for a three-state ladder system where a doubly excited state exists.

Fig.2 (a) Left: Monolayer TMDCs crystal structure, along with the excitons and excitonic complexes. Right: Exciton resonance with valley-dependent optical selection excitation. (b) Zero-quantum 2D spectrum of monolayer

W S e 2

obtained with the cross-circular polarization pulses. The linewidth extracted along the mixing frequency axis gives the valley coherence time. (c) One-quantum 2D spectrum of monolayer

M o S e 2

obtained using cross-circular polarization pulses. The peaks X and T denote the excitons and trions, and the additional peaks XX and

T X b

(

X T b

) are associated with the neutral and charged bound biexciton, respectively. (d) Double-quantum 2D spectrum shows an unbound two-excitons state

X X

and bound biexciton state

X X b

. Panels adapted with permission from: (b) Ref. [28]; (c) Ref. [43], under a Creative Commons license CC BY 4.0; (d) Ref. [45].

Fig.3 Future directions of 2DCS in TMDCs.

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