Gas pressure-sensitive regulation of exciton state of monolayer tungsten disulfide

doi:10.1007/s11705-024-2483-4

Front. Chem. Sci. Eng.

2024, Vol. 18

Issue (11) : 131 https://doi.org/10.1007/s11705-024-2483-4

Gas pressure-sensitive regulation of exciton state of monolayer tungsten disulfide

Shuangping Han¹, Pengyu Zan¹, Yu Yan¹, Yaoxing Bian¹, Chengbing Qin²(

), Liantuan Xiao^1,²(

)

¹. College of Physics, Taiyuan University of Technology, Taiyuan 030024, China
². State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University, Taiyuan 030006, China

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Abstract

Over the past few decades, significant progress has been made in thin-film optoelectronic devices based on transition metal dichalcogenides. However, the exciton states’ sensitivity to the environment presents challenges for device applications. This study reports the evolution of photoinduced exciton states in monolayer tungsten disulfide in a low-pressure environment to help elucidate the physical mechanism of the transition between neutral and charged excitons. At 222 mTorr, the transition rate between excitons comprises two components: 0.09 s^–1 and 1.68 s^–1. Based on this phenomenon, we developed a pressure-tuning method that allows for a tuning range of approximately 40% of exciton weight. Our study demonstrates that the intensity of neutral exciton emission from monolayer tungsten disulfide follows a power-law distribution in relation to pressure, indicating a highly sensitive pressure dependence. We provide a nondestructive and highly sensitive method for exciton conversion through in situ optical manipulation. This highlights the potential development of monolayer tungsten disulfide for pressure sensors and explains the impact of environmental factors on the product quality in photovoltaic devices. In addition, it demonstrates the promising future of monolayer transition metal dichalcogenides in applications such as photovoltaic devices and miniature biochemical sensors.

Keywords neutral exciton state charged exciton state transition metal dichalcogenides pressure sensitive

Corresponding Author(s): Chengbing Qin,Liantuan Xiao

Just Accepted Date: 31 May 2024 Issue Date: 30 August 2024

Cite this article:

Shuangping Han,Pengyu Zan,Yu Yan, et al. Gas pressure-sensitive regulation of exciton state of monolayer tungsten disulfide[J]. Front. Chem. Sci. Eng., 2024, 18(11): 131.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-024-2483-4
https://academic.hep.com.cn/fcse/EN/Y2024/V18/I11/131

Fig.1 Experimental setup and sample characterization. (a) Schematic diagram of the confocal microscopy imaging system. The 4f system ensures the light focuses on the sample within the scanning range. M: mirror; DM: dichroic mirror; SPCM: single photon counting module. (b) optical imaging of the mechanical exfoliated (ME) WS₂. The contour surrounded by the red dotted line is the monolayer WS₂ (1L-WS₂) region. The inset is the height profile of the marked line in the optical image produced through atomic force microscopy. Scale bar: 20 μm. (c) PL spectra of ME 1L-WS₂. The gray dots represent the experimental data, the solid red line is the sum curve obtained through the 2-peak Lorentz fitting, and the green and magenta represent the emission of A⁰ and A^? excitons, respectively. (d) Raman spectra of ME 1L-WS₂. The Raman signal of the silicon substrate is located at 521 cm^?1. The other two peaks are E_2g and A_1g Raman modes of the WS₂, with second-order longitudinal acoustic phonons emission also included in the left peak. Test temperature: room temperature.

Fig.2 Characterization of photoluminescence (PL) spectra at 760 Torr and 222 mTorr. (a, b) Two-dimensional intensity imaging of ME 1L-WS₂ at 760 Torr and 222 mTorr, respectively. The horizontal axis is the wavelength, while the vertical axis represents time (determined by the number of acquisition frames. Frame rate: 0.1 s/frame). (c, d) Time evolution of PL intensity at the peak position of A⁰ and A^? at 760 Torr and 222 mTorr, respectively.

Fig.3 Emission spectra of ME 1L-WS₂ at 222 mTorr. (a) PL intensity as a function of irradiation time; (b) PL spectra of ME 1L-WS₂ at different times at 222 mTorr; (c) Upper panel: Evolution of neutral-charged exciton conversion with time, where the magenta triangle and green circle are the spectral weights of A⁰ and A^?, respectively. The blue and black solid lines are the fitting results, which follow a bi-exponential distribution, representing the roles of laser radiation and gas pressure in the conversion process, respectively. Lower panel: The variation of the spectral weight of each exciton relative to the stable-stage average value; (d) Upper panel: The time evolution of the peak energy of A⁰ and A^? by Lorentz bimodal fitting. Lower panel: The variation in peak energy difference between A⁰ and A^? over time.

Tab.1 Bi-exponential fitting results of the curves in Fig.3(c) and Fig.3(d), in which the conversion rate of charged excitons and ΔE shows a high consistency

Fig.4 Exciton engineering based on pressure. (a) The evolution of conversion efficiency between A⁰ and A^? with pressure. The green circle and red triangle are the fitting results of

η A 0

and

η A ?

, respectively; (b) the evolution of the pressure as a function of the emission intensity. The red triangles correspond to A⁰; the dotted line is the power-law fitting trajectory. The green circle represents A^?.

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[1]	Yulun Liu, Yaojie Zhu, Zuowei Yan, Ruixue Bai, Xilin Zhang, Yanbo Ren, Xiaoyu Cheng, Hui Ma, Chongyun Jiang. Excitonic devices based on two-dimensional transition metal dichalcogenides van der Waals heterostructures[J]. Front. Chem. Sci. Eng., 2024, 18(2): 16-.

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