等离子体轰击单层WS<sub>2</sub>引入缺陷态对束缚激子光学性质的影响

刘海洋; 范晓跃; 范豪杰; 李阳阳; 唐天鸿; 王刚

doi:10.7498/aps.73.20240475

摘要

单层过渡金属硫化物具有原子级厚度、直接带隙、强自旋轨道耦合等优异性能, 使其在自旋电子学、光电子学等领域具有重要的研究价值和广泛的应用前景. 通常材料中包含多种结构缺陷, 这可能是在样品制备和生长过程中形成的, 也可以经过后期处理产生, 这些缺陷会显著改变其物理化学性质. 因此, 控制和理解缺陷是调控材料性质的重要途径. 本文利用氩等离子体对机械剥离的单层WS₂进行轰击处理, 通过控制轰击时间引入不同密度的缺陷. 光致发光和拉曼测试结果表明, 在未改变晶格结构的前提下, 引入了两种缺陷态的束缚激子, 两种激子的动力学过程与中性激子相比明显变慢. 对比真空和大气环境下的光致发光光谱(photoluminescence spectroscopy, PL), 两种激子的强度变化呈现相反的行为. 本文的研究结果可为二维材料缺陷的引入和调控以及特征光谱的研究提供依据.

关键词:

二维半导体 /
WS₂ /
缺陷态 /
激子

Abstract

Monolayer transition metal dichalcogenides (TMDCs) exhibit exceptional properties including atomic-scale thickness, direct bandgap, and strong spin-orbit coupling, which make them have great potential applications in spintronics, optoelectronics, and other fields. Usually, materials contain various structural defects, which are either formed during preparation and growth or induced by subsequent treatments. These defects can significantly change their physicochemical properties. Consequently, controlling and comprehending defects is an important approach to adjusting the properties of these materials.Herein, we use Ar⁺ plasma to bombard monolayer WS_2, which is exfoliated mechanically, thereby introducing defects whose density is controlled by changing the bombardment duration. The photoluminescence (PL) and Raman spectroscopic measurements at different temperatures and power values are utilized to investigate the optical properties of the defects. Furthermore, time-resolved photoluminescence is employed to unveil the dynamic behaviors of free and trapped excitons.The bombardment can introduce different types of defects into typical two-dimensional (2D) TMDCs such as MoS₂ and WS₂. Single sulfur vacancies are frequently generated, while other defects like double sulfur vacancies or metal atom vacancies can also occur. Exciton effects dominate the optical properties of monolayer TMDCs due to reduced screening and large effective mass. At low temperatures, bound exciton emissions arise from trapped states. Our measurements reveal two types of defect-bound excitons from the PL spectra at around 1.85 eV (X^B1) and 1.55 eV (X^B2). Meanwhile, the Raman peaks of the samples before and after treatment exhibit no obvious changes, indicating that the lattice structure remaines unchanged. After the Ar⁺ bombardment, the intensity of the free neutral exciton significantly decreases to 1/6 of untreated WS₂, owing to the free exciton population and the increased non-radiative centers. The dynamic processes of these two bound excitons are considerably slower than the neutral exciton’s, showing the typical dynamic behavior of defect-bound excitons. Furthermore, comparison between the PL under vacuum condition and the PL under atmospheric condition shows that the intensities of the two bound excitons exhibit opposing behaviors. In an atmospheric environment, neutral excitons and bound exciton X^B1 possess higher intensities. In the vacuum, the strength of neutral exciton and X^B1 decrease quickly, while the intensity of deep-level bound exciton X^B2 increases.In summary, we observe two bound exciton states arising from specific vacancy states in monolayer WS₂ after Ar⁺ bombardment. Their energy values are 200 meV and 500 meV lower than those of the neutral exciton, with a splitting energy value being about 300 meV. The detailed evolution of the relative spectral weight with temperature and excitation power are presented. This work provides insights into the generation, control, and characteristic spectra of defects in 2D materials.

Keywords:

作者及机构信息

北京理工大学物理学院, 量子物理实验中心, 先进光电量子结构设计与测量教育部重点实验室, 北京　100081

通信作者: 王刚, gw@bit.edu.cn

基金项目: 国家自然科学基金(批准号: 12074033)和北京理工大学科技创新计划培育专项(批准号: 2022CX01007)资助的课题.

Authors and contacts

Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement (Ministry of Education), Center for Quantum Physics, School of Physics, Beijing Institute of Technology, Beijing 100081, China

Corresponding author: Wang Gang, gw@bit.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12074033) and the Beijing Institute of Technology Science and Innovation Cultivation Program, China (Grant No. 2022CX01007).

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施引文献

图 1 (a)经过20 s处理的单层WS₂; (b)经过30 s处理的单层WS₂, 插图为处理前的单层WS₂; (c)室温下, 处理前后样品的PL谱; (d)室温下, 处理前后样品的Raman谱; (e)室温下, 处理前后样品的白光反射谱; (f)室温下, 处理前后样品的PL谱, 为图(c)淡蓝色区域位置的放大

Fig. 1. (a) Monolayer WS₂ after 20 s treatment; (b) monolayer WS₂ after 30 s treatment, the insets are the monolayer WS₂ before treatment; (c) PL spectra of the samples before and after treatment at room temperature; (d) Raman spectra of the samples before and after treatment at room temperature; (e) reflectivities of the samples before and after treatment at room temperature; (f) PL spectra of the sample before and after treatment at room temperature, zoom-in of the spectral range marked by the blue rectangle zone in panel (c).

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图 2 (a) 77 K下未处理的单层和经过20 s, 30 s处理的单层WS₂的PL谱; (b), (c)经过20 s, 30 s处理的单层WS₂变温PL谱; (d)经过20 s, 30 s处理的样品X^B1(X^B2)发光峰强度和X⁰强度比值随温度的变化; (e), (f)经过20 s, 30 s处理的单层WS₂的X⁰, X^B1, X^B2峰位随温度的变化

Fig. 2. (a) PL spectra of untreated monolayer WS₂ and monolayers treated for 20 s and 30 s at 77 K; (b), (c) temperature dependent PL spectra of monolayer WS₂ after 20 s and 30 s treatment; (d) temperature dependent PL intensity ratio of bound excitons X^B1 and X^B2 over X⁰ of monolayers treated for 20 s and 30 s; (e), (f) temperature dependent peak energies of X⁰, X^B1, and X^B2 of monolayers treated for 20 s and 30 s.

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图 3 200 K温度下功率依赖PL结果　(a)—(c) 20 s处理样品的结果; (d)—(f) 30 s处理样品的结果; (a), (d)样品变功率PL光谱; (b), (e)样品X^B1(X^B2)发光峰强度和X⁰强度比值随功率的变化; (c), (f)样品X⁰, X^B1, X^B2发光峰强度积分随功率的变化

Fig. 3. Power dependent PL results at 200 K: (a)–(c) Results of monolayer treated for 20 s; (d)–(f) results of monolayer treated for 30 s; (a), (d) power dependent PL spectra; (b), (e) power dependent PL intensity ratio of bound excitons X^B1 and X^B2 over X⁰; (c), (f) power dependent PL intensities of X⁰, X^B1, X^B2.

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图 4 (a) 150 K下30 s处理的样品变功率的PL; (b) 30 s处理的样品中X^B1变功率的PL; (c) 30 s处理的样品中X⁰变功率的PL

Fig. 4. (a) Power dependent PL spectra of the sample treated for 30 s at 150 K; (b) power dependent PL spectra of X^B1 in the sample treated for 30 s; (c) power dependent PL spectra of X⁰ in the sample treated for 30 s.

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图 5 20 s和30 s处理样品的时间分辨光谱　(a) 77 K; (b) 300 K

Fig. 5. Time-resolved PL of monolayer treated for 20 s and 30 s: (a) 77 K; (b) 300 K.

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图 6 室温下, 大气环境和真空下单层WS₂的PL　(a)未处理的单层; (b) 20 s处理的单层; (c) 30 s处理的单层

Fig. 6. PL of monolayer WS₂ under atmosphere and vacuum conditions at room temperature: (a) Results of untreated monolayer WS₂; (b) results of monolayer WS₂ treated for 20 s; (c) results of monolayer WS₂ treated for 30 s.

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map

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