Surface structure effect of F<sub>4</sub>TCNQ/MoS<sub>2</sub> nanocomposite heteromaterials on surface-enhanced Raman scattering

Liu Wen-Ying; Wang Gong-Tang; Duan Peng-Yi; Zhang Wen-Jie; Zhang Can; Hu Xiao-Xuan; Liu Mei

doi:10.7498/aps.72.20221958

Abstract

Surface-enhanced Raman scattering (SERS) has been widely used in food and drug detection, biological and medical sensing. In recent years, the study of non-metallic SERS substrates has gradually become a hot field of SERS. Here, we investigate the modulation effect on SERS activities of 2,3,5,6-tetrafluoro-7,7,8,8-tetrachyanoquindimethylene (F₄TCNQ) grown on molybdenum disulfide (MoS₂) films. The different nanostructures of F₄TCNQ can have an effect on the bound capability of charges transferred from the surface of MoS₂, which changes the electron density distribution on the surface of the F₄TCNQ/MoS₂ nanocomposite material. Therefore, the interface exhibits different charge localizations in the F₄TCNQ/MoS₂ nanocomposite. The charge transfer efficiency between the substrate and the adsorbed probe molecules leads the substrate to show a different SERS sensitivity. The enhancement factor of 4-mercaptobenzoic acid (4-MBA) molecules on the most optimized 7-min F₄TCNQ/MoS₂ nanocomposite substrate can reach $ 6.9\times {10}^{4} $, and the detection limit concentration is as low as 10^–6 mol/L. The result of research on F₄TCNQ/MoS₂ nanocomposite provides an effective optimization scheme of energy level regulation for SERS based on the chemical enhancement mechanism, and opens up a new way to further exploit its functional applications.

Keywords:

Authors and contacts

School of Physics and Electronics, Shandong Normal University, Jinan 250358, China

Corresponding author: Wang Gong-Tang, wanggt@sdnu.edu.cn ; Liu Mei, liumei@sdnu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 12074229).

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References

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图 1 (a)纯和(b)喷金MoS₂薄膜的扫描电子显微镜图; (c)—(g) 不同生长时间的F₄TCNQ/MoS₂ (T₁—T₅)的扫描电子显微镜图(喷金); (f) MoS₂薄膜上F₄TCNQ纳米岛的数量和直径随时间分布图

Figure 1. SEM images of (a) pure MoS₂ and (b) gold-sprayed MoS₂ thin films; (c)−(g) SEM images of F₄TCNQ/MoS₂ (T₁−T₅) with different growth times (gold-sprayed); (f) the quantity and size distributions of F₄TCNQ nanoisland deposited on MoS₂ film over time.

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图 2 (a), (b) MoS₂薄膜边缘处的AFM图和相应的高度图; (c), (d) 小范围的MoS₂薄膜表面的AFM图和相应高度图; (e)—(i) T₁—T₅样品的形貌图、沿图中直线扫描的高度和接触电势差谱线图

Figure 2. (a), (b) The AFM image and the corresponding height profile of the edge of MoS₂ film, respectively. (c), (d) The AFM image and the corresponding height profile of the small range of MoS₂ film surfaces, respectively. (e)−(i) The topography of T₁−T₅ samples, height and CPD spectrum scanned along the line in AFM figures.

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图 3 (a) 10 $\text{μ}\rm{L}$水滴在纯MoS₂薄膜和T₂基底上的光学图像; (b) F₄TCNQ, MoS₂和T₁—T₅的拉曼光谱; (c) F₄TCNQ, MoS₂和T₁—T₅的光致发光谱

Figure 3. (a) Optical images of 10 $\text{μ}\rm{L}$ water droplet on pristine MoS₂ film and T₂ substrate; (b) Raman spectra of F₄TCNQ, MoS₂ and T₁−T₅; (c) PL spectra of F₄TCNQ, MoS₂ and T₁−T₅.

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图 4 4-MBA分子(10^–3 mol/L)在T₁—T₅上的拉曼光谱(a)及其拉曼峰强度与生长时间之间的关系(b); (c) 5组4-MBA分子(10^–3 mol/L)在T₁—T₅基底上的1593 $ {\rm{c}\rm{m}}^{-1} $处的拉曼峰强度与生长时间之间的关系; (d) 10^–3 mol/L浓度的4-MBA分子在不同基底上的拉曼光谱; (e) 不同浓度(10^–7—10^–3 mol/L)的4-MBA分子在T₂上的SERS图谱; (f) T₂基底上4-MBA 分子的1097 $ {\rm{c}\rm{m}}^{-1} $和1593 $ {\rm{c}\rm{m}}^{-1} $处的拉曼峰值强度与浓度之间的关系; (g) F₄TCNQ/MoS₂纳米复合异质结构的电荷转移以及该基底与4-MBA探针分子的电荷转移示意图

Figure 4. The Raman spectra (a) of 4-MBA molecules (10^–3 mol/L) on T₁−T₅ substrates; (b) the interrelationship between the corresponding Raman peak intensities and different growth times in the panel (a); (c) the relationship of the Raman peak intensity at 1593 $ {\rm{c}\rm{m}}^{-1} $ for 5 groups of 4-MBA molecules (10^–3 mol/L) on T₁−T₅ substrates and the growth times; (d) Raman spectra of 4-MBA molecules on different substrates; (e) SERS spectra of 4-MBA molecules on T₂ substrate with different concentrations (10^–7− 10^–3 mol/L); (f) the relationship between the intensity of the SERS peak at 1097 and 1593 $ {\rm{c}\rm{m}}^{-1} $ and different 4-MBA concentrations; (g) the schematic of the charge transfer (CT) pathways in F₄TCNQ/MoS₂ nanocomposite heterostructures and the CT pathways between F₄TCNQ/MoS₂ substrate and 4-MBA probe molecule.

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图 5 (a) R6G分子(10^–9 mol/L)在T₁—T₅基底上的拉曼光谱; (b) MB分子(10^–5 mol/L)在T₁—T₅基底上的拉曼光谱; (c) R6G分子的拉曼峰强度与生长时间之间的关系; (d) MB分子的拉曼峰强度与生长时间之间的关系

Figure 5. (a) The Raman spectra of R6G molecules (10^–9 mol/L) on T₁−T₅ substrates; (b) the Raman spectra of MB molecules (10^–5 mol/L) on T₁−T₅ substrates; (c) the interrelationship between the Raman peak intensities of R6G molecules and growth times; (d) the interrelationship between the Raman peak intensities of MB molecules and growth times.

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表 1 MoS₂和T₁—T₅样品的水接触角、CPD和相应的费米能级值

Table 1. Water contact angles, CPD values and corresponding Fermi level values on MoS₂ and T₁−T₅ substrates.

检测基底	角度/(°)	CPD/$ \rm{V} $	费米能级/$ \rm{e}\rm{V} $
MoS₂	$ 47\pm 0.2 $	0.048	–5.08
T₁	$ 66.6\pm 1.1 $	–0.1	–5.23
T₂	$ 68\pm 0.9 $	–0.043	–5.17
T₃	$ 70.7\pm 1.6 $	–0.168	–5.3
T₄	$ 71\pm 2.8 $	–0.083	–5.21
T₅	$ 72.6\pm 2 $	–0.129	–5.26

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[1]	Zhang W, Ma J, Sun D W 2021 Crit. Rev. Food Sci. Nutr. 61 2623 Google Scholar
[2]	Zhang D, Pu H, Huang L, Sun D W 2021 Trends Food Sci. Technol. 109 690 Google Scholar
[3]	Zanchi C, Giuliani L, Lucotti A, Pistaffa M, Trusso S, Neri F, Tommasini M, Ossi P M 2020 Appl. Surf. Sci. 507 145109 Google Scholar
[4]	Premasiri W R, Lee J C, Sauer-Budge A, Theberge R, Costello C E, Ziegler L D 2016 Anal. Bioanal. Chem. 408 4631 Google Scholar
[5]	Perumal J, Wang Y, Attia A B E, Dinish U S, Olivo M 2021 Nanoscale 13 553 Google Scholar
[6]	Wei H, Peng Z, Yang C, Tian Y, Sun L, Wang G, Liu M 2021 Nanomaterials 11 2026 Google Scholar
[7]	Camden J P, Dieringer J A, Wang Y, Masiello D J, Marks L D, Schatz G C, Van Duyne R P 2008 J. Am. Chem. Soc. 130 12616 Google Scholar
[8]	Shafi M, Zhou M, Duan P, Liu W, Zhang W, Zha Z, Gao J, Wali S, Jiang S, Man B, Liu M 2022 Sensors and Actuators B: Chem. 356 131360 Google Scholar
[9]	Wang G, Wei H, Tian Y, Wu M, Sun Q, Peng Z, Sun L, Liu M 2020 Opt. Express 28 18843 Google Scholar
[10]	Ling X, Xie L, Fang Y, Xu H, Zhang H, Kong J, Dresselhaus M S, Zhang J, Liu Z 2010 Nano Lett. 10 553 Google Scholar
[11]	Liu M, Shi Y, Zhang G, Zhang Y, Wu M, Ren J, Man B 2018 Appl. Spectrosc. 72 1613 Google Scholar
[12]	Tian Y, Wei H, Xu Y, et al. 2020 Nanomaterials 10 1910 Google Scholar
[13]	Ling X, Fang W, Lee Y H, Araujo P T, Zhang X, Rodriguez-Nieva J F, Lin Y, Zhang J, Kong J, Dresselhaus M S 2014 Nano Lett. 14 3033 Google Scholar
[14]	Muehlethaler C, Considine C R, Menon V, Lin W C, Lee Y H, Lombardi J R 2016 ACS Photon. 3 1164 Google Scholar
[15]	Li J, Xu X, Huang B, Lou Z, Li B 2021 ACS Appl. Mater. Inter. 13 10047 Google Scholar
[16]	Zheng Z, Cong S, Gong W, Xuan J, Li G, Lu W, Geng F, Zhao Z 2017 Nat. Commun. 8 1993 Google Scholar
[17]	Chen L, Xie Q, Wan L, Zhang W, Fu S, Zhang H, Ling X, Yuan J, Miao L, Shen C, Li X, Zhang W, Zhu B, Wang H-Q 2019 ACS Appl. Energy Mater. 2 5862 Google Scholar
[18]	Mun J, Kang J, Zheng Y, Luo S, Wu Y, Gong H, Lai J C, Wu H C, Xue G, Tok J B H, Bao Z 2020 Adv. Electron. Mater. 6 2000251 Google Scholar
[19]	Wang H, Levchenko S V, Schultz T, Koch N, Scheffler M, Rossi M 2019 Adv. Electron. Mater. 5 1800891 Google Scholar
[20]	Venables J, Spiller G, Hanbucken M 1999 Rep. Prog. Phys. 47 399 Google Scholar
[21]	Park J, Choudhary N, Smith J, Lee G, Kim M, Choi W 2015 Appl. Phys. Lett. 106 012104 Google Scholar
[22]	McHale G, Aqil S, Shirtcliffe N J, Newton M I, Erbil H Y 2005 Langmuir 21 11053 Google Scholar
[23]	Xiao K, Rondinone A J, Puretzky A A, Ivanov I N, Retterer S T, Geohegan D B 2009 Chem. Mater. 21 4275 Google Scholar
[24]	Newaz A K M, Prasai D, Ziegler J I, Caudel D, Robinson S, Haglund Jr R F, Bolotin K I 2013 Solid State Commun. 155 49 Google Scholar
[25]	Finkelstein G, Shtrikman H, Bar-Joseph I I 1995 Phys. Rev. Lett. 74 976 Google Scholar
[26]	Tongay S, Suh J, Ataca C, Fan W, Luce A, Kang J S, Liu J, Ko C, Raghunathanan R, Zhou J, Ogletree F, Li J, Grossman J C, Wu J 2013 Sci. Rep. 3 2657 Google Scholar
[27]	Ji P, Mao Z, Wang Z, Xue X, Zhang Y, Lv J, Shi X 2019 Nanomaterials 9 983 Google Scholar
[28]	Wu H, Wang H, Li G 2017 Analyst 142 326 Google Scholar
[29]	Jiang X, Sun X, Yin D, Li X, Yang M, Han X, Yang L, Zhao B 2017 Phys. Chem. Chem. Phys. 19 11212 Google Scholar
[30]	Kuhrt R, Hantusch M, Buechner B, Knupfer M 2021 J. Phys. Chem. C 125 18961 Google Scholar
[31]	Wang J, Ji Z, Yang G, Chuai X, Liu F, Zhou Z, Lu C, Wei W, Shi X, Niu J, Wang L, Wang H, Chen J, Lu N, Jiang C, Li L, Liu M 2018 Adv. Funct. Mater. 28 1806244 Google Scholar
[32]	Le O K, Chihaia V, Van On V, Son D N 2021 RSC Adv. 11 8033 Google Scholar
[33]	Ji L F, Fan J X, Zhang S F, Ren A M 2018 Phys. Chem. Chem. Phys. 20 3784 Google Scholar
[34]	Deneme I, Liman G, Can A, Demirel G, Usta H 2021 Nat. Commun. 12 6119 Google Scholar

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Surface structure effect of F₄TCNQ/MoS₂ nanocomposite heteromaterials on surface-enhanced Raman scattering

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Corresponding author: Wang Gong-Tang, wanggt@sdnu.edu.cn ; Liu Mei, liumei@sdnu.edu.cn

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Surface structure effect of F4TCNQ/MoS2 nanocomposite heteromaterials on surface-enhanced Raman scattering

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Corresponding author: Wang Gong-Tang, wanggt@sdnu.edu.cn ; Liu Mei, liumei@sdnu.edu.cn

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Surface structure effect of F₄TCNQ/MoS₂ nanocomposite heteromaterials on surface-enhanced Raman scattering