J. Semicond. > 2021, Volume 42 > Issue 5 > 051001, doi: 10.1088/1674-4926/42/5/051001
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REVIEWS

Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene

Enqing Zhang1, 2, Zhengkun Xing1, 2, Dian Wan1, 2, Haoran Gao1, 2, Yingdong Han1, 2, Yisheng Gao3, Haofeng Hu1, 2, , Zhenzhou Cheng1, 2, 4, and Tiegen Liu1, 2

+ Author Affiliations

 Corresponding author: Haofeng Hu, haofeng_hu@tju.edu.cn; Zhenzhou Cheng, zhenzhoucheng@tju.edu.cn

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Abstract: Surface-enhanced Raman spectroscopy (SERS) based on two-dimensional (2D) materials has attracted great attention over the past decade. Compared with metallic materials, which enhance Raman signals via the surface plasmon effect, 2D materials integrated on silicon substrates are ideal for use in the fabrication of plasmon-free SERS chips, with the advantages of outstanding fluorescence quenching capability, excellent biomolecular compatibility, tunable Fermi levels, and potentially low-cost material preparation. Moreover, recent studies have shown that the limits of detection of 2D-material-based SERS may be comparable with those of metallic substrates, which has aroused significant research interest. In this review, we comprehensively summarize the advances in SERS chips based on 2D materials. As several excellent reviews of graphene-enhanced Raman spectroscopy have been published in the past decade, here, we focus only on 2D materials beyond graphene, i.e., transition metal dichalcogenides, black phosphorus, hexagonal boron nitride, 2D titanium carbide or nitride, and their heterostructures. We hope that this paper can serve as a useful reference for researchers specializing in 2D materials, spectroscopy, and diverse applications related to chemical and biological sensing.

Key words: Raman spectroscopy, surface-enhanced Raman spectroscopy, two-dimensional materials



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Fig. 1.  (Color online) Schematics of the mechanisms of SERS. (a) With respect to EMs, when the incident laser is in resonance with the nanoparticle LSPR frequency, the incident laser excites electrons on the metal surface, leading to a polarization of charge and oscillating dipoles. As the frequencies of Raman scattering light are close to that of the incident laser, the resonance also increases the intensity of the Raman scattering light. (b) For CMs, electrons are transferred from the Fermi level of the substrate to the LUMO of the molecule, thereby forming a charge transfer intermediate. The energy transition ($ {\mu }_{\rm{CT}} $) between the Fermi level of the substrate and LUMO is much stronger than that ($ {\mu }_{\rm{mol}} $) between the highest occupied molecular orbit (HOMO) and LUMO, resulting in a higher Raman scattering cross-section.

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Fig. 2.  (Color online) Comparison of various 2D materials beyond graphene for SERS applications, including TMDs, BP, h-BN, MXenes, and their heterostructures.

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Fig. 3.  (Color online) SERS studies based on TMDs. (a) Schematic of measurement and enhanced Raman spectra of 4-mercaptopyridine on monolayer MoS2. (b) Energy levels of the oxygen-incorporation MoS2-R6G system. Here, $ {\mu }_{\rm{ex}} $ and $ {\mu }_{\rm{mol}} $ denote exciton transition and molecular transition, and $ {\mu }_{\rm{PICT}} $ denotes PICT. (c) Measured Raman spectra of R6G molecules on 1T MoSe2, 1T MoS2, 2H MoSe2, and 2H MoS2 substrates. (d) Measured Raman spectra of $ 4\times {10}^{-7}\;{\rm{M}} $ R6G on a 1T’-WTe2 substrate, with and without the DBR. (a) is reprinted with permission from Ref. [50]. Copyright © 2016 American Chemical Society. (b) is reprinted with permission from Ref. [53]. Copyright © 2017, Nature Publishing Group. (c) is reprinted with permission from Ref. [57]. Copyright © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) is reprinted with permission from Ref. [58]. Copyright © 2018 American Chemical Society.

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Fig. 4.  (Color online) SERS studies based on h-BN, BP, and MXenes. (a) Preparation of SERS chips based on graphene, h-BN, and MoS2. The layered 2D materials are shown in gray, while probe molecules are shown in red. (b) Raman spectra of CuPc molecules on SiO2/Si (black line), MoS2 (green line), h-BN (red line), and graphene (blue line) substrates. (c) Raman spectra of RhB molecules (~10–8 M) on a BP substrate, showing different Raman peaks, which could be attributed to different vibrational transitions in the RhB molecules. (d) Schematic of Ti2NTx, etched and delaminated from Ti2AlN, and employed as a SERS substrate. (a) and (b) are reprinted with permission from Ref. [68]. © 2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim. (c) is reprinted with permission from Ref. [80]. Copyright © 2019 the Royal Society of Chemistry. (d) is reprinted with permission from Ref. [92]. Copyright © 2017 American Chemical Society.

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Fig. 5.  (Color online) SERS studies based on 2D heterostructures. (a) Schematic of Raman measurement of CuPc molecular coating on G/W/G/W chips. (b) Raman spectra of CuPc molecular coating on G/W/G/W and G/W chips, respectively. (c) Schematic of Raman enhancement mechanism of graphene/ReOxSy-MT chips. (d) Energy level diagrams and charge transfer in the R6G-W18O49/MoS2 complex. (a) and (b) are reprinted with permission from Ref. [16]. Copyright © 2017 American Chemical Society. (c) is reprinted with permission from Ref. [98]. Copyright © 2020 American Chemical Society. (d) is reprinted with permission from Ref. [104]. Copyright © 2019 American Chemical Society.

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Table 1.   Comparison of SERS results based on different substrates.

Materiala)Detection moleculeb)LOD (M)EFWavelength
(nm)		Ref.
MoS2R6G10–7–532[48]
MoS24-MPy–105488[50]
MoS2Py-EtOH–109555[47]
MoS2R6G10–7–532[53]
MoS2R6G–63532[52]
MoS2R6G10–8–532[55]
WS2R6G10–8–532
WS2R6G10–7–532[45]
WS2R6G10–7–532[42]
ReS2R6G10–9–532[46]
RhB10–8–532
CV10–8–532
MB10–9–532
NbS2MeB10–14–633[36]
1T’-MoSe2R6G10–8–532[57]
SnSe2R6G10–12106532[34]
SnS2CuPc10–1050633[33]
WSe2CuPc10–1050633
WSe2CuPc–120532[43]
WTe2R6G10–151010532[58]
MoTe2R6G10–14109–
h-BNNSCuPc-miR-2110–15–655[69]
BPCuPc–<10633[84]
BPRhB10–8106532[80]
BPCV10–5–532[76]
Ti3C2TxR6G10–7106488[91]
MB10–7106633
CV10–7105633
AB10–6103514
r-Ti3C2TxCV10–6106532[87]
Ti3C2TxMB10–6105–
Ti3C2TxR6G10–6107532
Ti3C2TxCV10–8–532[88]
R6G10–8104532
MB10–7–633
Ti3C2R6G10–11108532[90]
Ti2NR6G–1012532[92]
Graphene/WSe2CuPc–77633[16]
MoS2 QD/rGOR6G10–9107532[99]
MB10–8–532
MoS2/
graphene		R6G10–12–532[98]
R6G10–11–532
W18O49/
MoS2		R6G10–10107532[104]
GMFs/
W-MoS2		MB10–10––[100]
Adenosine10–9––
a)Materials: quantum dot MoS2 hybrid with reduced graphene oxide (MoS2 QD/rGO), wrinkled semiconducting 2H-phase MoS2 platform decorated with graphene-microflowers (GMFs/MoS2).
b)Molecules: rhodamine (RhB), rhodamine 6G (R6G), crystal violet (CV), methylene blue (MB), acid blue (AB), copper phthalocyanine (CuPc), pyridine and ethanol (Py-EtOH), and 4-Mercaptopyridine (4-MPy).
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    Received: 28 November 2020 Revised: 28 December 2020 Online: Accepted Manuscript: 19 March 2021Uncorrected proof: 31 March 2021Published: 01 May 2021

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      Article Navigation >  Journal of Semiconductors  > 2021  >  42(5): 051001
      Enqing Zhang, Zhengkun Xing, Dian Wan, Haoran Gao, Yingdong Han, Yisheng Gao, Haofeng Hu, Zhenzhou Cheng, Tiegen Liu. Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene[J]. Journal of Semiconductors, 2021, 42(5): 051001. doi: 10.1088/1674-4926/42/5/051001 E Q Zhang, Z K Xing, D Wan, H R Gao, Y D Han, Y S Gao, H F Hu, Z Z Cheng, T G Liu, Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene[J]. J. Semicond., 2021, 42(5): 051001. doi: 10.1088/1674-4926/42/5/051001.Export: BibTex EndNote
      Citation:
      Enqing Zhang, Zhengkun Xing, Dian Wan, Haoran Gao, Yingdong Han, Yisheng Gao, Haofeng Hu, Zhenzhou Cheng, Tiegen Liu. Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene[J]. Journal of Semiconductors, 2021, 42(5): 051001. doi: 10.1088/1674-4926/42/5/051001

      E Q Zhang, Z K Xing, D Wan, H R Gao, Y D Han, Y S Gao, H F Hu, Z Z Cheng, T G Liu, Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene[J]. J. Semicond., 2021, 42(5): 051001. doi: 10.1088/1674-4926/42/5/051001.
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      Surface-enhanced Raman spectroscopy chips based on two-dimensional materials beyond graphene

      doi: 10.1088/1674-4926/42/5/051001
      • 1.

        School of Precision Instruments and Opto-electronics Engineering, Tianjin University, Tianjin 300072, China

      • 2.

        Key Laboratory of Opto-electronics Information Technology, Ministry of Education, Tianjin 300072, China

      • 3.

        Department of Electrical Engineering, The Hong Kong Polytechnic University, Hong Kong, China

      • 4.

        Department of Chemistry, The University of Tokyo, Tokyo 113-0033, Japan

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      • Author Bio:

        Enqing Zhang is a graduate student in the School of Precision Instrument and Opto-Electronics Engineering, Tianjin University. He received his bachelor’s degree from the College of Electronic Information and Optical Engineering of Nankai University in 2019. His research interests include surface-enhanced Raman spectroscopy

        Haofeng Hu received his B.S., M.S., and, Ph.D. degrees from Nankai University, Tianjin, China, in 2006, 2008, and 2011, respectively. He is currently a professor at Tianjin University, Tianjin. His research interests include polarimetric imaging and spectroscopy

        Zhenzhou Cheng is a professor in the School of Precision Instrument and Opto-Electronics Engineering, Tianjin University. He received his Ph.D. degree from the Chinese University of Hong Kong and then worked at the University of Tokyo as an assistant professor. His research interests include silicon photonics and nanophotonics. He published over 70 SCI papers including Nature Photonics and Nature Communications

      • Corresponding author: haofeng_hu@tju.edu.cn; zhenzhoucheng@tju.edu.cn
      • Received Date: 2020-11-28
      • Revised Date: 2020-12-28
      • Published Date: 2021-05-10

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