Photonics Research, 2018, 6 (11): 11000991, Published Online: Oct. 11, 2018  

Raman spectroscopy regulation in van der Waals crystals

Author Affiliations
1 State Key Laboratory of Optoelectronic Materials and Technologies, School of Materials, Sun Yat-sen University, Guangzhou 510275, China
2 Key Laboratory of Materials Physics, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, China
3 e-mail: zhengw37@mail.sysu.edu.cn
Figures & Tables

Fig. 1. Typical Raman spectra of MoS2 and WS2 scattering from in-plane (eic axis). (a) Typical Raman-scattering spectrum of MoS2 excited by a 633 nm laser, and a large number of LA(M)-related RS modes are excited. All recoded modes in MoS2 Raman spectroscopy are identified as 179 [A1g(M)+LA(M)], 383 [E2g1(Γ)], 409 [A1g(Γ)], 421 [B2g2+E1u2(ΓA)], 454 [2LA(M)], 465 [A2u(Γ)], 529 [E1g(M)+LA(M)], 572 [2E1g(Γ)], 600 [E2g1(M)+LA(M)], 644 [A1g(M)+LA(M)], 767 (unknown), 785 (unknown), and 824 (unknown) cm1 [14,16]. (b) Typical Raman-scattering spectrum of WS2 excited by a 532 nm laser, and the recoded modes are identified as LA(M) at 175  cm1, E2g1(M)LA(M) at 195  cm1, A1g(M)LA(M) at 233  cm1, 2LA(M)2E2g2(M) at 298  cm1, E1g(M) at 323  cm1, 2LA(M) at 351  cm1, A1g(Γ) at 421  cm1,E2g1(M)+LA(M) at 523  cm1, A1g(M)+LA(M) at 585  cm1, and 4LA(M) at 701  cm1 [9].

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Fig. 2. Normalized optical absorption coefficients of the cross section (kia axis) in (a) MoS2 and (b) WS2 calculated via first principles, where ordinate θ is the angle between the incident light polarized vector ei and the c axis of the crystals. The absorption coefficients of the in-plane area (kic axis) in (c) MoS2 and (d) WS2, where the ordinate φ represents the angle between the incident light ei and the c axis.

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Fig. 3. Improved Raman spectra of (a) MoS2 and (b) WS2 scattering from out-of-plane polarization (eic axis). Compared to Fig. 1, the RS modes here are fully suppressed and the high SNR of the OP mode is highlighted.

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Fig. 4. The cross-sectional angle-dependent polarized (CAP) Raman spectra of (a) MoS2 and (b) WS2, where the ordinate θ is defined as the angle between the incident light polarization ei and the c axis, and the in-plane angle-dependent polarized (IAP) Raman spectra of (c) MoS2 and (d) WS2, where the ordinate φ is defined as the angle between the incident light polarization ei and the a axis.

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Fig. 5. Raman intensities of OP and RS modes extracted from Figs. 4(a) and 4(b) via Lorentzian fitting. (a) and (b) display angle-dependent intensities of A1g OP modes in MoS2 and WS2, respectively, and reveal a similar changing rule in MoS2 and WS2. The red line gives the corresponding fitting results based on the Raman selection rule, i.e., Eq. (1). (c) and (d) show the angle-dependent intensities of resonant scattering modes in layered MoS2 and WS2, respectively. All modes appear with the same θ angle dependence: when θ=(n+1/2)π, the scattering intensity reaches the highest value; while θ=nπ, the value approximates to zero.

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Wei Zheng, Yanming Zhu, Fadi Li, Feng Huang. Raman spectroscopy regulation in van der Waals crystals[J]. Photonics Research, 2018, 6(11): 11000991.

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