Skip to main content
SpringerLink
Log in

The effect of the substrate on the Raman and photoluminescence emission of single-layer MoS2

  • Research Article
  • Published:
Nano Research Aims and scope Submit manuscript

Abstract

We quantitatively study the Raman and photoluminescence (PL) emission from single-layer molybdenum disulfide (MoS2) on dielectric (SiO2, hexagonal boron nitride, mica and the polymeric dielectric Gel-Film®) and conducting substrates (Au and few-layer graphene). We find that the substrate can affect the Raman and PL emission in a twofold manner. First, the absorption and emission intensities are strongly modulated by the constructive/destructive interference within the different substrates. Second, the position of the A1g Raman mode peak and the spectral weight between neutral and charged excitons in the PL spectra are modified by the substrate. We attribute this effect to substrate-induced changes in the doping level and in the decay rates of the excitonic transitions. Our results provide a method to quantitatively study the Raman and PL emission from MoS2-based vertical heterostructures and represent the first step in ad hoc tuning the PL emission of 1L MoS2 by selecting the proper substrate.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Similar content being viewed by others

References

  1. Ayari, A.; Cobas, E.; Ogundadegbe, O.; Fuhrer, M. S. Realization and electrical characterization of ultrathin crystals of layered transition-metal dichalcogenides. J. Appl. Phys. 2007, 101, 014507.

    Article  Google Scholar 

  2. Bao, W. Z.; Cai, X. H.; Kim, D.; Sridhara, K.; Fuhrer, M. S. High mobility ambipolar MoS2 field-effect transistors: Substrate and dielectric effects. Appl. Phys. Lett. 2013, 102, 042104.

    Article  Google Scholar 

  3. Buscema, M.; Barkelid, M.; Zwiller, V.; van der Zant, H. S. J.; Steele, G. A.; Castellanos-Gomez, A. Large and tunable photothermoelectric effect in single-layer MoS2. Nano Lett. 2013, 13, 358–363.

    Article  Google Scholar 

  4. Castellanos-Gomez, A.; Poot, M.; Steele, G. A.; van der Zant, H. S. J.; Agraït, N.; Rubio-Bollinger, G. Elastic properties of freely suspended MoS2 nanosheets. Adv. Mater. 2012, 24, 772–775.

    Article  Google Scholar 

  5. Cooper, R. C.; Lee, C.; Marianetti, C. A.; Wei, X. D.; Hone, J.; Kysar, J. W. Nonlinear elastic behavior of two-dimensional molybdenum disulfide. Phys. Rev. B 2013, 87, 035423.

    Article  Google Scholar 

  6. Castellanos-Gomez, A.; van Leeuwen, R.; Buscema, M.; van der Zant, H. S.; Steele, G. A.; Venstra, W. J. Single-layer MoS2 mechanical resonators. Adv. Mater. 2013, 25, 6719–6723.

    Article  Google Scholar 

  7. Splendiani, A.; Sun, L.; Zhang, Y. B.; Li, T. S.; Kim, J.; Chim, C. Y.; Galli, G.; Wang, F. Emerging photoluminescence in monolayer MoS2. Nano Lett. 2010, 10, 1271–1275.

    Article  Google Scholar 

  8. Mak, K. F.; Lee, C.; Hone, J.; Shan, J.; Heinz, T. F. Atomically thin MoS2: A new direct-gap semiconductor. Phys. Rev. Lett. 2010, 105, 136805.

    Article  Google Scholar 

  9. Yin, Z. Y.; Li, H.; Li, H.; Jiang, L.; Shi, Y. M.; Sun, Y. H.; Lu, G.; Zhang, Q.; Chen, X. D.; Zhang, H. Single-layer MoS2 phototransistors. ACS Nano 2012, 6, 74–80.

    Article  Google Scholar 

  10. Lee, H. S.; Min, S. W.; Chang, Y. G.; Park, M. K.; Nam, T.; Kim, H.; Kim, J. H.; Ryu, S.; Im, S. MoS2 nanosheet phototransistors with thickness-modulated optical energy gap. Nano Lett. 2012, 12, 3695–3700.

    Article  Google Scholar 

  11. Mak, K. F.; He, K. L.; Lee, C.; Lee, G. H.; Hone, J.; Heinz, T. F.; Shan, J. Tightly bound trions in monolayer MoS2. Nat. Mater. 2013, 12, 207–211.

    Article  Google Scholar 

  12. Zeng, H. L.; Dai, J. F.; Yao, W.; Xiao, D.; Cui, X. D. Valley polarization in MoS2 monolayers by optical pumping. Nat. Nanotechnol. 2012, 7, 490–493.

    Article  Google Scholar 

  13. Mak, K. F.; He, K. L.; Shan, J.; Heinz, T. F. Control of valley polarization in monolayer MoS2 by optical helicity. Nat. Nanotechnol. 2012, 7, 494–498.

    Article  Google Scholar 

  14. Xiao, D.; Liu, G. B.; Feng, W. X.; Xu, X. D.; Yao, W. Coupled spin and valley physics in monolayers of MoS2 and other group-vi dichalcogenides. Phys. Rev. Lett. 2012, 108, 196802.

    Article  Google Scholar 

  15. Kioseoglou, G.; Hanbicki, A. T.; Currie, M.; Friedman, A. L.; Gunlycke, D.; Jonker, B. T. Valley polarization and intervalley scattering in monolayer MoS2. Appl. Phys. Lett. 2012, 101, 221907.

    Article  Google Scholar 

  16. Sercombe, D.; Schwarz, S.; Pozo-Zamudio, O. D.; Liu, F.; Robinson, B. J.; Chekhovich, E. A.; Tartakovskii, I. I.; Kolosov, O.; Tartakovskii, A. I. Optical investigation of the natural electron doping in thin MoS2 films deposited on dielectric substrates. Sci. Rep. 2013, 3, 3489.

    Article  Google Scholar 

  17. Mao, N. N.; Chen, Y. F.; Liu, D. M.; Zhang, J.; Xie, L. M. Solvatochromic effect on the photoluminescence of MoS2 monolayers. Small 2013, 9, 1312–1315.

    Article  Google Scholar 

  18. Dean, C. R.; Young, A. F.; Meric, I.; Lee, C.; Wang, L.; Sorgenfrei, S.; Watanabe, K.; Taniguchi, T.; Kim., P.; Shepard, K. L. et al. Boron nitride substrates for high-quality graphene electronics. Nat. Nanotechnol. 2010, 5, 722–726.

    Article  Google Scholar 

  19. Britnell, L.; Ribeiro, R. M.; Eckmann, A.; Jalil, R.; Belle, B. D.; Mishchenko, A.; Kim, Y. J.; Gorbachev, R. V.; Georgiou, T.; Morozov, S. V. et al. Strong light-matter interactions in heterostructures of atomically thin films. Science 2013, 340, 1311–1314.

    Article  Google Scholar 

  20. Geim, A. K.; Grigorieva, I. V. Van der waals heterostructures. Nature 2013, 499, 419–425.

    Article  Google Scholar 

  21. Lu, X. M.; Xia, Y. N. Electronic materials: Buckling down for flexible electronics. Nat. Nanotechnol. 2006, 1, 163–164.

    Article  Google Scholar 

  22. Castellanos-Gomez, A.; Wojtaszek, M.; Tombros, N.; Agrait, N.; van Wees, B. J.; Rubio-Bollinger, G. Atomically thin mica flakes and their application as ultrathin insulating substrates for graphene. Small 2011, 7, 2491–2497.

    Google Scholar 

  23. Castellanos-Gomez, A.; Buscema, M.; Molenaar, R.; Singh, V.; Janssen, L.; Zant, H. S. J. v. d.; Steele, G. A. Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping. arXiv:1311.4829 2013.

    Google Scholar 

  24. Castellanos-Gomez, A.; Agrait, N.; Rubio-Bollinger, G. Optical identification of atomically thin dichalcogenide crystals. Appl. Phys. Lett. 2010, 96, 213116.

    Article  Google Scholar 

  25. Late, D. J.; Liu, B.; Matte, H. S. S. R.; Rao, C. N. R.; Dravid, V. P. Rapid characterization of ultrathin layers of chalcogenides on SiO2/Si substrates. Adv. Funct. Mater. 2012, 22, 1894–1905.

    Article  Google Scholar 

  26. Li, H.; Wu, J.; Huang, X.; Lu, G.; Yang, J.; Lu, X.; Xiong, Q.; Zhang, H. Rapid and reliable thickness identification of two-dimensional nanosheets using optical microscopy. ACS Nano 2013, 7, 10344–10353.

    Article  Google Scholar 

  27. Castellanos-Gomez, A.; Barkelid, M.; Goossens, A. M.; Calado, V. E.; van der Zant, H. S. J.; Steele, G. A. Laser-thinning of MoS2: On demand generation of a single-layer semiconductor. Nano Lett. 2012, 12, 3187–3192.

    Article  Google Scholar 

  28. Lee, C.; Yan, H.; Brus, L. E.; Heinz, T. F.; Hone, J.; Ryu, S. Anomalous lattice vibrations of single- and few-layer MoS2. ACS Nano 2010, 4, 2695–2700.

    Article  Google Scholar 

  29. Novoselov, K. S.; Jiang, D.; Schedin, F.; Booth, T. J.; Khotkevich, V. V.; Morozov, S. V.; Geim, A. K. Two-dimensional atomic crystals. Proc. Natl. Acad. Sci. USA 2005, 102, 10451–10453.

    Article  Google Scholar 

  30. Ferrari, A. C.; Meyer, J. C.; Scardaci, V.; Casiraghi, C.; Lazzeri, M.; Mauri, F.; Piscanec, S.; Jiang, D.; Novoselov, K. S.; Roth, S. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 2006, 97, 187401.

    Article  Google Scholar 

  31. van der Zande, A. M.; Huang, P. Y.; Chenet, D. A.; Berkelbach, T. C.; You, Y.; Lee, G. H.; Heinz, T. F.; Reichman, D. R.; Muller, D. A.; Hone, J. C. Grains and grain boundaries in highly crystalline monolayer molybdenum disulphide. Nat. Mater. 2013, 12, 554–561.

    Article  Google Scholar 

  32. Ji, Q. Q.; Zhang, Y. F.; Gao, T.; Zhang, Y.; Ma, D. L.; Liu, M. X.; Chen, Y. B.; Qiao, X. F.; Tan, P. H.; Kan, M. et al. Epitaxial monolayer MoS2 on mica with novel photoluminescence. Nano Lett. 2013, 13, 3870–3877.

    Article  Google Scholar 

  33. Li, S. L.; Miyazaki, H.; Song, H.; Kuramochi, H.; Nakaharai, S.; Tsukagoshi, K. Quantitative raman spectrum and reliable thickness identification for atomic layers on insulating substrates. ACS Nano 2012, 6, 7381–7388.

    Article  Google Scholar 

  34. Casiraghi, C.; Hartschuh, A.; Lidorikis, E.; Qian, H.; Harutyunyan, H.; Gokus, T.; Novoselov, K. S.; Ferrari, A. C. Rayleigh imaging of graphene and graphene layers. Nano Lett. 2007, 7, 2711–2717.

    Article  Google Scholar 

  35. Rice, C.; Young, R. J.; Zan, R.; Bangert, U.; Wolverson, D.; Georgiou, T.; Jalil, R.; Novoselov, K. S. Raman-scattering measurements and first-principles calculations of strain-induced phonon shifts in monolayer MoS2. Phys. Rev. B 2013, 87, 081307.

    Article  Google Scholar 

  36. Chakraborty, B.; Bera, A.; Muthu, D. V. S.; Bhowmick, S.; Waghmare, U. V.; Sood, A. K. Symmetry-dependent phonon renormalization in monolayer MoS2 transistor. Phys. Rev. B 2012, 85, 161403.

    Article  Google Scholar 

  37. Hui, Y. Y.; Liu, X. F.; Jie, W. J.; Chan, N. Y.; Hao, J. H.; Hsu, Y. T.; Li, L. J.; Guo, W. L.; Lau, S. P. Exceptional tunability of band energy in a compressively strained trilayer MoS2 sheet. ACS Nano 2013, 7, 7126–7131.

    Article  Google Scholar 

  38. McKeown, D. A.; Bell, M. I.; Etz, E. S. Vibrational analysis of the dioctahedral mica: 2m∼ 1 muscovite. Am. Mineral. 1999, 84, 1041–1048.

    Google Scholar 

  39. Ghatak, S.; Pal, A. N.; Ghosh, A. Nature of electronic states in atomically thin MoS2 field-effect transistors. ACS Nano 2011, 5, 7707–7712.

    Article  Google Scholar 

  40. Tongay, S.; Zhou, J.; Ataca, C.; Liu, J.; Kang, J. S.; Matthews, T. S.; You, L.; Li, J. B.; Grossman, J. C.; Wu, J. Q. Broad-range modulation of light emission in two-dimensional semiconductors by molecular physisorption gating. Nano Lett. 2013, 13, 2831–2836.

    Article  Google Scholar 

  41. Jones, A. M.; Yu, H. Y.; Ghimire, N. J.; Wu, S. F.; Aivazian, G.; Ross, J. S.; Zhao, B.; Yan, J. Q.; Mandrus, D. G.; Xiao, D. et al. Optical generation of excitonic valley coherence in monolayer WSe2. Nat. Nanotechol. 2013, 8, 634–638.

    Article  Google Scholar 

  42. Limited, R. T. In Polymers in rheology conference: A two-day conference, Shrewsbury, UK, 26th & 27th April, 2001.

    Google Scholar 

  43. Lefebvre, J.; Homma, Y.; Finnie, P. Bright band gap photoluminescence from unprocessed single-walled carbon nanotubes. Phys. Rev. Lett. 2003, 90, 217401.

    Article  Google Scholar 

  44. Avouris, P.; Freitag, M.; Perebeinos, V. Carbon-nanotube optoelectronics. In Carbon nanotubes. Springer: Berlin Heidelberg, 2008; pp 423–454.

    Google Scholar 

  45. Avouris, P.; Freitag, M.; Perebeinos, V. Carbon-nanotube photonics and optoelectronics. Nat. Photon. 2008, 2, 341–350.

    Article  Google Scholar 

  46. Kim, J.; Cote, L. J.; Kim, F.; Huang, J. X. Visualizing graphene based sheets by fluorescence quenching microscopy. J. Am. Chem. Soc. 2010, 132, 260–267.

    Article  Google Scholar 

  47. Gaudreau, L.; Tielrooij, K. J.; Prawiroatmodjo, G. E. D. K.; Osmond, J.; de Abajo, F. J. G.; Koppens, F. H. L. Universal distance-scaling of nonradiative energy transfer to graphene. Nano Lett. 2013, 13, 2030–2035.

    Article  Google Scholar 

  48. Swathi, R. S.; Sebastian, K. L. Long range resonance energy transfer from a dye molecule to graphene has (distance)-4 dependence. J. Chem. Phys. 2009, 130, 086101.

    Article  Google Scholar 

  49. Adarsh, S.; Klaus, K.; Kannan, B. Marker-free on-the-fly fabrication of graphene devices based on fluorescence quenching. Nanotechnology 2010, 21, 015303.

    Article  Google Scholar 

  50. Chen, Z. Y.; Berciaud, S.; Nuckolls, C.; Heinz, T. F.; Brus, L. E. Energy transfer from individual semiconductor nanocrystals to graphene. ACS Nano 2010, 4, 2964–2968.

    Article  Google Scholar 

  51. Ross, J. S.; Wu, S. F.; Yu, H. Y.; Ghimire, N. J.; Jones, A. M.; Aivazian, G.; Yan, J. Q.; Mandrus, D. G.; Xiao, D.; Yao, W. et al. Electrical control of neutral and charged excitons in a monolayer semiconductor. Nat. Commun. 2013, 4, 1474.

    Article  Google Scholar 

  52. Ron, A.; Yoon, H. W.; Sturge, M. D.; Manassen, A.; Cohen, E.; Pfeiffer, L. N. Thermodynamics of free trions in mixed type GaAs/AlAs quantum wells. Solid State Commun. 1996, 97, 741–745.

    Article  Google Scholar 

Download references

Author information

Authors and Affiliations

  1. Kavli Institute of Nanoscience, Delft University of Technology, Lorentzweg 1, 2628 CJ, Delft, The Netherlands

    Michele Buscema, Gary A. Steele, Herre S. J. van der Zant & Andres Castellanos-Gomez

Authors
  1. Michele Buscema
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Gary A. Steele
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Herre S. J. van der Zant
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Andres Castellanos-Gomez
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Michele Buscema, Gary A. Steele or Andres Castellanos-Gomez.

Electronic supplementary material

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Buscema, M., Steele, G.A., van der Zant, H.S.J. et al. The effect of the substrate on the Raman and photoluminescence emission of single-layer MoS2 . Nano Res. 7, 561–571 (2014). https://doi.org/10.1007/s12274-014-0424-0

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12274-014-0424-0

Keywords

Search

Navigation