Abstract

In this work, we investigated the nonlinear optical properties of monolayer MoS2 and WS2 modulated by defect engineering via chemical treatment. The results demonstrate that the two-photon luminescence (TPL) and two-photon absorption (TPA) coefficient were remarkably improved after the repair of sulfur vacancies for both monolayer MoS2 and WS2. After the chemical treatment, the nonradiative relaxation path dominant in pristine monolayer MoS2 is significantly alleviated, resulting in enhanced TPL. Our work affords an effective way to tailor the nonlinear absorption, luminescence and relaxation properties of sulfur-based two-dimensional metal dichalcogenides by defect engineering.

© 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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    [Crossref] [PubMed]
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  3. C. Sweet, A. Pramanik, S. Jones, and P. C. Ray, “Two-photon fluorescent molybdenum disulfide dots for targeted Prostate cancer imaging in the biological II window,” ACS Omega 2(5), 1826–1835 (2017).
    [Crossref] [PubMed]
  4. K. P. Loh, H. Zhang, W. Z. Chen, and W. Ji, “Templated deposition of MoS2 nanotubules using single source precursor and studies of their optical limiting properties,” J. Phys. Chem. B 110(3), 1235–1239 (2006).
    [Crossref] [PubMed]
  5. E. E. Hoover and J. A. Squier, “Advances in multiphoton microscopy technology,” Nat. Photonics 7(2), 93–101 (2013).
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  6. K. Zagorovsky and W. C. Chan, “Illuminating the deep,” Nat. Mater. 12(4), 285–287 (2013).
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  7. D. A. Fishman, C. M. Cirloganu, S. Webster, L. A. Padilha, M. Monroe, D. J. Hagan, and E. W. Van Stryland, “Sensitive mid-infrared detection in wide-bandgap semiconductors using extreme non-degenerate two-photon absorption,” Nat. Photonics 5(9), 561–565 (2011).
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    [Crossref] [PubMed]
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    [Crossref] [PubMed]
  23. S. Bertolazzi, J. Brivio, and A. Kis, “Stretching and breaking of ultrathin MoS2,” ACS Nano 5(12), 9703–9709 (2011).
    [Crossref] [PubMed]
  24. D. Dumcenco, D. Ovchinnikov, K. Marinov, P. Lazić, M. Gibertini, N. Marzari, O. L. Sanchez, Y. C. Kung, D. Krasnozhon, M. W. Chen, S. Bertolazzi, P. Gillet, A. Fontcuberta i Morral, A. Radenovic, and A. Kis, “Large-area epitaxial monolayer MoS2,” ACS Nano 9(4), 4611–4620 (2015).
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  26. K. Wu, Z. Li, J. Tang, X. Lv, H. Wang, R. Luo, P. Liu, S. Zhang, and S. Yuan, “Controllable defects implantation in MoS2, grown by chemical vapor deposition for photoluminescence enhancement,” Nano Res. 11(8), 4123–4132 (2018).
    [Crossref]
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    [Crossref] [PubMed]
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  29. X. Liu, Q. Guo, and J. Qiu, “Emerging low-dimensional materials for nonlinear optics and ultrafast photonics,” Adv. Mater. 29(14), 1605886 (2017).
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  30. T. L. Atallah, J. Wang, M. Bosch, D. Seo, R. A. Burke, O. Moneer, J. Zhu, M. Theibault, L. E. Brus, J. Hone, and X. Y. Zhu, “Electrostatic screening of charged defects in monolayer MoS2,” J. Phys. Chem. Lett. 8(10), 2148–2152 (2017).
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    [Crossref] [PubMed]
  32. M. Amani, P. Taheri, R. Addou, G. H. Ahn, D. Kiriya, D. H. Lien, J. W. Ager, R. M. Wallace, and A. Javey, “Recombination kinetics and effects of superacid treatment in sulfur and selenium based transition metal dichalcogenides,” Nano Lett. 16(4), 2786–2791 (2016).
    [Crossref] [PubMed]
  33. L. Yuan and L. Huang, “Exciton dynamics and annihilation in WS2 2D semiconductors,” Nanoscale 7(16), 7402–7408 (2015).
    [Crossref] [PubMed]
  34. Z. Ye, T. Cao, K. O’Brien, H. Zhu, X. Yin, Y. Wang, S. G. Louie, and X. Zhang, “Probing excitonic dark states in single-layer tungsten disulphide,” Nature 513(7517), 214–218 (2014).
    [Crossref] [PubMed]
  35. B. Taheri, H. Liu, B. Jassemnejad, D. Appling, R. Powell, and J. Song, “Intensity scan and two photon absorption and nonlinear refraction of C-60 in toluene,” Appl. Phys. Lett. 68(10), 1317–1319 (1996).
    [Crossref]
  36. Y. Li, N. Dong, S. Zhang, X. Zhang, Y. Feng, K. Wang, L. Zhang, and J. Wang, “Giant two-photon absorption in monolayer MoS2,” Laser Photonics Rev. 9(4), 427–434 (2015).
    [Crossref]
  37. N. Dong, Y. Li, S. Zhang, N. McEyoy, R. Gatensby, G. Duesberg, and J. Wang, “Saturation of two-photon absorption in layered transition metal dichalcogenides: Experiment and theory,” ACS Photonics 5(4), 1558–1565 (2018).
    [Crossref]
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    [Crossref] [PubMed]
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    [Crossref] [PubMed]
  40. E. A. Pogna, M. Marsili, D. De Fazio, S. Dal Conte, C. Manzoni, D. Sangalli, D. Yoon, A. Lombardo, A. C. Ferrari, A. Marini, G. Cerullo, and D. Prezzi, “Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2,” ACS Nano 10(1), 1182–1188 (2016).
    [Crossref] [PubMed]
  41. H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, “Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies,” Nat. Mater. 15(1), 48–53 (2016).
    [Crossref] [PubMed]

2018 (4)

X. Zhang, S. Zhang, Y. Xie, J. Huang, L. Wang, Y. Cui, and J. Wang, “Tailoring the nonlinear optical performance of two-dimensional MoS2 nanofilms via defect engineering,” Nanoscale 10(37), 17924–17932 (2018).
[Crossref] [PubMed]

N. Dong, Y. Li, S. Zhang, N. McEyoy, R. Gatensby, G. Duesberg, and J. Wang, “Saturation of two-photon absorption in layered transition metal dichalcogenides: Experiment and theory,” ACS Photonics 5(4), 1558–1565 (2018).
[Crossref]

A. Förster, S. Gemming, and G. Seifert, “Functional thiols as repair and doping agents of defective MoS2 monolayers,” J. Phys. Condens. Matter 30(23), 235302 (2018).
[Crossref] [PubMed]

K. Wu, Z. Li, J. Tang, X. Lv, H. Wang, R. Luo, P. Liu, S. Zhang, and S. Yuan, “Controllable defects implantation in MoS2, grown by chemical vapor deposition for photoluminescence enhancement,” Nano Res. 11(8), 4123–4132 (2018).
[Crossref]

2017 (8)

S. Bettis Homan, V. K. Sangwan, I. Balla, H. Bergeron, E. A. Weiss, and M. C. Hersam, “Ultrafast exciton dissociation and long-lived charge separation in a photovoltaic pentacene-MoS2 van der Waals heterojunction,” Nano Lett. 17(1), 164–169 (2017).
[Crossref] [PubMed]

O. Ajayi, J. Ardelean, G. D. Shepard, J. Wang, A. Antony, T. Taniguchi, K. Watanabe, T. F. Heinz, S. Strauf, X. Y. Zhu, and J. C. Hone, “Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers,” 2D Mater. 4(3), 031011 (2017).
[Crossref]

G. Kime, M. Leontiadou, J. Brent, N. Savjani, P. O’Brien, and D. Binks, “Ultrafast charge dynamics in dispersions of monolayer MoS2 nanosheets,” J. Phys. Chem. C 121(40), 22415–22421 (2017).
[Crossref]

X. Liu, Q. Guo, and J. Qiu, “Emerging low-dimensional materials for nonlinear optics and ultrafast photonics,” Adv. Mater. 29(14), 1605886 (2017).
[Crossref] [PubMed]

T. L. Atallah, J. Wang, M. Bosch, D. Seo, R. A. Burke, O. Moneer, J. Zhu, M. Theibault, L. E. Brus, J. Hone, and X. Y. Zhu, “Electrostatic screening of charged defects in monolayer MoS2,” J. Phys. Chem. Lett. 8(10), 2148–2152 (2017).
[Crossref] [PubMed]

X. Zhang, Q. Liao, S. Liu, Z. Kang, Z. Zhang, J. Du, F. Li, S. Zhang, J. Xiao, B. Liu, Y. Ou, X. Liu, L. Gu, and Y. Zhang, “Poly(4-styrenesulfonate)-induced sulfur vacancy self-healing strategy for monolayer MoS2 homojunction photodiode,” Nat. Commun. 8, 15881 (2017).
[Crossref] [PubMed]

F. Zhou and W. Ji, “Giant three-photon absorption in monolayer MoS2 and its application in near-infrared photodetection,” Laser Photonics Rev. 11(4), 1700021 (2017).
[Crossref]

C. Sweet, A. Pramanik, S. Jones, and P. C. Ray, “Two-photon fluorescent molybdenum disulfide dots for targeted Prostate cancer imaging in the biological II window,” ACS Omega 2(5), 1826–1835 (2017).
[Crossref] [PubMed]

2016 (6)

H. V. Han, A. Y. Lu, L. S. Lu, J. K. Huang, H. Li, C. L. Hsu, Y. C. Lin, M. H. Chiu, K. Suenaga, C. W. Chu, H. C. Kuo, W. H. Chang, L. J. Li, and Y. Shi, “Photoluminescence enhancement and structure repairing of monolayer MoSe2 by hydrohalic acid treatment,” ACS Nano 10(1), 1454–1461 (2016).
[Crossref] [PubMed]

B. Liu, W. Zhao, Z. Ding, I. Verzhbitskiy, L. Li, J. Lu, J. Chen, G. Eda, and K. P. Loh, “Engineering bandgaps of monolayer MoS2 and WS2 on fluoropolymer substrates by electrostatically tuned many-body effects,” Adv. Mater. 28(30), 6457–6464 (2016).
[Crossref] [PubMed]

M. Amani, P. Taheri, R. Addou, G. H. Ahn, D. Kiriya, D. H. Lien, J. W. Ager, R. M. Wallace, and A. Javey, “Recombination kinetics and effects of superacid treatment in sulfur and selenium based transition metal dichalcogenides,” Nano Lett. 16(4), 2786–2791 (2016).
[Crossref] [PubMed]

E. A. Pogna, M. Marsili, D. De Fazio, S. Dal Conte, C. Manzoni, D. Sangalli, D. Yoon, A. Lombardo, A. C. Ferrari, A. Marini, G. Cerullo, and D. Prezzi, “Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2,” ACS Nano 10(1), 1182–1188 (2016).
[Crossref] [PubMed]

H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, “Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies,” Nat. Mater. 15(1), 48–53 (2016).
[Crossref] [PubMed]

M. S. Kim, S. J. Yun, Y. Lee, C. Seo, G. H. Han, K. K. Kim, Y. H. Lee, and J. Kim, “Biexciton emission from edges and grain boundaries of triangular WS2 monolayers,” ACS Nano 10(2), 2399–2405 (2016).
[Crossref] [PubMed]

2015 (7)

Y. Li, N. Dong, S. Zhang, X. Zhang, Y. Feng, K. Wang, L. Zhang, and J. Wang, “Giant two-photon absorption in monolayer MoS2,” Laser Photonics Rev. 9(4), 427–434 (2015).
[Crossref]

M. Amani, D. H. Lien, D. Kiriya, J. Xiao, A. Azcatl, J. Noh, S. R. Madhvapathy, R. Addou, S. Kc, M. Dubey, K. Cho, R. M. Wallace, S. C. Lee, J. H. He, J. W. Ager, X. Zhang, E. Yablonovitch, and A. Javey, “Near-unity photoluminescence quantum yield in MoS2,” Science 350(6264), 1065–1068 (2015).
[Crossref] [PubMed]

D. Dumcenco, D. Ovchinnikov, K. Marinov, P. Lazić, M. Gibertini, N. Marzari, O. L. Sanchez, Y. C. Kung, D. Krasnozhon, M. W. Chen, S. Bertolazzi, P. Gillet, A. Fontcuberta i Morral, A. Radenovic, and A. Kis, “Large-area epitaxial monolayer MoS2,” ACS Nano 9(4), 4611–4620 (2015).
[Crossref] [PubMed]

P. K. Chow, R. B. Jacobs-Gedrim, J. Gao, T. M. Lu, B. Yu, H. Terrones, and N. Koratkar, “Defect-induced photoluminescence in monolayer semiconducting transition metal dichalcogenides,” ACS Nano 9(2), 1520–1527 (2015).
[Crossref] [PubMed]

L. Yuan and L. Huang, “Exciton dynamics and annihilation in WS2 2D semiconductors,” Nanoscale 7(16), 7402–7408 (2015).
[Crossref] [PubMed]

R. Addou, L. Colombo, and R. M. Wallace, “Surface defects on natural MoS2,” ACS Appl. Mater. Interfaces 7(22), 11921–11929 (2015).
[Crossref] [PubMed]

G. Walters, B. R. Sutherland, S. Hoogland, D. Shi, R. Comin, D. P. Sellan, O. M. Bakr, and E. H. Sargent, “Two-photon absorption in organometallic bromide perovskites,” ACS Nano 9(9), 9340–9346 (2015).
[Crossref] [PubMed]

2014 (4)

X. Yin, Z. Ye, D. A. Chenet, Y. Ye, K. O’Brien, J. C. Hone, and X. Zhang, “Edge nonlinear optics on a MoS2 atomic monolayer,” Science 344(6183), 488–490 (2014).
[Crossref] [PubMed]

S. Wang, H. Yu, H. Zhang, A. Wang, M. Zhao, Y. Chen, L. Mei, and J. Wang, “Broadband few-layer MoS2 saturable absorbers,” Adv. Mater. 26(21), 3538–3544 (2014).
[Crossref] [PubMed]

H. Nan, Z. Wang, W. Wang, Z. Liang, Y. Lu, Q. Chen, D. He, P. Tan, F. Miao, X. Wang, J. Wang, and Z. Ni, “Strong photoluminescence enhancement of MoS2 through defect engineering and oxygen bonding,” ACS Nano 8(6), 5738–5745 (2014).
[Crossref] [PubMed]

Z. Ye, T. Cao, K. O’Brien, H. Zhu, X. Yin, Y. Wang, S. G. Louie, and X. Zhang, “Probing excitonic dark states in single-layer tungsten disulphide,” Nature 513(7517), 214–218 (2014).
[Crossref] [PubMed]

2013 (5)

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

H. Qiu, T. Xu, Z. Wang, W. Ren, H. Nan, Z. Ni, Q. Chen, S. Yuan, F. Miao, F. Song, G. Long, Y. Shi, L. Sun, J. Wang, and X. Wang, “Hopping transport through defect-induced localized states in molybdenum disulphide,” Nat. Commun. 4(1), 2642 (2013).
[Crossref] [PubMed]

W. Zhou, X. Zou, S. Najmaei, Z. Liu, Y. Shi, J. Kong, J. Lou, P. M. Ajayan, B. I. Yakobson, and J. C. Idrobo, “Intrinsic structural defects in monolayer molybdenum disulfide,” Nano Lett. 13(6), 2615–2622 (2013).
[Crossref] [PubMed]

E. E. Hoover and J. A. Squier, “Advances in multiphoton microscopy technology,” Nat. Photonics 7(2), 93–101 (2013).
[Crossref] [PubMed]

K. Zagorovsky and W. C. Chan, “Illuminating the deep,” Nat. Mater. 12(4), 285–287 (2013).
[Crossref] [PubMed]

2011 (3)

D. A. Fishman, C. M. Cirloganu, S. Webster, L. A. Padilha, M. Monroe, D. J. Hagan, and E. W. Van Stryland, “Sensitive mid-infrared detection in wide-bandgap semiconductors using extreme non-degenerate two-photon absorption,” Nat. Photonics 5(9), 561–565 (2011).
[Crossref]

A. Hayat, A. Nevet, P. Ginzburg, and M. Orenstein, “Applications of two-photon processes in semiconductor photonic devices: invited review,” Semicond. Sci. Technol. 26(8), 083001 (2011).
[Crossref]

S. Bertolazzi, J. Brivio, and A. Kis, “Stretching and breaking of ultrathin MoS2,” ACS Nano 5(12), 9703–9709 (2011).
[Crossref] [PubMed]

2007 (1)

T. F. Jaramillo, K. P. Jørgensen, J. Bonde, J. H. Nielsen, S. Horch, and I. Chorkendorff, “Identification of active edge sites for electrochemical H2 evolution from MoS2 nanocatalysts,” Science 317(5834), 100–102 (2007).
[Crossref] [PubMed]

2006 (1)

K. P. Loh, H. Zhang, W. Z. Chen, and W. Ji, “Templated deposition of MoS2 nanotubules using single source precursor and studies of their optical limiting properties,” J. Phys. Chem. B 110(3), 1235–1239 (2006).
[Crossref] [PubMed]

2001 (1)

H. Murata, K. Kataoka, and A. Koma, “Scanning tunneling microscope images of locally modulated structures in layered materials, MoS2(0001) and MoSe2(0001), induced by impurity atoms,” Surf. Sci. 478(3), 131–144 (2001).
[Crossref]

1996 (1)

B. Taheri, H. Liu, B. Jassemnejad, D. Appling, R. Powell, and J. Song, “Intensity scan and two photon absorption and nonlinear refraction of C-60 in toluene,” Appl. Phys. Lett. 68(10), 1317–1319 (1996).
[Crossref]

Abild-Pedersen, F.

H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, “Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies,” Nat. Mater. 15(1), 48–53 (2016).
[Crossref] [PubMed]

Addou, R.

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M. S. Kim, S. J. Yun, Y. Lee, C. Seo, G. H. Han, K. K. Kim, Y. H. Lee, and J. Kim, “Biexciton emission from edges and grain boundaries of triangular WS2 monolayers,” ACS Nano 10(2), 2399–2405 (2016).
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B. Liu, W. Zhao, Z. Ding, I. Verzhbitskiy, L. Li, J. Lu, J. Chen, G. Eda, and K. P. Loh, “Engineering bandgaps of monolayer MoS2 and WS2 on fluoropolymer substrates by electrostatically tuned many-body effects,” Adv. Mater. 28(30), 6457–6464 (2016).
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X. Zhang, Q. Liao, S. Liu, Z. Kang, Z. Zhang, J. Du, F. Li, S. Zhang, J. Xiao, B. Liu, Y. Ou, X. Liu, L. Gu, and Y. Zhang, “Poly(4-styrenesulfonate)-induced sulfur vacancy self-healing strategy for monolayer MoS2 homojunction photodiode,” Nat. Commun. 8, 15881 (2017).
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M. Amani, P. Taheri, R. Addou, G. H. Ahn, D. Kiriya, D. H. Lien, J. W. Ager, R. M. Wallace, and A. Javey, “Recombination kinetics and effects of superacid treatment in sulfur and selenium based transition metal dichalcogenides,” Nano Lett. 16(4), 2786–2791 (2016).
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K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

Zhang, Y.

X. Zhang, Q. Liao, S. Liu, Z. Kang, Z. Zhang, J. Du, F. Li, S. Zhang, J. Xiao, B. Liu, Y. Ou, X. Liu, L. Gu, and Y. Zhang, “Poly(4-styrenesulfonate)-induced sulfur vacancy self-healing strategy for monolayer MoS2 homojunction photodiode,” Nat. Commun. 8, 15881 (2017).
[Crossref] [PubMed]

Zhang, Z.

X. Zhang, Q. Liao, S. Liu, Z. Kang, Z. Zhang, J. Du, F. Li, S. Zhang, J. Xiao, B. Liu, Y. Ou, X. Liu, L. Gu, and Y. Zhang, “Poly(4-styrenesulfonate)-induced sulfur vacancy self-healing strategy for monolayer MoS2 homojunction photodiode,” Nat. Commun. 8, 15881 (2017).
[Crossref] [PubMed]

Zhao, J.

H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, “Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies,” Nat. Mater. 15(1), 48–53 (2016).
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Zhao, M.

S. Wang, H. Yu, H. Zhang, A. Wang, M. Zhao, Y. Chen, L. Mei, and J. Wang, “Broadband few-layer MoS2 saturable absorbers,” Adv. Mater. 26(21), 3538–3544 (2014).
[Crossref] [PubMed]

Zhao, Q.

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

Zhao, W.

B. Liu, W. Zhao, Z. Ding, I. Verzhbitskiy, L. Li, J. Lu, J. Chen, G. Eda, and K. P. Loh, “Engineering bandgaps of monolayer MoS2 and WS2 on fluoropolymer substrates by electrostatically tuned many-body effects,” Adv. Mater. 28(30), 6457–6464 (2016).
[Crossref] [PubMed]

Zheng, X.

H. Li, C. Tsai, A. L. Koh, L. Cai, A. W. Contryman, A. H. Fragapane, J. Zhao, H. S. Han, H. C. Manoharan, F. Abild-Pedersen, J. K. Nørskov, and X. Zheng, “Activating and optimizing MoS2 basal planes for hydrogen evolution through the formation of strained sulphur vacancies,” Nat. Mater. 15(1), 48–53 (2016).
[Crossref] [PubMed]

Zhou, F.

F. Zhou and W. Ji, “Giant three-photon absorption in monolayer MoS2 and its application in near-infrared photodetection,” Laser Photonics Rev. 11(4), 1700021 (2017).
[Crossref]

Zhou, W.

W. Zhou, X. Zou, S. Najmaei, Z. Liu, Y. Shi, J. Kong, J. Lou, P. M. Ajayan, B. I. Yakobson, and J. C. Idrobo, “Intrinsic structural defects in monolayer molybdenum disulfide,” Nano Lett. 13(6), 2615–2622 (2013).
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Zhu, H.

Z. Ye, T. Cao, K. O’Brien, H. Zhu, X. Yin, Y. Wang, S. G. Louie, and X. Zhang, “Probing excitonic dark states in single-layer tungsten disulphide,” Nature 513(7517), 214–218 (2014).
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Zhu, J.

T. L. Atallah, J. Wang, M. Bosch, D. Seo, R. A. Burke, O. Moneer, J. Zhu, M. Theibault, L. E. Brus, J. Hone, and X. Y. Zhu, “Electrostatic screening of charged defects in monolayer MoS2,” J. Phys. Chem. Lett. 8(10), 2148–2152 (2017).
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Zhu, X. Y.

T. L. Atallah, J. Wang, M. Bosch, D. Seo, R. A. Burke, O. Moneer, J. Zhu, M. Theibault, L. E. Brus, J. Hone, and X. Y. Zhu, “Electrostatic screening of charged defects in monolayer MoS2,” J. Phys. Chem. Lett. 8(10), 2148–2152 (2017).
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O. Ajayi, J. Ardelean, G. D. Shepard, J. Wang, A. Antony, T. Taniguchi, K. Watanabe, T. F. Heinz, S. Strauf, X. Y. Zhu, and J. C. Hone, “Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers,” 2D Mater. 4(3), 031011 (2017).
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Zou, X.

W. Zhou, X. Zou, S. Najmaei, Z. Liu, Y. Shi, J. Kong, J. Lou, P. M. Ajayan, B. I. Yakobson, and J. C. Idrobo, “Intrinsic structural defects in monolayer molybdenum disulfide,” Nano Lett. 13(6), 2615–2622 (2013).
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2D Mater. (1)

O. Ajayi, J. Ardelean, G. D. Shepard, J. Wang, A. Antony, T. Taniguchi, K. Watanabe, T. F. Heinz, S. Strauf, X. Y. Zhu, and J. C. Hone, “Approaching the intrinsic photoluminescence linewidth in transition metal dichalcogenide monolayers,” 2D Mater. 4(3), 031011 (2017).
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ACS Appl. Mater. Interfaces (1)

R. Addou, L. Colombo, and R. M. Wallace, “Surface defects on natural MoS2,” ACS Appl. Mater. Interfaces 7(22), 11921–11929 (2015).
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ACS Nano (9)

K. Wang, J. Wang, J. Fan, M. Lotya, A. O’Neill, D. Fox, Y. Feng, X. Zhang, B. Jiang, Q. Zhao, H. Zhang, J. N. Coleman, L. Zhang, and W. J. Blau, “Ultrafast saturable absorption of two-dimensional MoS2 nanosheets,” ACS Nano 7(10), 9260–9267 (2013).
[Crossref] [PubMed]

G. Walters, B. R. Sutherland, S. Hoogland, D. Shi, R. Comin, D. P. Sellan, O. M. Bakr, and E. H. Sargent, “Two-photon absorption in organometallic bromide perovskites,” ACS Nano 9(9), 9340–9346 (2015).
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H. V. Han, A. Y. Lu, L. S. Lu, J. K. Huang, H. Li, C. L. Hsu, Y. C. Lin, M. H. Chiu, K. Suenaga, C. W. Chu, H. C. Kuo, W. H. Chang, L. J. Li, and Y. Shi, “Photoluminescence enhancement and structure repairing of monolayer MoSe2 by hydrohalic acid treatment,” ACS Nano 10(1), 1454–1461 (2016).
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H. Nan, Z. Wang, W. Wang, Z. Liang, Y. Lu, Q. Chen, D. He, P. Tan, F. Miao, X. Wang, J. Wang, and Z. Ni, “Strong photoluminescence enhancement of MoS2 through defect engineering and oxygen bonding,” ACS Nano 8(6), 5738–5745 (2014).
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S. Bertolazzi, J. Brivio, and A. Kis, “Stretching and breaking of ultrathin MoS2,” ACS Nano 5(12), 9703–9709 (2011).
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D. Dumcenco, D. Ovchinnikov, K. Marinov, P. Lazić, M. Gibertini, N. Marzari, O. L. Sanchez, Y. C. Kung, D. Krasnozhon, M. W. Chen, S. Bertolazzi, P. Gillet, A. Fontcuberta i Morral, A. Radenovic, and A. Kis, “Large-area epitaxial monolayer MoS2,” ACS Nano 9(4), 4611–4620 (2015).
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P. K. Chow, R. B. Jacobs-Gedrim, J. Gao, T. M. Lu, B. Yu, H. Terrones, and N. Koratkar, “Defect-induced photoluminescence in monolayer semiconducting transition metal dichalcogenides,” ACS Nano 9(2), 1520–1527 (2015).
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M. S. Kim, S. J. Yun, Y. Lee, C. Seo, G. H. Han, K. K. Kim, Y. H. Lee, and J. Kim, “Biexciton emission from edges and grain boundaries of triangular WS2 monolayers,” ACS Nano 10(2), 2399–2405 (2016).
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E. A. Pogna, M. Marsili, D. De Fazio, S. Dal Conte, C. Manzoni, D. Sangalli, D. Yoon, A. Lombardo, A. C. Ferrari, A. Marini, G. Cerullo, and D. Prezzi, “Photo-Induced Bandgap Renormalization Governs the Ultrafast Response of Single-Layer MoS2,” ACS Nano 10(1), 1182–1188 (2016).
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ACS Omega (1)

C. Sweet, A. Pramanik, S. Jones, and P. C. Ray, “Two-photon fluorescent molybdenum disulfide dots for targeted Prostate cancer imaging in the biological II window,” ACS Omega 2(5), 1826–1835 (2017).
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ACS Photonics (1)

N. Dong, Y. Li, S. Zhang, N. McEyoy, R. Gatensby, G. Duesberg, and J. Wang, “Saturation of two-photon absorption in layered transition metal dichalcogenides: Experiment and theory,” ACS Photonics 5(4), 1558–1565 (2018).
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Adv. Mater. (3)

S. Wang, H. Yu, H. Zhang, A. Wang, M. Zhao, Y. Chen, L. Mei, and J. Wang, “Broadband few-layer MoS2 saturable absorbers,” Adv. Mater. 26(21), 3538–3544 (2014).
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X. Liu, Q. Guo, and J. Qiu, “Emerging low-dimensional materials for nonlinear optics and ultrafast photonics,” Adv. Mater. 29(14), 1605886 (2017).
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B. Liu, W. Zhao, Z. Ding, I. Verzhbitskiy, L. Li, J. Lu, J. Chen, G. Eda, and K. P. Loh, “Engineering bandgaps of monolayer MoS2 and WS2 on fluoropolymer substrates by electrostatically tuned many-body effects,” Adv. Mater. 28(30), 6457–6464 (2016).
[Crossref] [PubMed]

Appl. Phys. Lett. (1)

B. Taheri, H. Liu, B. Jassemnejad, D. Appling, R. Powell, and J. Song, “Intensity scan and two photon absorption and nonlinear refraction of C-60 in toluene,” Appl. Phys. Lett. 68(10), 1317–1319 (1996).
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J. Phys. Chem. B (1)

K. P. Loh, H. Zhang, W. Z. Chen, and W. Ji, “Templated deposition of MoS2 nanotubules using single source precursor and studies of their optical limiting properties,” J. Phys. Chem. B 110(3), 1235–1239 (2006).
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J. Phys. Chem. C (1)

G. Kime, M. Leontiadou, J. Brent, N. Savjani, P. O’Brien, and D. Binks, “Ultrafast charge dynamics in dispersions of monolayer MoS2 nanosheets,” J. Phys. Chem. C 121(40), 22415–22421 (2017).
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J. Phys. Chem. Lett. (1)

T. L. Atallah, J. Wang, M. Bosch, D. Seo, R. A. Burke, O. Moneer, J. Zhu, M. Theibault, L. E. Brus, J. Hone, and X. Y. Zhu, “Electrostatic screening of charged defects in monolayer MoS2,” J. Phys. Chem. Lett. 8(10), 2148–2152 (2017).
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J. Phys. Condens. Matter (1)

A. Förster, S. Gemming, and G. Seifert, “Functional thiols as repair and doping agents of defective MoS2 monolayers,” J. Phys. Condens. Matter 30(23), 235302 (2018).
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Laser Photonics Rev. (2)

Y. Li, N. Dong, S. Zhang, X. Zhang, Y. Feng, K. Wang, L. Zhang, and J. Wang, “Giant two-photon absorption in monolayer MoS2,” Laser Photonics Rev. 9(4), 427–434 (2015).
[Crossref]

F. Zhou and W. Ji, “Giant three-photon absorption in monolayer MoS2 and its application in near-infrared photodetection,” Laser Photonics Rev. 11(4), 1700021 (2017).
[Crossref]

Nano Lett. (3)

W. Zhou, X. Zou, S. Najmaei, Z. Liu, Y. Shi, J. Kong, J. Lou, P. M. Ajayan, B. I. Yakobson, and J. C. Idrobo, “Intrinsic structural defects in monolayer molybdenum disulfide,” Nano Lett. 13(6), 2615–2622 (2013).
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M. Amani, P. Taheri, R. Addou, G. H. Ahn, D. Kiriya, D. H. Lien, J. W. Ager, R. M. Wallace, and A. Javey, “Recombination kinetics and effects of superacid treatment in sulfur and selenium based transition metal dichalcogenides,” Nano Lett. 16(4), 2786–2791 (2016).
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S. Bettis Homan, V. K. Sangwan, I. Balla, H. Bergeron, E. A. Weiss, and M. C. Hersam, “Ultrafast exciton dissociation and long-lived charge separation in a photovoltaic pentacene-MoS2 van der Waals heterojunction,” Nano Lett. 17(1), 164–169 (2017).
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Nano Res. (1)

K. Wu, Z. Li, J. Tang, X. Lv, H. Wang, R. Luo, P. Liu, S. Zhang, and S. Yuan, “Controllable defects implantation in MoS2, grown by chemical vapor deposition for photoluminescence enhancement,” Nano Res. 11(8), 4123–4132 (2018).
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Nanoscale (2)

L. Yuan and L. Huang, “Exciton dynamics and annihilation in WS2 2D semiconductors,” Nanoscale 7(16), 7402–7408 (2015).
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X. Zhang, S. Zhang, Y. Xie, J. Huang, L. Wang, Y. Cui, and J. Wang, “Tailoring the nonlinear optical performance of two-dimensional MoS2 nanofilms via defect engineering,” Nanoscale 10(37), 17924–17932 (2018).
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Nat. Commun. (2)

H. Qiu, T. Xu, Z. Wang, W. Ren, H. Nan, Z. Ni, Q. Chen, S. Yuan, F. Miao, F. Song, G. Long, Y. Shi, L. Sun, J. Wang, and X. Wang, “Hopping transport through defect-induced localized states in molybdenum disulphide,” Nat. Commun. 4(1), 2642 (2013).
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X. Zhang, Q. Liao, S. Liu, Z. Kang, Z. Zhang, J. Du, F. Li, S. Zhang, J. Xiao, B. Liu, Y. Ou, X. Liu, L. Gu, and Y. Zhang, “Poly(4-styrenesulfonate)-induced sulfur vacancy self-healing strategy for monolayer MoS2 homojunction photodiode,” Nat. Commun. 8, 15881 (2017).
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Nat. Mater. (2)

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Nat. Photonics (2)

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Nature (1)

Z. Ye, T. Cao, K. O’Brien, H. Zhu, X. Yin, Y. Wang, S. G. Louie, and X. Zhang, “Probing excitonic dark states in single-layer tungsten disulphide,” Nature 513(7517), 214–218 (2014).
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Science (3)

M. Amani, D. H. Lien, D. Kiriya, J. Xiao, A. Azcatl, J. Noh, S. R. Madhvapathy, R. Addou, S. Kc, M. Dubey, K. Cho, R. M. Wallace, S. C. Lee, J. H. He, J. W. Ager, X. Zhang, E. Yablonovitch, and A. Javey, “Near-unity photoluminescence quantum yield in MoS2,” Science 350(6264), 1065–1068 (2015).
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Figures (5)

Fig. 1
Fig. 1 (a) Schematic of the TFSI treatment procedure. AFM topography of (b) the as-transferred and (c) TFSI-treated monolayer MoS2 on quartz substrate. Insets show the height profiles. (d) Absorption, (e) Raman spectra of the as-transferred and TFSI-treated monolayer MoS2. (f) Schematic structures of the monolayer MoS2 with S vacancies. (g) XPS spectra of the C 1s and Mo 3d core levels of monolayer MoS2 before and after the treatment.
Fig. 2
Fig. 2 (a, b) PL spectra for monolayer MoS2 and WS2 before and after the TFSI treatment. Inset in (a) shows the normalized spectra. Inset in (b) shows the stability of PL intensity and peak shift with time. (c,d) TPL spectra for TFSI-treated monolayer MoS2 and WS2 on quartz substrate pumped by 1030-nm fs laser pulses, respectively. Inset shows a quadratic power dependence of the TPL emission.
Fig. 3
Fig. 3 Analysis of the PL spectral shapes for as-transferred and TFSI-treated monolayer MoS2.
Fig. 4
Fig. 4 Nonlinear transmittance versus incident pulse peak irradiance for (a) monolayer MoS2 and (b) monolayer WS2 before and after TFSI treatment. (c) TPA coefficient versus incident pulse intensity for monolayer MoS2 before and after TFSI treatment. (d) The schematic representation of TPA influenced by defect state in monolayer MoS2. (e) Pump–probe results of as-transferred and TFSI-treated MoS2 monolayer. (f) A single plot of the data shows three different temporal regions in monolayer MoS2.
Fig. 5
Fig. 5 Transient absorption spectra for as-transferred (a) and TFSI-treated (b) MoS2 monolayer upon excitation at 365 nm pump pulse (~8 nJ/pulse). (c, d) Decay curves for the two bleaching pits of A and B for the monolayer MoS2 before and after the TFSI treatment, respectively.

Tables (1)

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Table 1 Parameters Obtained from the Fitting of I-scan and Pump−Probe Results.

Equations (3)

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dI( z ) dz =αIβ( I ) I 2 ( z ),
β(I)= β 0 1+ ( I I sat ) 2 ,
g( t )= D 1 exp( t τ 1 )erfc( σ 2 τ 1 t 2 σ )+ D 2 exp( t τ 2 )erfc( σ 2 τ 2 t 2 σ )+ D 3 exp( t τ 3 )erfc( σ 2 τ 3 t 2 σ ),

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