Abstract

Two-dimensional semiconductor materials have shown strong non-linear optical properties at the monolayer limit due to the lack of inversion symmetry. These non-linear materials can ideally be combined with top-down planar fabrication methods to offer new optical devices that can be integrated on-chip as compared to large bulk non-linear crystals. Here, we show enhanced second harmonic generation (SHG) from monolayer MoS2 embedded within an all-dielectric Fabry-Perót microcavity that is resonant at the pump wavelength. Power dependency shows a 10-fold increase in second harmonic generation matching theoretical estimate.

© 2016 Optical Society of America

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References

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    [Crossref] [PubMed]

2016 (2)

F. Yi, M. Ren, J. C. Reed, H. Zhu, J. Hou, C. H. Naylor, A. T. C. Johnson, R. Agarwal, and E. Cubukcu, “Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity,” Nano Lett. 16(3), 1631–1636 (2016).
[Crossref] [PubMed]

Z. Lin, X. Liang, M. Loncar, S. G. Johnson, and A. W. Rodriguez, “Cavity-enhanced second-harmonic generation via nonlinear-overlap optimization,” Optica 3(3), 233–238 (2016).
[Crossref]

2015 (4)

G. Wang, X. Marie, I. Gerber, T. Amand, D. Lagarde, L. Bouet, M. Vidal, A. Balocchi, and B. Urbaszek, “Giant Enhancement of the Optical Second-Harmonic Emission of WSe2 monolayers by laser excitation at exciton resonances,” Phys. Rev. Lett. 114, 1–6 (2015).
[Crossref]

D. H. Kim and D. Lim, “Optical second-harmonic generation in few-layer MoSe2,” J. Korean Phys. Soc. 66(5), 816–820 (2015).
[Crossref]

K. L. Seyler, J. R. Schaibley, P. Gong, P. Rivera, A. M. Jones, S. Wu, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Electrical control of second-harmonic generation in a WSe2 monolayer transistor,” Nat. Nanotechnol. 10(5), 407–411 (2015).
[Crossref] [PubMed]

X. Q. Zhang, C. H. Lin, Y. W. Tseng, K. H. Huang, and Y. H. Lee, “Synthesis of lateral heterostructures of semiconducting atomic layers,” Nano Lett. 15(1), 410–415 (2015).
[Crossref] [PubMed]

2014 (2)

C. Janisch, Y. Wang, D. Ma, N. Mehta, A. L. Elías, N. Perea-López, M. Terrones, V. Crespi, and Z. Liu, “Extraordinary Second Harmonic Generation in tungsten disulfide monolayers,” Sci. Rep. 4, 5530 (2014).
[Crossref] [PubMed]

X. Liu, T. Galfsky, Z. Sun, F. Xia, E. Lin, Y.-H. Lee, S. Kéna-Cohen, and V. M. Menon, “Strong light–matter coupling in two-dimensional atomic crystals,” Nat. Photonics 9(1), 30–34 (2014).
[Crossref]

2013 (4)

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Y. Li, Y. Rao, K. F. Mak, Y. You, S. Wang, C. R. Dean, and T. F. Heinz, “Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation,” Nano Lett. 13(7), 3329–3333 (2013).
[Crossref] [PubMed]

N. Kumar, S. Najmaei, Q. Cui, F. Ceballos, P. Ajayan, J. Lou, and H. Zhao, “Second harmonic microscopy of monolayer MoS2,” Phys. Rev. B 87(16), 161403 (2013).
[Crossref]

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8(9), 634–638 (2013).
[Crossref] [PubMed]

2012 (1)

K. F. Mak, K. He, J. Shan, and T. F. Heinz, “Control of valley polarization in monolayer MoS2 by optical helicity,” Nat. Nanotechnol. 7(8), 494–498 (2012).
[Crossref] [PubMed]

2010 (2)

K. F. Mak, C. Lee, J. Hone, J. Shan, and T. F. Heinz, “Atomically thin MoS2: a new direct-gap semiconductor,” Phys. Rev. Lett. 105(13), 136805 (2010).
[Crossref] [PubMed]

A. Splendiani, L. Sun, Y. Zhang, T. Li, J. Kim, C.-Y. Chim, G. Galli, and F. Wang, “Emerging photoluminescence in monolayer MoS2.,” Nano Lett. 10(4), 1271–1275 (2010).
[Crossref] [PubMed]

2005 (1)

K. J. Vahala, “Optical microcavities,” Nature 424, 839–846 (2005).

2004 (1)

J. P. Reithmaier, G. Sek, A. Löffler, C. Hofmann, S. Kuhn, S. Reitzenstein, L. V. Keldysh, V. D. Kulakovskii, T. L. Reinecke, and A. Forchel, “Strong coupling in a single quantum dot-semiconductor microcavity system,” Nature 432(7014), 197–200 (2004).
[Crossref] [PubMed]

1998 (1)

J. Gérard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V. Thierry-Mieg, “Enhanced Spontaneous Emission by Quantum Boxes in a Monolithic Optical Microcavity,” Phys. Rev. Lett. 81(5), 1110–1113 (1998).
[Crossref]

Agarwal, R.

F. Yi, M. Ren, J. C. Reed, H. Zhu, J. Hou, C. H. Naylor, A. T. C. Johnson, R. Agarwal, and E. Cubukcu, “Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity,” Nano Lett. 16(3), 1631–1636 (2016).
[Crossref] [PubMed]

Aivazian, G.

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8(9), 634–638 (2013).
[Crossref] [PubMed]

Ajayan, P.

N. Kumar, S. Najmaei, Q. Cui, F. Ceballos, P. Ajayan, J. Lou, and H. Zhao, “Second harmonic microscopy of monolayer MoS2,” Phys. Rev. B 87(16), 161403 (2013).
[Crossref]

Amand, T.

G. Wang, X. Marie, I. Gerber, T. Amand, D. Lagarde, L. Bouet, M. Vidal, A. Balocchi, and B. Urbaszek, “Giant Enhancement of the Optical Second-Harmonic Emission of WSe2 monolayers by laser excitation at exciton resonances,” Phys. Rev. Lett. 114, 1–6 (2015).
[Crossref]

Balocchi, A.

G. Wang, X. Marie, I. Gerber, T. Amand, D. Lagarde, L. Bouet, M. Vidal, A. Balocchi, and B. Urbaszek, “Giant Enhancement of the Optical Second-Harmonic Emission of WSe2 monolayers by laser excitation at exciton resonances,” Phys. Rev. Lett. 114, 1–6 (2015).
[Crossref]

Bouet, L.

G. Wang, X. Marie, I. Gerber, T. Amand, D. Lagarde, L. Bouet, M. Vidal, A. Balocchi, and B. Urbaszek, “Giant Enhancement of the Optical Second-Harmonic Emission of WSe2 monolayers by laser excitation at exciton resonances,” Phys. Rev. Lett. 114, 1–6 (2015).
[Crossref]

Ceballos, F.

N. Kumar, S. Najmaei, Q. Cui, F. Ceballos, P. Ajayan, J. Lou, and H. Zhao, “Second harmonic microscopy of monolayer MoS2,” Phys. Rev. B 87(16), 161403 (2013).
[Crossref]

Chang, C. S.

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Chang, M. T.

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Chim, C.-Y.

A. Splendiani, L. Sun, Y. Zhang, T. Li, J. Kim, C.-Y. Chim, G. Galli, and F. Wang, “Emerging photoluminescence in monolayer MoS2.,” Nano Lett. 10(4), 1271–1275 (2010).
[Crossref] [PubMed]

Costard, E.

J. Gérard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V. Thierry-Mieg, “Enhanced Spontaneous Emission by Quantum Boxes in a Monolithic Optical Microcavity,” Phys. Rev. Lett. 81(5), 1110–1113 (1998).
[Crossref]

Crespi, V.

C. Janisch, Y. Wang, D. Ma, N. Mehta, A. L. Elías, N. Perea-López, M. Terrones, V. Crespi, and Z. Liu, “Extraordinary Second Harmonic Generation in tungsten disulfide monolayers,” Sci. Rep. 4, 5530 (2014).
[Crossref] [PubMed]

Cubukcu, E.

F. Yi, M. Ren, J. C. Reed, H. Zhu, J. Hou, C. H. Naylor, A. T. C. Johnson, R. Agarwal, and E. Cubukcu, “Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity,” Nano Lett. 16(3), 1631–1636 (2016).
[Crossref] [PubMed]

Cui, Q.

N. Kumar, S. Najmaei, Q. Cui, F. Ceballos, P. Ajayan, J. Lou, and H. Zhao, “Second harmonic microscopy of monolayer MoS2,” Phys. Rev. B 87(16), 161403 (2013).
[Crossref]

Dean, C. R.

Y. Li, Y. Rao, K. F. Mak, Y. You, S. Wang, C. R. Dean, and T. F. Heinz, “Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation,” Nano Lett. 13(7), 3329–3333 (2013).
[Crossref] [PubMed]

Dresselhaus, M.

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Elías, A. L.

C. Janisch, Y. Wang, D. Ma, N. Mehta, A. L. Elías, N. Perea-López, M. Terrones, V. Crespi, and Z. Liu, “Extraordinary Second Harmonic Generation in tungsten disulfide monolayers,” Sci. Rep. 4, 5530 (2014).
[Crossref] [PubMed]

Fang, W.

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Forchel, A.

J. P. Reithmaier, G. Sek, A. Löffler, C. Hofmann, S. Kuhn, S. Reitzenstein, L. V. Keldysh, V. D. Kulakovskii, T. L. Reinecke, and A. Forchel, “Strong coupling in a single quantum dot-semiconductor microcavity system,” Nature 432(7014), 197–200 (2004).
[Crossref] [PubMed]

Galfsky, T.

X. Liu, T. Galfsky, Z. Sun, F. Xia, E. Lin, Y.-H. Lee, S. Kéna-Cohen, and V. M. Menon, “Strong light–matter coupling in two-dimensional atomic crystals,” Nat. Photonics 9(1), 30–34 (2014).
[Crossref]

Galli, G.

A. Splendiani, L. Sun, Y. Zhang, T. Li, J. Kim, C.-Y. Chim, G. Galli, and F. Wang, “Emerging photoluminescence in monolayer MoS2.,” Nano Lett. 10(4), 1271–1275 (2010).
[Crossref] [PubMed]

Gayral, B.

J. Gérard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V. Thierry-Mieg, “Enhanced Spontaneous Emission by Quantum Boxes in a Monolithic Optical Microcavity,” Phys. Rev. Lett. 81(5), 1110–1113 (1998).
[Crossref]

Gérard, J.

J. Gérard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V. Thierry-Mieg, “Enhanced Spontaneous Emission by Quantum Boxes in a Monolithic Optical Microcavity,” Phys. Rev. Lett. 81(5), 1110–1113 (1998).
[Crossref]

Gerber, I.

G. Wang, X. Marie, I. Gerber, T. Amand, D. Lagarde, L. Bouet, M. Vidal, A. Balocchi, and B. Urbaszek, “Giant Enhancement of the Optical Second-Harmonic Emission of WSe2 monolayers by laser excitation at exciton resonances,” Phys. Rev. Lett. 114, 1–6 (2015).
[Crossref]

Ghimire, N. J.

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8(9), 634–638 (2013).
[Crossref] [PubMed]

Gong, P.

K. L. Seyler, J. R. Schaibley, P. Gong, P. Rivera, A. M. Jones, S. Wu, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Electrical control of second-harmonic generation in a WSe2 monolayer transistor,” Nat. Nanotechnol. 10(5), 407–411 (2015).
[Crossref] [PubMed]

He, K.

K. F. Mak, K. He, J. Shan, and T. F. Heinz, “Control of valley polarization in monolayer MoS2 by optical helicity,” Nat. Nanotechnol. 7(8), 494–498 (2012).
[Crossref] [PubMed]

Heinz, T. F.

Y. Li, Y. Rao, K. F. Mak, Y. You, S. Wang, C. R. Dean, and T. F. Heinz, “Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation,” Nano Lett. 13(7), 3329–3333 (2013).
[Crossref] [PubMed]

K. F. Mak, K. He, J. Shan, and T. F. Heinz, “Control of valley polarization in monolayer MoS2 by optical helicity,” Nat. Nanotechnol. 7(8), 494–498 (2012).
[Crossref] [PubMed]

K. F. Mak, C. Lee, J. Hone, J. Shan, and T. F. Heinz, “Atomically thin MoS2: a new direct-gap semiconductor,” Phys. Rev. Lett. 105(13), 136805 (2010).
[Crossref] [PubMed]

Hofmann, C.

J. P. Reithmaier, G. Sek, A. Löffler, C. Hofmann, S. Kuhn, S. Reitzenstein, L. V. Keldysh, V. D. Kulakovskii, T. L. Reinecke, and A. Forchel, “Strong coupling in a single quantum dot-semiconductor microcavity system,” Nature 432(7014), 197–200 (2004).
[Crossref] [PubMed]

Hone, J.

K. F. Mak, C. Lee, J. Hone, J. Shan, and T. F. Heinz, “Atomically thin MoS2: a new direct-gap semiconductor,” Phys. Rev. Lett. 105(13), 136805 (2010).
[Crossref] [PubMed]

Hou, J.

F. Yi, M. Ren, J. C. Reed, H. Zhu, J. Hou, C. H. Naylor, A. T. C. Johnson, R. Agarwal, and E. Cubukcu, “Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity,” Nano Lett. 16(3), 1631–1636 (2016).
[Crossref] [PubMed]

Huang, J. K.

Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
[Crossref] [PubMed]

Huang, K. H.

X. Q. Zhang, C. H. Lin, Y. W. Tseng, K. H. Huang, and Y. H. Lee, “Synthesis of lateral heterostructures of semiconducting atomic layers,” Nano Lett. 15(1), 410–415 (2015).
[Crossref] [PubMed]

Janisch, C.

C. Janisch, Y. Wang, D. Ma, N. Mehta, A. L. Elías, N. Perea-López, M. Terrones, V. Crespi, and Z. Liu, “Extraordinary Second Harmonic Generation in tungsten disulfide monolayers,” Sci. Rep. 4, 5530 (2014).
[Crossref] [PubMed]

Johnson, A. T. C.

F. Yi, M. Ren, J. C. Reed, H. Zhu, J. Hou, C. H. Naylor, A. T. C. Johnson, R. Agarwal, and E. Cubukcu, “Optomechanical Enhancement of Doubly Resonant 2D Optical Nonlinearity,” Nano Lett. 16(3), 1631–1636 (2016).
[Crossref] [PubMed]

Johnson, S. G.

Jones, A. M.

K. L. Seyler, J. R. Schaibley, P. Gong, P. Rivera, A. M. Jones, S. Wu, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Electrical control of second-harmonic generation in a WSe2 monolayer transistor,” Nat. Nanotechnol. 10(5), 407–411 (2015).
[Crossref] [PubMed]

A. M. Jones, H. Yu, N. J. Ghimire, S. Wu, G. Aivazian, J. S. Ross, B. Zhao, J. Yan, D. G. Mandrus, D. Xiao, W. Yao, and X. Xu, “Optical generation of excitonic valley coherence in monolayer WSe2,” Nat. Nanotechnol. 8(9), 634–638 (2013).
[Crossref] [PubMed]

Keldysh, L. V.

J. P. Reithmaier, G. Sek, A. Löffler, C. Hofmann, S. Kuhn, S. Reitzenstein, L. V. Keldysh, V. D. Kulakovskii, T. L. Reinecke, and A. Forchel, “Strong coupling in a single quantum dot-semiconductor microcavity system,” Nature 432(7014), 197–200 (2004).
[Crossref] [PubMed]

Kéna-Cohen, S.

X. Liu, T. Galfsky, Z. Sun, F. Xia, E. Lin, Y.-H. Lee, S. Kéna-Cohen, and V. M. Menon, “Strong light–matter coupling in two-dimensional atomic crystals,” Nat. Photonics 9(1), 30–34 (2014).
[Crossref]

Kim, D. H.

D. H. Kim and D. Lim, “Optical second-harmonic generation in few-layer MoSe2,” J. Korean Phys. Soc. 66(5), 816–820 (2015).
[Crossref]

Kim, J.

A. Splendiani, L. Sun, Y. Zhang, T. Li, J. Kim, C.-Y. Chim, G. Galli, and F. Wang, “Emerging photoluminescence in monolayer MoS2.,” Nano Lett. 10(4), 1271–1275 (2010).
[Crossref] [PubMed]

Kong, J.

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X. Q. Zhang, C. H. Lin, Y. W. Tseng, K. H. Huang, and Y. H. Lee, “Synthesis of lateral heterostructures of semiconducting atomic layers,” Nano Lett. 15(1), 410–415 (2015).
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X. Liu, T. Galfsky, Z. Sun, F. Xia, E. Lin, Y.-H. Lee, S. Kéna-Cohen, and V. M. Menon, “Strong light–matter coupling in two-dimensional atomic crystals,” Nat. Photonics 9(1), 30–34 (2014).
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K. L. Seyler, J. R. Schaibley, P. Gong, P. Rivera, A. M. Jones, S. Wu, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Electrical control of second-harmonic generation in a WSe2 monolayer transistor,” Nat. Nanotechnol. 10(5), 407–411 (2015).
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K. L. Seyler, J. R. Schaibley, P. Gong, P. Rivera, A. M. Jones, S. Wu, J. Yan, D. G. Mandrus, W. Yao, and X. Xu, “Electrical control of second-harmonic generation in a WSe2 monolayer transistor,” Nat. Nanotechnol. 10(5), 407–411 (2015).
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J. Gérard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V. Thierry-Mieg, “Enhanced Spontaneous Emission by Quantum Boxes in a Monolithic Optical Microcavity,” Phys. Rev. Lett. 81(5), 1110–1113 (1998).
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K. F. Mak, K. He, J. Shan, and T. F. Heinz, “Control of valley polarization in monolayer MoS2 by optical helicity,” Nat. Nanotechnol. 7(8), 494–498 (2012).
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Y. H. Lee, L. Yu, H. Wang, W. Fang, X. Ling, Y. Shi, C. T. Lin, J. K. Huang, M. T. Chang, C. S. Chang, M. Dresselhaus, T. Palacios, L. J. Li, and J. Kong, “Synthesis and transfer of single-layer transition metal disulfides on diverse surfaces,” Nano Lett. 13(4), 1852–1857 (2013).
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Y. Li, Y. Rao, K. F. Mak, Y. You, S. Wang, C. R. Dean, and T. F. Heinz, “Probing symmetry properties of few-layer MoS2 and h-BN by optical second-harmonic generation,” Nano Lett. 13(7), 3329–3333 (2013).
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X. Q. Zhang, C. H. Lin, Y. W. Tseng, K. H. Huang, and Y. H. Lee, “Synthesis of lateral heterostructures of semiconducting atomic layers,” Nano Lett. 15(1), 410–415 (2015).
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A. Splendiani, L. Sun, Y. Zhang, T. Li, J. Kim, C.-Y. Chim, G. Galli, and F. Wang, “Emerging photoluminescence in monolayer MoS2.,” Nano Lett. 10(4), 1271–1275 (2010).
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Figures (3)

Fig. 1
Fig. 1

Linear Characterization of DBR-based microcavity with embedded MoS2. (A) Schematic of microcavity with DBR mirrors consisting of interleaving layers of SiNx and SiO2 and SiO2 cavity layers. (B) Brightfield image of MoS2 flakes. (C) Reflectivity of the microcavity showing the cavity resonance at the fundamental wavelength (~800nm).

Fig. 2
Fig. 2

Second Harmonic Generation (SHG) emission from MoS2 at different microcavity fabrication stages. Scanning SH confocal images of (A) as grown, (B) water transferred, and (C) fully embedded MoS2. (D) Power dependence of SH signal from MoS2 sample at the three fabrication stages. Quadratic linear fit with a slope of 2.17 is displayed for the “Full Cavity” power dependence plot.

Fig. 3
Fig. 3

Fully Embedded MoS2 site excited off resonance. (A) SH Confocal image of embedded MoS2 excited off resonance at 876 nm. (B) Reflection plot of cavity resonant at 818 nm with the red arrow indicating the pump wavelength.

Equations (1)

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  η cav = P cav P inc | λ 0 2π = Q 0 Δλ λ 0 2π

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