Abstract

We report the simultaneous increase of both nonlinear Kerr coefficient n2 and third-order nonlinear susceptibility χ(3) in aluminum zinc oxide (AZO) attained by pump-probe spectroscopy in a frequency degenerate configuration. Our experiments demonstrate a 6-fold enhancement in the third-order nonlinear susceptibility and over one order of magnitude increase in the nonlinear Kerr coefficient, while also determining two distinct operational wavelengths for optimal modulation of either the real or the imaginary part of the complex refractive index. These results, besides providing a broader spectral characterization of the third-order nonlinearity in AZO thin films, also show the fundamental advantages of performing nonlinear optics via degenerate excitation near the ENZ wavelength.

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References

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    [Crossref] [PubMed]
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  39. [Crossref]

2018 (6)

X. Niu, X. Hu, S. Chu, and Q. Gong, “Epsilon-Near-Zero Photonics: A New Platform for Integrated Devices,” Adv. Opt. Mater. 6(10), 1701292 (2018).
[Crossref]

S. Vezzoli, V. Bruno, C. DeVault, T. Roger, V. M. Shalaev, A. Boltasseva, M. Ferrera, M. Clerici, A. Dubietis, and D. Faccio, “Optical Time Reversal from Time-Dependent Epsilon-Near-Zero Media,” Phys. Rev. Lett. 120(4), 043902 (2018).
[Crossref] [PubMed]

M. Z. Alam, S. A. Schulz, J. Upham, I. De Leon, and R. W. Boyd, “Large optical nonlinearity of nanoantennas coupled to an epsilon-near-zero material,” Nat. Photonics 12(2), 79–83 (2018).
[Crossref]

P. Kelly and L. Kuznetsova, “Pulse shaping in the presence of enormous second-order dispersion in Al:ZnO/ZnO epsilon-near-zero metamaterial,” Appl. Phys. B 124(4), 60 (2018).
[Crossref]

M. Ferrera and E. G. Carnemolla, “Ultra-fast transient plasmonics using transparent conductive oxides,” J. Opt. 20(2), 024007 (2018).
[Crossref]

J. Kim, E. G. Carnemolla, C. DeVault, A. M. Shaltout, D. Faccio, V. M. Shalaev, A. V. Kildishev, M. Ferrera, and A. Boltasseva, “Dynamic Control of Nanocavities with Tunable Metal Oxides,” Nano Lett. 18(2), 740–746 (2018).
[Crossref] [PubMed]

2017 (9)

D. G. Baranov, D. A. Zuev, S. I. Lepeshov, O. V. Kotov, A. E. Krasnok, A. B. Evlyukhin, and B. N. Chichkov, “All-dielectric nanophotonics: the quest for better materials and fabrication techniques,” Optica 4(7), 814–825 (2017).
[Crossref]

O. Reshef, E. Giese, M. Zahirul Alam, I. De Leon, J. Upham, and R. W. Boyd, “Beyond the perturbative description of the nonlinear optical response of low-index materials,” Opt. Lett. 42(16), 3225–3228 (2017).
[Crossref] [PubMed]

H. Frostig, E. Small, A. Daniel, P. Oulevey, S. Derevyanko, and Y. Silberberg, “Focusing light by wavefront shaping through disorder and nonlinearity,” Optica 4(9), 1073–1079 (2017).
[Crossref]

J. Guo, H. Zhang, C. Zhang, Z. Li, Y. Sheng, C. Li, X. Bao, B. Man, Y. Jiao, and S. Jiang, “Indium tin oxide nanocrystals as saturable absorbers for passively Q-switched erbium-doped fiber laser,” Opt. Mater. Express 7(10), 3494–3502 (2017).
[Crossref]

I. Liberal and N. Engheta, “Near-zero refractive index photonics,” Nat. Photonics 11(3), 149–158 (2017).
[Crossref]

I. Staude and J. Schilling, “Metamaterial-inspired silicon nanophotonics,” Nat. Photonics 11(5), 274–284 (2017).
[Crossref]

M. R. Shcherbakov, S. Liu, V. V. Zubyuk, A. Vaskin, P. P. Vabishchevich, G. Keeler, T. Pertsch, T. V. Dolgova, I. Staude, I. Brener, and A. A. Fedyanin, “Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces,” Nat. Commun. 8(1), 17 (2017).
[Crossref] [PubMed]

P. Guo, R. P. H. Chang, and R. D. Schaller, “Transient negative optical nonlinearity of indium oxide nanorods arrays in the full-visible range,” ACS Photonics 4(6), 1494–1500 (2017).
[Crossref]

M. Clerici, N. Kinsey, C. DeVault, J. Kim, E. G. Carnemolla, L. Caspani, A. Shaltout, D. Faccio, V. Shalaev, A. Boltasseva, and M. Ferrera, “Controlling hybrid nonlinearities in transparent conducting oxides via two-colour excitation,” Nat. Commun. 8, 15829 (2017).
[Crossref] [PubMed]

2016 (8)

P. Guo, R. D. Schaller, J. B. Ketterson, and R. P. H. Chang, “Ultrafast switching of tunable infrared plasmons in indium tin oxide nanorod arrays with large absolute amplitude,” Nat. Photonics 10(4), 267–273 (2016).
[Crossref]

J. Kim, S. Choudhury, C. DeVault, Y. Zhao, A. V. Kildishev, V. M. Shalaev, A. Alù, and A. Boltasseva, “Controlling the Polarization State of Light with Plasmonic Metal Oxide Metasurface,” ACS Nano 10(10), 9326–9333 (2016).
[Crossref] [PubMed]

S. Liu, M. B. Sinclair, S. Saravi, G. A. Keeler, Y. Yang, J. Reno, G. M. Peake, F. Setzpfandt, I. Staude, T. Pertsch, and I. Brener, “Resonantly Enhanced Second-Harmonic Generation Using III-V Semiconductor All-Dielectric Metasurfaces,” Nano Lett. 16(9), 5426–5432 (2016).
[Crossref] [PubMed]

Z Yue, B. Cai, L. Wang, X. Wang, and M. Gu, “Intrinsically core-shell plasmonic dielectric nanostructures with ultrahigh refractive index,” Sci. Adv. 2, 1501536 (2016).

R. M. Kaipurath, M. Pietrzyk, L. Caspani, T. Roger, M. Clerici, C. Rizza, A. Ciattoni, A. Di Falco, and D. Faccio, “Optically induced metal-to-dielectric transition in Epsilon-Near-Zero metamaterials,” Sci. Rep. 6(1), 27700 (2016).
[Crossref] [PubMed]

A. M. Urbas, Z. Jacob, L. Dal Negro, N. Engheta, A. D. Boardman, P. Egan, A. B. Khanikaev, V. Menon, M. Ferrera, N. Kinsey, C. DeVault, J. Kim, V. M. Shalaev, A. Boltasseva, J. Valentine, C. Pfeiffer, A. Grbic, E. Narimanov, L. Zhu, S. Fan, A. Alù, E. Poutrina, N. M. Litchinitser, M. A. Noginov, K. F. Macdonald, E. Plum, X. Liu, P. F. Nealey, C. R. Kagan, C. B. Murray, D. A. Pawlak, I. I. Smolyaninov, V. N. Smolyaninova, and D. Chanda, “Roadmap on optical metamaterials,” J. Opt. 18(9), 093005 (2016).
[Crossref]

L. Caspani, R. P. M. Kaipurath, M. Clerici, M. Ferrera, T. Roger, J. Kim, N. Kinsey, M. Pietrzyk, A. Di Falco, V. M. Shalaev, A. Boltasseva, and D. Faccio, “Enhanced nonlinear refractive index in ε-near-zero materials,” Phys. Rev. Lett. 116(23), 233901 (2016).
[Crossref] [PubMed]

M. Z. Alam, I. De Leon, and R. W. Boyd, “Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region,” Science 352(6287), 795–797 (2016).
[Crossref] [PubMed]

2015 (4)

2014 (1)

M. Abb, Y. Wang, C. H. de Groot, and O. L. Muskens, “Hotspot-mediated ultrafast nonlinear control of multifrequency plasmonic nanoantennas,” Nat. Commun. 5(1), 4869 (2014).
[Crossref] [PubMed]

2013 (1)

S. B. Raghunathan, H. F. Schouten, W. Ubachs, B. E. Kim, C. H. Gan, and T. D. Visser, “Dynamic beam steering from a subwavelength slit by selective excitation of guided modes,” Phys. Rev. Lett. 111(15), 153901 (2013).
[Crossref] [PubMed]

2012 (1)

G. V. Naik, J. Liu, A. V. Kildishev, V. M. Shalaev, and A. Boltasseva, “Demonstration of Al:ZnO as a plasmonic component for near-infrared metamaterials,” Proc. Natl. Acad. Sci. U.S.A. 109(23), 8834–8838 (2012).
[Crossref] [PubMed]

2011 (1)

M. Abb, P. Albella, J. Aizpurua, and O. L. Muskens, “All-Optical Control of a Single Plasmonic Nanoantenna-ITO Hybrid,” Nano Lett. 11(6), 2457–2463 (2011).
[Crossref] [PubMed]

2002 (1)

H. Kim, J. Horwitz, S. Qadri, and D. Chrisey, “Epitaxial growth of Al-doped ZnO thin films grown by pulsed laser deposition,” Thin Solid Films 420–421, 107–111 (2002).
[Crossref]

2001 (1)

A. V. Singh, R. M. Mehra, N. Buthrath, A. Wakahara, and A. Yoshida, “Highly conductive and transparent aluminum-doped zinc oxide thin films prepared by pulsed laser deposition in oxygen ambient,” J. Appl. Phys. 90(11), 5661–5665 (2001).
[Crossref]

1991 (1)

E. M. Vogel, M. J. Weber, and D. M. Krol, “Nonlinear optical phenomena in glass,” Phys. Chem. Glasses 32(6), 231–254 (1991).

1970 (1)

C. C. Wang, “Empirical Relation between the Linear and the Third-order Nonlinear Optical Susceptibilities,” Phys. Rev. B 2(6), 2045–2048 (1970).
[Crossref]

1964 (1)

R. C. Miller, “Optical second harmonic generation in piezoelectric crystals,” Appl. Phys. Lett. 5(1), 17–19 (1964).
[Crossref]

Abb, M.

M. Abb, Y. Wang, C. H. de Groot, and O. L. Muskens, “Hotspot-mediated ultrafast nonlinear control of multifrequency plasmonic nanoantennas,” Nat. Commun. 5(1), 4869 (2014).
[Crossref] [PubMed]

M. Abb, P. Albella, J. Aizpurua, and O. L. Muskens, “All-Optical Control of a Single Plasmonic Nanoantenna-ITO Hybrid,” Nano Lett. 11(6), 2457–2463 (2011).
[Crossref] [PubMed]

Ahn, J.

G. Kang, J. Yoo, J. Ahn, and K. Kim, “Transparent dielectric nanostructures for efficient light management in optoelectronic applications,” Nano Today 10(1), 22–47 (2015).
[Crossref]

Aizpurua, J.

M. Abb, P. Albella, J. Aizpurua, and O. L. Muskens, “All-Optical Control of a Single Plasmonic Nanoantenna-ITO Hybrid,” Nano Lett. 11(6), 2457–2463 (2011).
[Crossref] [PubMed]

Alam, M. Z.

M. Z. Alam, S. A. Schulz, J. Upham, I. De Leon, and R. W. Boyd, “Large optical nonlinearity of nanoantennas coupled to an epsilon-near-zero material,” Nat. Photonics 12(2), 79–83 (2018).
[Crossref]

M. Z. Alam, I. De Leon, and R. W. Boyd, “Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region,” Science 352(6287), 795–797 (2016).
[Crossref] [PubMed]

Albella, P.

M. Abb, P. Albella, J. Aizpurua, and O. L. Muskens, “All-Optical Control of a Single Plasmonic Nanoantenna-ITO Hybrid,” Nano Lett. 11(6), 2457–2463 (2011).
[Crossref] [PubMed]

Alù, A.

J. Kim, S. Choudhury, C. DeVault, Y. Zhao, A. V. Kildishev, V. M. Shalaev, A. Alù, and A. Boltasseva, “Controlling the Polarization State of Light with Plasmonic Metal Oxide Metasurface,” ACS Nano 10(10), 9326–9333 (2016).
[Crossref] [PubMed]

A. M. Urbas, Z. Jacob, L. Dal Negro, N. Engheta, A. D. Boardman, P. Egan, A. B. Khanikaev, V. Menon, M. Ferrera, N. Kinsey, C. DeVault, J. Kim, V. M. Shalaev, A. Boltasseva, J. Valentine, C. Pfeiffer, A. Grbic, E. Narimanov, L. Zhu, S. Fan, A. Alù, E. Poutrina, N. M. Litchinitser, M. A. Noginov, K. F. Macdonald, E. Plum, X. Liu, P. F. Nealey, C. R. Kagan, C. B. Murray, D. A. Pawlak, I. I. Smolyaninov, V. N. Smolyaninova, and D. Chanda, “Roadmap on optical metamaterials,” J. Opt. 18(9), 093005 (2016).
[Crossref]

Bao, X.

Baranov, D. G.

Boardman, A. D.

A. M. Urbas, Z. Jacob, L. Dal Negro, N. Engheta, A. D. Boardman, P. Egan, A. B. Khanikaev, V. Menon, M. Ferrera, N. Kinsey, C. DeVault, J. Kim, V. M. Shalaev, A. Boltasseva, J. Valentine, C. Pfeiffer, A. Grbic, E. Narimanov, L. Zhu, S. Fan, A. Alù, E. Poutrina, N. M. Litchinitser, M. A. Noginov, K. F. Macdonald, E. Plum, X. Liu, P. F. Nealey, C. R. Kagan, C. B. Murray, D. A. Pawlak, I. I. Smolyaninov, V. N. Smolyaninova, and D. Chanda, “Roadmap on optical metamaterials,” J. Opt. 18(9), 093005 (2016).
[Crossref]

Boltasseva, A.

S. Vezzoli, V. Bruno, C. DeVault, T. Roger, V. M. Shalaev, A. Boltasseva, M. Ferrera, M. Clerici, A. Dubietis, and D. Faccio, “Optical Time Reversal from Time-Dependent Epsilon-Near-Zero Media,” Phys. Rev. Lett. 120(4), 043902 (2018).
[Crossref] [PubMed]

J. Kim, E. G. Carnemolla, C. DeVault, A. M. Shaltout, D. Faccio, V. M. Shalaev, A. V. Kildishev, M. Ferrera, and A. Boltasseva, “Dynamic Control of Nanocavities with Tunable Metal Oxides,” Nano Lett. 18(2), 740–746 (2018).
[Crossref] [PubMed]

M. Clerici, N. Kinsey, C. DeVault, J. Kim, E. G. Carnemolla, L. Caspani, A. Shaltout, D. Faccio, V. Shalaev, A. Boltasseva, and M. Ferrera, “Controlling hybrid nonlinearities in transparent conducting oxides via two-colour excitation,” Nat. Commun. 8, 15829 (2017).
[Crossref] [PubMed]

A. M. Urbas, Z. Jacob, L. Dal Negro, N. Engheta, A. D. Boardman, P. Egan, A. B. Khanikaev, V. Menon, M. Ferrera, N. Kinsey, C. DeVault, J. Kim, V. M. Shalaev, A. Boltasseva, J. Valentine, C. Pfeiffer, A. Grbic, E. Narimanov, L. Zhu, S. Fan, A. Alù, E. Poutrina, N. M. Litchinitser, M. A. Noginov, K. F. Macdonald, E. Plum, X. Liu, P. F. Nealey, C. R. Kagan, C. B. Murray, D. A. Pawlak, I. I. Smolyaninov, V. N. Smolyaninova, and D. Chanda, “Roadmap on optical metamaterials,” J. Opt. 18(9), 093005 (2016).
[Crossref]

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[Crossref]

O. Reshef, E. Giese, M. Zahirul Alam, I. De Leon, J. Upham, and R. W. Boyd, “Beyond the perturbative description of the nonlinear optical response of low-index materials,” Opt. Lett. 42(16), 3225–3228 (2017).
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Faccio, D.

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S. Vezzoli, V. Bruno, C. DeVault, T. Roger, V. M. Shalaev, A. Boltasseva, M. Ferrera, M. Clerici, A. Dubietis, and D. Faccio, “Optical Time Reversal from Time-Dependent Epsilon-Near-Zero Media,” Phys. Rev. Lett. 120(4), 043902 (2018).
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M. Ferrera and E. G. Carnemolla, “Ultra-fast transient plasmonics using transparent conductive oxides,” J. Opt. 20(2), 024007 (2018).
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J. Kim, E. G. Carnemolla, C. DeVault, A. M. Shaltout, D. Faccio, V. M. Shalaev, A. V. Kildishev, M. Ferrera, and A. Boltasseva, “Dynamic Control of Nanocavities with Tunable Metal Oxides,” Nano Lett. 18(2), 740–746 (2018).
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M. Clerici, N. Kinsey, C. DeVault, J. Kim, E. G. Carnemolla, L. Caspani, A. Shaltout, D. Faccio, V. Shalaev, A. Boltasseva, and M. Ferrera, “Controlling hybrid nonlinearities in transparent conducting oxides via two-colour excitation,” Nat. Commun. 8, 15829 (2017).
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P. Guo, R. P. H. Chang, and R. D. Schaller, “Transient negative optical nonlinearity of indium oxide nanorods arrays in the full-visible range,” ACS Photonics 4(6), 1494–1500 (2017).
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P. Guo, R. D. Schaller, J. B. Ketterson, and R. P. H. Chang, “Ultrafast switching of tunable infrared plasmons in indium tin oxide nanorod arrays with large absolute amplitude,” Nat. Photonics 10(4), 267–273 (2016).
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ACS Nano (1)

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Nano Today (1)

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[Crossref]

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Figures (3)

Fig. 1
Fig. 1 (a) Real and imaginary part of the experimentally measured nonlinear susceptibility χ(3) (cross points) compared with the χ(3) trend obtained by the application of the Wang (dashed curves) and Miller (solid curves) relations in the wavelength range 1120 nm - 1450 nm. (b) Real (blue curve) and imaginary (red curve) part of the AZO film permittivity. The black dashed lines indicate the cross-over wavelength, which was λENZ = 1360 nm. (c) Comparison between the nonlinear Kerr coefficient n2r for the degenerate case (λpump = λprobe, magenta line) and for the non-degenerate case (λpump = 787 nm, black line) as a function of λpump in the wavelength range 1120 nm - 1450 nm. The values of the n2r are obtained using the Eq. (2). Black and magenta asterisks indicate non-degenerate and degenerate experimental data, respectively. (d) Comparison between the nonlinear absorption coefficient β2 for the degenerate case (λpump = λprobe, magenta line) and for the non-degenerate case (λpump = 787 nm, black line) as a function of λprobe in the wavelength range 1120 nm - 1450 nm. The values of the n2i are obtained using the Eq. (3) and used in the Eq. (4) to calculate the β2. Black and magenta asterisks indicate non-degenerate and degenerate experimental data, respectively.
Fig. 2
Fig. 2 Sketch of the degenerate pump and probe setup. A Ti:Sapphire laser pumps the optical parametric oscillator, whose signal is split in a high intensity pump and a weak probe, both vertically polarized and incident in the AZO sample with angle of incidence <10°.
Fig. 3
Fig. 3 Variation of the real (a) and imaginary (b) part of the refractive index ∆nr and ∆ni, respectively, as a function of both pump/probe wavelength and the incident pump intensity Ipump.

Equations (8)

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n 2 = 3 2 ε 0 c χ ( 3 ) n r p u m p ( n r + i n i )
n 2 r = 3 2 ε 0 c n r χ r ( 3 ) + n i χ i ( 3 ) D
n 2 i = 3 2 ε 0 c n r χ r ( 3 ) n i χ i ( 3 ) D
β 2 = 4 π n 2 i / λ
χ ( 3 ) ( ω p u m p , ω p r o b e ) = n r p u m p ε 0 c 3 ε N L ( ω p r o b e , I ^ p u m p ) I ^ p u m p
Δ n r , i = n N L r , i n L r , i
n L r = | ε L | + | ε L r | 2 , n N L r = | ε N L | + | ε N L r | 2
n L i = | ε L | | ε L r | 2 , n N L i = | ε N L | | ε N L r | 2

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