Abstract

We measure third harmonic generation (THG) as a function of infrared fundamental wavelength for gold nanoparticles over a gold film. An order of magnitude enhancement in THG is found at ~2.5 eV. We ensure that this enhancement is away from plasmonic resonances, so that it may be attributed directly to the ultrafast third-order susceptibility of gold. Using a simple relation between linear and third-order susceptibilities in conjunction with the linear response of gold, we show that the experimental results agree well with the enhancement from interband transitions. This result is interesting for potential applications leveraging telecom-band sources, such as third harmonic deep-tissue imaging with plasmonic nanoparticle markers.

© 2015 Optical Society of America

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References

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    [Crossref]

2015 (4)

P. N. Melentiev, A. E. Afanasiev, A. A. Kuzin, A. V. Zablotskiy, and V. I. Balykin, “Giant enhancement of two photon induced luminescence in metal nanostructure,” Opt. Express 23(9), 11444–11452 (2015).
[Crossref] [PubMed]

V. Knittel, M. P. Fischer, T. de Roo, S. Mecking, A. Leitenstorfer, and D. Brida, “Nonlinear photoluminescence spectrum of single gold nanostructures,” ACS Nano 9(1), 894–900 (2015).
[Crossref] [PubMed]

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

S. Linic, U. Aslam, C. Boerigter, and M. Morabito, “Photochemical transformations on plasmonic metal nanoparticles,” Nat. Mater. 14(6), 567–576 (2015).
[Crossref] [PubMed]

2014 (7)

G. Hajisalem, Q. Min, R. Gelfand, and R. Gordon, “Effect of surface roughness on self-assembled monolayer plasmonic ruler in nonlocal regime,” Opt. Express 22(8), 9604–9610 (2014).
[Crossref]

A. Manjavacas, J. G. Liu, V. Kulkarni, and P. Nordlander, “Plasmon-induced hot carriers in metallic nanoparticles,” ACS Nano 8(8), 7630–7638 (2014).
[Crossref] [PubMed]

B. Metzger, L. Gui, and H. Giessen, “Ultrabroadband chirped pulse second-harmonic spectroscopy: measuring the frequency-dependent second-order response of different metal films,” Opt. Lett. 39(18), 5293–5296 (2014).
[Crossref]

R. W. Boyd, Z. Shi, and I. De Leon, “The third-order nonlinear optical susceptibility of gold,” Opt. Commun. 326, 74–79 (2014).
[Crossref]

G. Hajisalem, M. S. Nezami, and R. Gordon, “Probing the quantum tunneling limit of plasmonic enhancement by third harmonic generation,” Nano Lett. 14(11), 6651–6654 (2014).
[Crossref] [PubMed]

H. Aouani, M. Rahmani, M. Navarro-Cía, and S. A. Maier, “Third-harmonic-upconversion enhancement from a single semiconductor nanoparticle coupled to a plasmonic antenna,” Nat. Nanotechnol. 9(4), 290–294 (2014).
[Crossref] [PubMed]

B. Metzger, M. Hentschel, T. Schumacher, M. Lippitz, X. Ye, C. B. Murray, B. Knabe, K. Buse, and H. Giessen, “Doubling the efficiency of third harmonic generation by positioning ITO nanocrystals into the hot-spot of plasmonic gap-antennas,” Nano Lett. 14(5), 2867–2872 (2014).
[Crossref] [PubMed]

2013 (4)

P. N. Melentiev, A. E. Afanasiev, A. A. Kuzin, A. S. Baturin, and V. I. Balykin, “Subwavelength light localization based on optical nonlinearity and light polarization,” Opt. Lett. 38(13), 2274–2276 (2013).
[Crossref] [PubMed]

P. N. Melentiev, T. V. Konstantinova, A. E. Afanasiev, A. A. Kuzin, A. S. Baturin, A. V. Tausenev, A. V. Konyaschenko, and V. I. Balykin, “Single nano-hole as a new effective nonlinear element for third-harmonic generation,” Laser Phys. Lett. 10(7), 075901 (2013).
[Crossref]

P. N. Melentiev, A. E. Afanasiev, A. A. Kuzin, A. S. Baturin, and V. I. Balykin, “Giant optical nonlinearity of a single plasmonic nanostructure,” Opt. Express 21(12), 13896–13905 (2013).
[Crossref] [PubMed]

A. Marini, M. Conforti, G. Della Valle, H. W. Lee, T. X. Tran, W. Chang, M. A. Schmidt, S. Longhi, P. S. J. Russell, and F. Biancalana, “Ultrafast nonlinear dynamics of surface plasmon polaritons in gold nanowires due to the intrinsic nonlinearity of metals,” New J. Phys. 15(1), 013033 (2013).
[Crossref]

2012 (5)

M. Conforti and G. Della Valle, “Derivation of third-order nonlinear susceptibility of thin metal films as a delayed optical response,” Phys. Rev. B 85(24), 245423 (2012).
[Crossref]

H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett. 12(9), 4997–5002 (2012).
[Crossref] [PubMed]

G. Hajisalem, A. Ahmed, Y. Pang, and R. Gordon, “Plasmon hybridization for enhanced nonlinear optical response,” Opt. Express 20(28), 29923–29930 (2012).
[Crossref] [PubMed]

H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett. 108(21), 217403 (2012).
[Crossref] [PubMed]

B. Metzger, M. Hentschel, M. Lippitz, and H. Giessen, “Third-harmonic spectroscopy and modeling of the nonlinear response of plasmonic nanoantennas,” Opt. Lett. 37(22), 4741–4743 (2012).
[Crossref] [PubMed]

2011 (3)

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett. 11(12), 5519–5523 (2011).
[Crossref] [PubMed]

N. J. Halas, S. Lal, W.-S. Chang, S. Link, and P. Nordlander, “Plasmons in strongly coupled metallic nanostructures,” Chem. Rev. 111(6), 3913–3961 (2011).
[Crossref] [PubMed]

D. Greszik, H. Yang, T. Dreier, and C. Schulz, “Measurement of water film thickness by laser-induced fluorescence and Raman imaging,” Appl. Phys. B 102(1), 123–132 (2011).
[Crossref]

2010 (1)

N. Large, M. Abb, J. Aizpurua, and O. L. Muskens, “Photoconductively loaded plasmonic nanoantenna as building block for ultracompact optical switches,” Nano Lett. 10(5), 1741–1746 (2010).
[Crossref] [PubMed]

2009 (4)

T. Xu, X. Jiao, and S. Blair, “Third-harmonic generation from arrays of sub-wavelength metal apertures,” Opt. Express 17(26), 23582–23588 (2009).
[Crossref] [PubMed]

K. F. MacDonald, Z. L. Sámson, M. I. Stockman, and N. I. Zheludev, “Ultrafast active plasmonics,” Nat. Photonics 3(1), 55–58 (2009).
[Crossref]

S. Palomba and L. Novotny, “Near-field imaging with a localized nonlinear light source,” Nano Lett. 9(11), 3801–3804 (2009).
[Crossref] [PubMed]

S. Palomba, M. Danckwerts, and L. Novotny, “Nonlinear plasmonics with gold nanoparticle antennas,” J. Opt. A, Pure Appl. Opt. 11(11), 114030 (2009).
[Crossref]

2008 (1)

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature 453(7196), 757–760 (2008).
[Crossref] [PubMed]

2007 (3)

N. J. Durr, T. Larson, D. K. Smith, B. A. Korgel, K. Sokolov, and A. Ben-Yakar, “Two-photon luminescence imaging of cancer cells using molecularly targeted gold nanorods,” Nano Lett. 7(4), 941–945 (2007).
[Crossref] [PubMed]

J. Bravo-Abad, A. Rodriguez, P. Bermel, S. G. Johnson, J. D. Joannopoulos, and M. Soljačić, “Enhanced nonlinear optics in photonic-crystal microcavities,” Opt. Express 15(24), 16161–16176 (2007).
[Crossref] [PubMed]

E. Xenogiannopoulou, P. Aloukos, S. Couris, E. Kaminska, A. Piotrowska, and E. Dynowska, “Third-order nonlinear optical properties of thin sputtered gold films,” Opt. Commun. 275(1), 217–222 (2007).
[Crossref]

2006 (2)

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, “Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy,” Nat. Methods 3(1), 47–53 (2006).
[Crossref] [PubMed]

P. G. Etchegoin, E. C. Le Ru, and M. Meyer, “An analytic model for the optical properties of gold,” J. Chem. Phys. 125(16), 164705 (2006).
[Crossref] [PubMed]

2005 (5)

J. T. Krug, E. J. Sánchez, and X. S. Xie, “Fluorescence quenching in tip-enhanced nonlinear optical microscopy,” Appl. Phys. Lett. 86(23), 233102 (2005).
[Crossref]

F. Helmchen and W. Denk, “Deep tissue two-photon microscopy,” Nat. Methods 2(12), 932–940 (2005).
[Crossref] [PubMed]

M. Airola, Y. Liu, and S. Blair, “Second-harmonic generation from an array of sub-wavelength metal apertures,” J. Opt. A, Pure Appl. Opt. 7(2), S118–S123 (2005).
[Crossref]

M. Lippitz, M. A. van Dijk, and M. Orrit, “Third-harmonic generation from single gold nanoparticles,” Nano Lett. 5(4), 799–802 (2005).
[Crossref] [PubMed]

J. Aizpurua, G. W. Bryant, L. J. Richter, F. J. García de Abajo, B. K. Kelley, and T. Mallouk, “Optical properties of coupled metallic nanorods for field-enhanced spectroscopy,” Phys. Rev. B 71(23), 235420 (2005).
[Crossref]

2004 (1)

P. Wang, Y. Lu, L. Tang, J. Zhang, H. Ming, J. Xie, F. H. Ho, H. H. Chang, H. Y. Lin, and D. P. Tsai, “Surface-enhanced optical nonlinearty of a gold film,” Opt. Commun. 229(1), 425–429 (2004).
[Crossref] [PubMed]

2003 (4)

A. Nahata, R. A. Linke, T. Ishi, and K. Ohashi, “Enhanced nonlinear optical conversion from a periodically nanostructured metal film,” Opt. Lett. 28(6), 423–425 (2003).
[Crossref] [PubMed]

W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature 424(6950), 824–830 (2003).
[Crossref] [PubMed]

E. Prodan, C. Radloff, N. J. Halas, and P. Nordlander, “A hybridization model for the plasmon response of complex nanostructures,” Science 302(5644), 419–422 (2003).
[Crossref] [PubMed]

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68(11), 115433 (2003).
[Crossref]

2000 (1)

N. Del Fatti, C. Voisin, M. Achermann, S. Tzortzakis, D. Christofilos, and F. Vallée, “Nonequilibrium electron dynamics in noble metals,” Phys. Rev. B 61(24), 16956–16966 (2000).
[Crossref]

1999 (4)

S. Link and M. A. El-Sayed, “Spectral properties and relaxation dynamics of surface plasmon electronic oscillations in gold and silver nanodots and nanorods,” J. Phys. Chem. B 103(40), 8410–8426 (1999).
[Crossref]

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

E. J. Sánchez, L. Novotny, and X. S. Xie, “Near-field fluorescence microscopy based on two-photon excitation with metal tips,” Phys. Rev. Lett. 82(20), 4014–4017 (1999).
[Crossref]

C. G. Durfee, A. R. Rundquist, S. Backus, C. Herne, M. M. Murnane, and H. C. Kapteyn, “Phase matching of high-order harmonics in hollow waveguides,” Phys. Rev. Lett. 83(11), 2187–2190 (1999).
[Crossref]

1998 (1)

A. Fiore, V. Berger, E. Rosencher, P. Bravetti, and J. Nagle, “Phase matching using an isotropic nonlinear optical material,” Nature 391(6666), 463–466 (1998).
[Crossref]

1994 (1)

C. Sun, F. Vallée, L. H. Acioli, E. P. Ippen, and J. G. Fujimoto, “Femtosecond-tunable measurement of electron thermalization in gold,” Phys. Rev. B Condens. Matter 50(20), 15337–15348 (1994).
[Crossref] [PubMed]

1988 (1)

F. Hache, D. Ricard, C. Flytzanis, and U. Kreibig, “The optical Kerr effect in small metal particles and metal colloids: The case of gold,” Appl. Phys., A Mater. Sci. Process. 47(4), 347–357 (1988).

1987 (1)

1972 (1)

P. B. Johnson and R. W. Christy, “Optical constants of the noble metals,” Phys. Rev. B 6(12), 4370–4379 (1972).
[Crossref]

Abb, M.

N. Large, M. Abb, J. Aizpurua, and O. L. Muskens, “Photoconductively loaded plasmonic nanoantenna as building block for ultracompact optical switches,” Nano Lett. 10(5), 1741–1746 (2010).
[Crossref] [PubMed]

Achermann, M.

N. Del Fatti, C. Voisin, M. Achermann, S. Tzortzakis, D. Christofilos, and F. Vallée, “Nonequilibrium electron dynamics in noble metals,” Phys. Rev. B 61(24), 16956–16966 (2000).
[Crossref]

Acioli, L. H.

C. Sun, F. Vallée, L. H. Acioli, E. P. Ippen, and J. G. Fujimoto, “Femtosecond-tunable measurement of electron thermalization in gold,” Phys. Rev. B Condens. Matter 50(20), 15337–15348 (1994).
[Crossref] [PubMed]

Afanasiev, A. E.

Ahmed, A.

Airola, M.

M. Airola, Y. Liu, and S. Blair, “Second-harmonic generation from an array of sub-wavelength metal apertures,” J. Opt. A, Pure Appl. Opt. 7(2), S118–S123 (2005).
[Crossref]

Aizpurua, J.

N. Large, M. Abb, J. Aizpurua, and O. L. Muskens, “Photoconductively loaded plasmonic nanoantenna as building block for ultracompact optical switches,” Nano Lett. 10(5), 1741–1746 (2010).
[Crossref] [PubMed]

J. Aizpurua, G. W. Bryant, L. J. Richter, F. J. García de Abajo, B. K. Kelley, and T. Mallouk, “Optical properties of coupled metallic nanorods for field-enhanced spectroscopy,” Phys. Rev. B 71(23), 235420 (2005).
[Crossref]

Aloukos, P.

E. Xenogiannopoulou, P. Aloukos, S. Couris, E. Kaminska, A. Piotrowska, and E. Dynowska, “Third-order nonlinear optical properties of thin sputtered gold films,” Opt. Commun. 275(1), 217–222 (2007).
[Crossref]

Aouani, H.

H. Aouani, M. Rahmani, M. Navarro-Cía, and S. A. Maier, “Third-harmonic-upconversion enhancement from a single semiconductor nanoparticle coupled to a plasmonic antenna,” Nat. Nanotechnol. 9(4), 290–294 (2014).
[Crossref] [PubMed]

H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett. 12(9), 4997–5002 (2012).
[Crossref] [PubMed]

Aslam, U.

S. Linic, U. Aslam, C. Boerigter, and M. Morabito, “Photochemical transformations on plasmonic metal nanoparticles,” Nat. Mater. 14(6), 567–576 (2015).
[Crossref] [PubMed]

Ayala-Orozco, C.

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett. 11(12), 5519–5523 (2011).
[Crossref] [PubMed]

Backus, S.

C. G. Durfee, A. R. Rundquist, S. Backus, C. Herne, M. M. Murnane, and H. C. Kapteyn, “Phase matching of high-order harmonics in hollow waveguides,” Phys. Rev. Lett. 83(11), 2187–2190 (1999).
[Crossref]

Baker, L. A.

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

Balykin, V. I.

Barnes, W. L.

W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature 424(6950), 824–830 (2003).
[Crossref] [PubMed]

Baturin, A. S.

Beaurepaire, E.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, “Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy,” Nat. Methods 3(1), 47–53 (2006).
[Crossref] [PubMed]

Ben-Yakar, A.

N. J. Durr, T. Larson, D. K. Smith, B. A. Korgel, K. Sokolov, and A. Ben-Yakar, “Two-photon luminescence imaging of cancer cells using molecularly targeted gold nanorods,” Nano Lett. 7(4), 941–945 (2007).
[Crossref] [PubMed]

Berger, V.

A. Fiore, V. Berger, E. Rosencher, P. Bravetti, and J. Nagle, “Phase matching using an isotropic nonlinear optical material,” Nature 391(6666), 463–466 (1998).
[Crossref]

Bermel, P.

Beversluis, M. R.

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68(11), 115433 (2003).
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Biancalana, F.

A. Marini, M. Conforti, G. Della Valle, H. W. Lee, T. X. Tran, W. Chang, M. A. Schmidt, S. Longhi, P. S. J. Russell, and F. Biancalana, “Ultrafast nonlinear dynamics of surface plasmon polaritons in gold nanowires due to the intrinsic nonlinearity of metals,” New J. Phys. 15(1), 013033 (2013).
[Crossref]

Blair, S.

T. Xu, X. Jiao, and S. Blair, “Third-harmonic generation from arrays of sub-wavelength metal apertures,” Opt. Express 17(26), 23582–23588 (2009).
[Crossref] [PubMed]

M. Airola, Y. Liu, and S. Blair, “Second-harmonic generation from an array of sub-wavelength metal apertures,” J. Opt. A, Pure Appl. Opt. 7(2), S118–S123 (2005).
[Crossref]

Boerigter, C.

S. Linic, U. Aslam, C. Boerigter, and M. Morabito, “Photochemical transformations on plasmonic metal nanoparticles,” Nat. Mater. 14(6), 567–576 (2015).
[Crossref] [PubMed]

Bouhelier, A.

M. R. Beversluis, A. Bouhelier, and L. Novotny, “Continuum generation from single gold nanostructures through near-field mediated intraband transitions,” Phys. Rev. B 68(11), 115433 (2003).
[Crossref]

Boyd, R. W.

R. W. Boyd, Z. Shi, and I. De Leon, “The third-order nonlinear optical susceptibility of gold,” Opt. Commun. 326, 74–79 (2014).
[Crossref]

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

Bravetti, P.

A. Fiore, V. Berger, E. Rosencher, P. Bravetti, and J. Nagle, “Phase matching using an isotropic nonlinear optical material,” Nature 391(6666), 463–466 (1998).
[Crossref]

Bravo-Abad, J.

Brida, D.

V. Knittel, M. P. Fischer, T. de Roo, S. Mecking, A. Leitenstorfer, and D. Brida, “Nonlinear photoluminescence spectrum of single gold nanostructures,” ACS Nano 9(1), 894–900 (2015).
[Crossref] [PubMed]

Bryant, G. W.

J. Aizpurua, G. W. Bryant, L. J. Richter, F. J. García de Abajo, B. K. Kelley, and T. Mallouk, “Optical properties of coupled metallic nanorods for field-enhanced spectroscopy,” Phys. Rev. B 71(23), 235420 (2005).
[Crossref]

Buse, K.

B. Metzger, M. Hentschel, T. Schumacher, M. Lippitz, X. Ye, C. B. Murray, B. Knabe, K. Buse, and H. Giessen, “Doubling the efficiency of third harmonic generation by positioning ITO nanocrystals into the hot-spot of plasmonic gap-antennas,” Nano Lett. 14(5), 2867–2872 (2014).
[Crossref] [PubMed]

Campbell, J. K.

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

Chang, H. H.

P. Wang, Y. Lu, L. Tang, J. Zhang, H. Ming, J. Xie, F. H. Ho, H. H. Chang, H. Y. Lin, and D. P. Tsai, “Surface-enhanced optical nonlinearty of a gold film,” Opt. Commun. 229(1), 425–429 (2004).
[Crossref] [PubMed]

Chang, W.

A. Marini, M. Conforti, G. Della Valle, H. W. Lee, T. X. Tran, W. Chang, M. A. Schmidt, S. Longhi, P. S. J. Russell, and F. Biancalana, “Ultrafast nonlinear dynamics of surface plasmon polaritons in gold nanowires due to the intrinsic nonlinearity of metals,” New J. Phys. 15(1), 013033 (2013).
[Crossref]

Chang, W.-S.

N. J. Halas, S. Lal, W.-S. Chang, S. Link, and P. Nordlander, “Plasmons in strongly coupled metallic nanostructures,” Chem. Rev. 111(6), 3913–3961 (2011).
[Crossref] [PubMed]

Christofilos, D.

N. Del Fatti, C. Voisin, M. Achermann, S. Tzortzakis, D. Christofilos, and F. Vallée, “Nonequilibrium electron dynamics in noble metals,” Phys. Rev. B 61(24), 16956–16966 (2000).
[Crossref]

Christy, R. W.

P. B. Johnson and R. W. Christy, “Optical constants of the noble metals,” Phys. Rev. B 6(12), 4370–4379 (1972).
[Crossref]

Combettes, L.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, “Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy,” Nat. Methods 3(1), 47–53 (2006).
[Crossref] [PubMed]

Conforti, M.

A. Marini, M. Conforti, G. Della Valle, H. W. Lee, T. X. Tran, W. Chang, M. A. Schmidt, S. Longhi, P. S. J. Russell, and F. Biancalana, “Ultrafast nonlinear dynamics of surface plasmon polaritons in gold nanowires due to the intrinsic nonlinearity of metals,” New J. Phys. 15(1), 013033 (2013).
[Crossref]

M. Conforti and G. Della Valle, “Derivation of third-order nonlinear susceptibility of thin metal films as a delayed optical response,” Phys. Rev. B 85(24), 245423 (2012).
[Crossref]

Couris, S.

E. Xenogiannopoulou, P. Aloukos, S. Couris, E. Kaminska, A. Piotrowska, and E. Dynowska, “Third-order nonlinear optical properties of thin sputtered gold films,” Opt. Commun. 275(1), 217–222 (2007).
[Crossref]

Crooks, R. M.

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

Danckwerts, M.

S. Palomba, M. Danckwerts, and L. Novotny, “Nonlinear plasmonics with gold nanoparticle antennas,” J. Opt. A, Pure Appl. Opt. 11(11), 114030 (2009).
[Crossref]

De Leon, I.

R. W. Boyd, Z. Shi, and I. De Leon, “The third-order nonlinear optical susceptibility of gold,” Opt. Commun. 326, 74–79 (2014).
[Crossref]

de Roo, T.

V. Knittel, M. P. Fischer, T. de Roo, S. Mecking, A. Leitenstorfer, and D. Brida, “Nonlinear photoluminescence spectrum of single gold nanostructures,” ACS Nano 9(1), 894–900 (2015).
[Crossref] [PubMed]

Débarre, D.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, “Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy,” Nat. Methods 3(1), 47–53 (2006).
[Crossref] [PubMed]

Del Fatti, N.

N. Del Fatti, C. Voisin, M. Achermann, S. Tzortzakis, D. Christofilos, and F. Vallée, “Nonequilibrium electron dynamics in noble metals,” Phys. Rev. B 61(24), 16956–16966 (2000).
[Crossref]

Della Valle, G.

A. Marini, M. Conforti, G. Della Valle, H. W. Lee, T. X. Tran, W. Chang, M. A. Schmidt, S. Longhi, P. S. J. Russell, and F. Biancalana, “Ultrafast nonlinear dynamics of surface plasmon polaritons in gold nanowires due to the intrinsic nonlinearity of metals,” New J. Phys. 15(1), 013033 (2013).
[Crossref]

M. Conforti and G. Della Valle, “Derivation of third-order nonlinear susceptibility of thin metal films as a delayed optical response,” Phys. Rev. B 85(24), 245423 (2012).
[Crossref]

Denk, W.

F. Helmchen and W. Denk, “Deep tissue two-photon microscopy,” Nat. Methods 2(12), 932–940 (2005).
[Crossref] [PubMed]

Dereux, A.

W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature 424(6950), 824–830 (2003).
[Crossref] [PubMed]

Dreier, T.

D. Greszik, H. Yang, T. Dreier, and C. Schulz, “Measurement of water film thickness by laser-induced fluorescence and Raman imaging,” Appl. Phys. B 102(1), 123–132 (2011).
[Crossref]

Durfee, C. G.

C. G. Durfee, A. R. Rundquist, S. Backus, C. Herne, M. M. Murnane, and H. C. Kapteyn, “Phase matching of high-order harmonics in hollow waveguides,” Phys. Rev. Lett. 83(11), 2187–2190 (1999).
[Crossref]

Durr, N. J.

N. J. Durr, T. Larson, D. K. Smith, B. A. Korgel, K. Sokolov, and A. Ben-Yakar, “Two-photon luminescence imaging of cancer cells using molecularly targeted gold nanorods,” Nano Lett. 7(4), 941–945 (2007).
[Crossref] [PubMed]

Dynowska, E.

E. Xenogiannopoulou, P. Aloukos, S. Couris, E. Kaminska, A. Piotrowska, and E. Dynowska, “Third-order nonlinear optical properties of thin sputtered gold films,” Opt. Commun. 275(1), 217–222 (2007).
[Crossref]

Ebbesen, T. W.

W. L. Barnes, A. Dereux, and T. W. Ebbesen, “Surface plasmon subwavelength optics,” Nature 424(6950), 824–830 (2003).
[Crossref] [PubMed]

El-Sayed, M. A.

S. Link and M. A. El-Sayed, “Spectral properties and relaxation dynamics of surface plasmon electronic oscillations in gold and silver nanodots and nanorods,” J. Phys. Chem. B 103(40), 8410–8426 (1999).
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Etchegoin, P. G.

P. G. Etchegoin, E. C. Le Ru, and M. Meyer, “An analytic model for the optical properties of gold,” J. Chem. Phys. 125(16), 164705 (2006).
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Fabre, A.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, T. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, “Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy,” Nat. Methods 3(1), 47–53 (2006).
[Crossref] [PubMed]

Fiore, A.

A. Fiore, V. Berger, E. Rosencher, P. Bravetti, and J. Nagle, “Phase matching using an isotropic nonlinear optical material,” Nature 391(6666), 463–466 (1998).
[Crossref]

Fischer, M. P.

V. Knittel, M. P. Fischer, T. de Roo, S. Mecking, A. Leitenstorfer, and D. Brida, “Nonlinear photoluminescence spectrum of single gold nanostructures,” ACS Nano 9(1), 894–900 (2015).
[Crossref] [PubMed]

Floess, D.

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

Flytzanis, C.

F. Hache, D. Ricard, C. Flytzanis, and U. Kreibig, “The optical Kerr effect in small metal particles and metal colloids: The case of gold,” Appl. Phys., A Mater. Sci. Process. 47(4), 347–357 (1988).

Fuchs, J.

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

Fujimoto, J. G.

C. Sun, F. Vallée, L. H. Acioli, E. P. Ippen, and J. G. Fujimoto, “Femtosecond-tunable measurement of electron thermalization in gold,” Phys. Rev. B Condens. Matter 50(20), 15337–15348 (1994).
[Crossref] [PubMed]

García de Abajo, F. J.

J. Aizpurua, G. W. Bryant, L. J. Richter, F. J. García de Abajo, B. K. Kelley, and T. Mallouk, “Optical properties of coupled metallic nanorods for field-enhanced spectroscopy,” Phys. Rev. B 71(23), 235420 (2005).
[Crossref]

Gelfand, R.

George, M.

D. D. Smith, Y. Yoon, R. W. Boyd, J. K. Campbell, L. A. Baker, R. M. Crooks, and M. George, “Z-scan measurement of the nonlinear absorption of a thin gold film,” J. Appl. Phys. 86(11), 6200–6205 (1999).
[Crossref]

Giessen, H.

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

B. Metzger, L. Gui, and H. Giessen, “Ultrabroadband chirped pulse second-harmonic spectroscopy: measuring the frequency-dependent second-order response of different metal films,” Opt. Lett. 39(18), 5293–5296 (2014).
[Crossref]

B. Metzger, M. Hentschel, T. Schumacher, M. Lippitz, X. Ye, C. B. Murray, B. Knabe, K. Buse, and H. Giessen, “Doubling the efficiency of third harmonic generation by positioning ITO nanocrystals into the hot-spot of plasmonic gap-antennas,” Nano Lett. 14(5), 2867–2872 (2014).
[Crossref] [PubMed]

B. Metzger, M. Hentschel, M. Lippitz, and H. Giessen, “Third-harmonic spectroscopy and modeling of the nonlinear response of plasmonic nanoantennas,” Opt. Lett. 37(22), 4741–4743 (2012).
[Crossref] [PubMed]

Gordon, R.

Grady, N. K.

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett. 11(12), 5519–5523 (2011).
[Crossref] [PubMed]

Greszik, D.

D. Greszik, H. Yang, T. Dreier, and C. Schulz, “Measurement of water film thickness by laser-induced fluorescence and Raman imaging,” Appl. Phys. B 102(1), 123–132 (2011).
[Crossref]

Gui, L.

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

B. Metzger, L. Gui, and H. Giessen, “Ultrabroadband chirped pulse second-harmonic spectroscopy: measuring the frequency-dependent second-order response of different metal films,” Opt. Lett. 39(18), 5293–5296 (2014).
[Crossref]

Hache, F.

F. Hache, D. Ricard, C. Flytzanis, and U. Kreibig, “The optical Kerr effect in small metal particles and metal colloids: The case of gold,” Appl. Phys., A Mater. Sci. Process. 47(4), 347–357 (1988).

Hajisalem, G.

Halas, N. J.

N. J. Halas, S. Lal, W.-S. Chang, S. Link, and P. Nordlander, “Plasmons in strongly coupled metallic nanostructures,” Chem. Rev. 111(6), 3913–3961 (2011).
[Crossref] [PubMed]

Y. Zhang, N. K. Grady, C. Ayala-Orozco, and N. J. Halas, “Three-dimensional nanostructures as highly efficient generators of second harmonic light,” Nano Lett. 11(12), 5519–5523 (2011).
[Crossref] [PubMed]

E. Prodan, C. Radloff, N. J. Halas, and P. Nordlander, “A hybridization model for the plasmon response of complex nanostructures,” Science 302(5644), 419–422 (2003).
[Crossref] [PubMed]

Harutyunyan, H.

H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett. 108(21), 217403 (2012).
[Crossref] [PubMed]

Helmchen, F.

F. Helmchen and W. Denk, “Deep tissue two-photon microscopy,” Nat. Methods 2(12), 932–940 (2005).
[Crossref] [PubMed]

Hentschel, M.

B. Metzger, L. Gui, J. Fuchs, D. Floess, M. Hentschel, and H. Giessen, “Strong enhancement of second harmonic emission by plasmonic resonances at the second harmonic wavelength,” Nano Lett. 15(6), 3917–3922 (2015).
[Crossref] [PubMed]

B. Metzger, M. Hentschel, T. Schumacher, M. Lippitz, X. Ye, C. B. Murray, B. Knabe, K. Buse, and H. Giessen, “Doubling the efficiency of third harmonic generation by positioning ITO nanocrystals into the hot-spot of plasmonic gap-antennas,” Nano Lett. 14(5), 2867–2872 (2014).
[Crossref] [PubMed]

B. Metzger, M. Hentschel, M. Lippitz, and H. Giessen, “Third-harmonic spectroscopy and modeling of the nonlinear response of plasmonic nanoantennas,” Opt. Lett. 37(22), 4741–4743 (2012).
[Crossref] [PubMed]

Herne, C.

C. G. Durfee, A. R. Rundquist, S. Backus, C. Herne, M. M. Murnane, and H. C. Kapteyn, “Phase matching of high-order harmonics in hollow waveguides,” Phys. Rev. Lett. 83(11), 2187–2190 (1999).
[Crossref]

Ho, F. H.

P. Wang, Y. Lu, L. Tang, J. Zhang, H. Ming, J. Xie, F. H. Ho, H. H. Chang, H. Y. Lin, and D. P. Tsai, “Surface-enhanced optical nonlinearty of a gold film,” Opt. Commun. 229(1), 425–429 (2004).
[Crossref] [PubMed]

Hong, M.

H. Aouani, M. Navarro-Cia, M. Rahmani, T. P. H. Sidiropoulos, M. Hong, R. F. Oulton, and S. A. Maier, “Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light,” Nano Lett. 12(9), 4997–5002 (2012).
[Crossref] [PubMed]

Ippen, E. P.

C. Sun, F. Vallée, L. H. Acioli, E. P. Ippen, and J. G. Fujimoto, “Femtosecond-tunable measurement of electron thermalization in gold,” Phys. Rev. B Condens. Matter 50(20), 15337–15348 (1994).
[Crossref] [PubMed]

Ishi, T.

Jiao, X.

Jin, J.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature 453(7196), 757–760 (2008).
[Crossref] [PubMed]

Joannopoulos, J. D.

Johnson, P. B.

P. B. Johnson and R. W. Christy, “Optical constants of the noble metals,” Phys. Rev. B 6(12), 4370–4379 (1972).
[Crossref]

Johnson, S. G.

Kaminska, E.

E. Xenogiannopoulou, P. Aloukos, S. Couris, E. Kaminska, A. Piotrowska, and E. Dynowska, “Third-order nonlinear optical properties of thin sputtered gold films,” Opt. Commun. 275(1), 217–222 (2007).
[Crossref]

Kapteyn, H. C.

C. G. Durfee, A. R. Rundquist, S. Backus, C. Herne, M. M. Murnane, and H. C. Kapteyn, “Phase matching of high-order harmonics in hollow waveguides,” Phys. Rev. Lett. 83(11), 2187–2190 (1999).
[Crossref]

Kelley, B. K.

J. Aizpurua, G. W. Bryant, L. J. Richter, F. J. García de Abajo, B. K. Kelley, and T. Mallouk, “Optical properties of coupled metallic nanorods for field-enhanced spectroscopy,” Phys. Rev. B 71(23), 235420 (2005).
[Crossref]

Kim, S.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature 453(7196), 757–760 (2008).
[Crossref] [PubMed]

Kim, S.-W.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature 453(7196), 757–760 (2008).
[Crossref] [PubMed]

Kim, Y.

S. Kim, J. Jin, Y.-J. Kim, I.-Y. Park, Y. Kim, and S.-W. Kim, “High-harmonic generation by resonant plasmon field enhancement,” Nature 453(7196), 757–760 (2008).
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H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett. 108(21), 217403 (2012).
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[Crossref]

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C. Sun, F. Vallée, L. H. Acioli, E. P. Ippen, and J. G. Fujimoto, “Femtosecond-tunable measurement of electron thermalization in gold,” Phys. Rev. B Condens. Matter 50(20), 15337–15348 (1994).
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E. J. Sánchez, L. Novotny, and X. S. Xie, “Near-field fluorescence microscopy based on two-photon excitation with metal tips,” Phys. Rev. Lett. 82(20), 4014–4017 (1999).
[Crossref]

H. Harutyunyan, G. Volpe, R. Quidant, and L. Novotny, “Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas,” Phys. Rev. Lett. 108(21), 217403 (2012).
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Figures (4)

Fig. 1
Fig. 1 Band structure near the (a) X and (b) L points of the Brillouin zone of gold (adapted from Refs. 21 and 32). The blue curves are the 5d bands, and the red curve is the 6s-6p band. The black line at E= E f =0 is the Fermi level. Resonant contribution to the third-order susceptibility is shown for ~2-3 eV energies.
Fig. 2
Fig. 2 (a) A schematic of gold nanoparticle (NP) separated from ultraflat gold film by a SAM. (b) Scanning electron microscope image of a typical sample. (c) Dark field scattering spectrum of the sample does not show resonance in the fundamental region as well as the THG region (within the limits of our detection system).
Fig. 3
Fig. 3 (a) A schematic of the nonlinear measurement setup where LPF is longpass filter, Au-MR is 10 nm Au substrate used as beam splitter, MO is microscope objective, EM is energy meter, MR is mirror, L is lens, C is collimator, OF is optical fiber, NIR-SPEC is near-IR spectrometer, and VIS-SPEC is visible spectrometer. Top left is a schematic of the sample, gold nanoparticles-over-gold film separated by a SAM. (b) Spectrum of nonlinear conversion showing with black curve THG, SHG and a broad three photon photoluminescence. Red curve shows optimized THG where THG signal is maximized by adjusting the focus. Grey curve shows signal from the film only with no clear THG but some three photon photoluminescence. Background counts are subtracted from the curves. (c) Spectrum of the fundamental beam that was the source of the nonlinear spectrum shown in (b) after maximizing the THG signals (red curve). (d) The power-law dependence of THG signal, measured on one spot for incident energy varying between 14 µJ per pulse and 28 µJ per pulse, gives a slope of 3.2 ± 0.2 on a log-log plot.
Fig. 4
Fig. 4 (a) Normalized THG response as a function of wavelength. Counts per pulse have been normalized to the pulse energy cubed and calibrated using a black-body source of known temperature. The THG shows peaks in the range of 470 nm to 550 nm, which we attribute to the interband transition enhancements. For each wavelength, the standard deviation was obtained from measurements at different locations on two separate samples. (b) Normalized THG response calculated using a simple linear-polarization model for the third order susceptibility.

Equations (2)

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χ (3) ( ω )= bm N 3 e 4 [ ( χ ( 1 ) ( ω ) ) 3 χ ( 1 ) ( ω THG ) ]
χ Au ,interband ( 1 ) ( λ )= A 1 λ 1 ( exp( i π 4 ) ( 1 λ 1 1 λ i γ 1 ) + exp( i π 4 ) ( 1 λ 1 + 1 λ + i γ 1 ) )+ A 2 λ 2 ( exp(i π 4 ) ( 1 λ 2 1 λ i γ 2 ) + exp(i π 4 ) ( 1 λ 2 + 1 λ + i γ 2 ) )

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