Abstract
When light interacts with metal nanostructures, it can couple to free-electron excitations near the metal surface. The electromagnetic resonances associated with these surface plasmons depend on the details of the nanostructure, opening up opportunities for controlling light confinement on the nanoscale. The resulting strong electromagnetic fields allow weak nonlinear processes, which depend superlinearly on the local field, to be significantly enhanced. In addition to providing enhanced nonlinear effects with ultrafast response times, plasmonic nanostructures allow nonlinear optical components to be scaled down in size. In this Review, we discuss the principles of nonlinear plasmonic effects and present an overview of their main applications, including frequency conversion, switching and modulation of optical signals, and soliton effects.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$209.00 per year
only $17.42 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Boyd, R. W. Nonlinear Optics 3rd edn (Academic, 2008).
Zayats, A. V., Smolyaninov, I. I. & Maradudin, A. A. Nano-optics of surface plasmon polaritons. Phys. Rep. 408, 131–314 (2005).
Stockman, M. I. Nanoplasmonics: past, present, and glimpse into future. Opt. Express 19, 22029–22106 (2011).
Gramotnev, D. K. & Bozhevolnyi, S. I. Plasmonics beyond the diffraction limit. Nature Photon. 4, 83–91 (2010).
Novotny, L. & van Hulst, N. Antennas for light. Nature Photon. 5, 83–90 (2011).
Soukoulis, C. M. & Wegener, M. Past achievements and future challenges in the development of three-dimensional photonic metamaterials. Nature Photon. 5, 523–530 (2011).
Sharma, B., Frontiera, R. R., Henry, A., Ringe, E. & van Duyne, R. P. SERS: materials, applications, and the future. Mater. Today 15, 16–25 (2012).
Homola, J. Surface plasmon resonance sensors for detection of chemical and biological species. Chem. Rev. 108, 462–493 (2008).
Berini, P. & De Leon, I. Surface plasmon-polariton amplifiers and lasers. Nature Photon. 6, 16–24 (2012).
Herink, G., Solli, D. R., Gulde, M. & Ropers, C. Field-driven photoemission from nanostructures quenches the quiver motion. Nature 483, 190–193 (2012).
Sipe, J. E., So, V. C. Y., Fukui, M. & Stegeman, G. I. Analysis of second-harmonic generation at metal surfaces. Phys. Rev. B 21, 4389–4402 (1980).
Wang, F. X. et al. Surface and bulk contributions to the second-order nonlinear optical response of a gold film. Phys. Rev. B 80, 233402 (2009).
Anisimov, S. I., Kapeliovich, B. L. & Perelman, T. L. Electron emission from metal surfaces exposed to ultrashort laser pulses. Sov. Phys. JETP 39, 375–377 (1974).
Pines, D. & Nozieres, P. The Theory of Quantum Liquids Vol. I (Benjamin, 1966).
Ginzburg, P., Hayat, A., Berkovitch, N. & Orenstein, M. Nonlocal ponderomotive nonlinearity in plasmonics. Opt. Lett. 35, 1551–1553 (2010).
Chen, C. K., de Castro, A. R. B. & Shen, Y. R. Surface-enhanced second-harmonic generation. Phys. Rev. Lett. 46, 145–148 (1981).
Wokaun, A. et al. Surface second-harmonic generation from metal island films and microlithographic structures. Phys. Rev. B 24, 849–856 (1981).
Smolyaninov, I. I., Zayats, A. V. & Davis, C. C. Near-field second harmonic generation from a rough metal surface. Phys. Rev. B 56, 9290–9293 (1997).
Zayats, A. V., Kalkbrenner, T., Sandoghdar, V. & Mlynek, J. Second-harmonic generation from individual surface defects under local excitation. Phys. Rev. B 61, 4545–4548 (2000).
Bozhevolnyi, S. I., Beermann, J. & Coello, V. Direct observation of localized second-harmonic enhancement in random metal nanostructures. Phys. Rev. Lett. 90, 197403 (2003).
Anceau, C., Brasselet, S., Zyss, J. & Gadenne, P. Local second-harmonic generation enhancement on gold nanostructures probed by two-photon microscopy. Opt. Lett. 28, 713–715 (2003).
Stockman, M. I., Bergman, D. J., Anceau, C., Brasselet, S. & Zyss, J. Enhanced second-harmonic generation by metal surfaces with nanoscale roughness: nanoscale dephasing, depolarization, and correlations. Phys. Rev. Lett. 92, 057402 (2004).
Breit, M. et al. Experimental observation of percolation-enhanced nonlinear light scattering from semicontinuous metal films. Phys. Rev. B 64, 125106 (2001).
Kim, E. M. et al. Surface-enhanced optical third-harmonic generation in Ag island films. Phys. Rev. Lett. 95, 227402 (2005).
Simon, H. J., Mitchell, D. E. & Watson, J. G. Optical second-harmonic generation with surface plasmons in silver films. Phys. Rev. Lett. 33, 1531–1534 (1974).
Renger, J., Quidant, R., van Hulst, N. & Novotny, L. Surface-enhanced nonlinear four-wave mixing. Phys. Rev. Lett. 104, 046803 (2010).
Grosse, N. B., Heckmann, J. & Woggon, U. Nonlinear plasmon-photon interaction resolved by k-space spectroscopy. Phys. Rev. Lett. 108, 136802 (2012).
Dadap, J. I., Shan, J., Eisenthal, K. B. & Heinz, T. F. Second-harmonic Rayleigh scattering from a sphere of centrosymmetric material. Phys. Rev. Lett. 83, 4045–4048 (1999).
Dadap, J. I., Shan, J. & Heinz, T. F. Theory of optical second-harmonic generation from a sphere of centrosymmetric material: small-particle limit. J. Opt. Soc. Am. B 21, 1328–1347 (2004).
Vance, F. W., Lemon, B. I. & Hupp, J. T. Enormous hyper-Rayleigh scattering from nanocrystalline gold particle suspensions. J. Phys. Chem. B 102, 10091–10093 (1998).
Hao, E. C., Schatz, G. C., Johnson, R. C. & Hupp, J. T. Hyper-Rayleigh scattering from silver nanoparticles. J. Chem. Phys. 117, 5963–5966 (2002).
Nappa, J., Russier-Antoine, I., Benichou, E., Jonin, C. & Brevet, P. F. Second harmonic generation from small gold metallic particles: from the dipolar to the quadrupolar response. J. Chem. Phys. 125, 184712 (2006).
Butet, J. et al. Interference between selected dipoles and octupoles in the optical second-harmonic generation from spherical gold nanoparticles. Phys. Rev. Lett. 105, 077401 (2010).
Butet, J. et al. Optical second harmonic generation of single metallic nanoparticles embedded in a homogeneous medium. Nano Lett. 10, 1717–1721 (2010).
Butet, J. et al. Sensing with multipolar second harmonic generation from spherical metallic nanoparticles. Nano Lett. 12, 1697–1701 (2012).
Bouhelier, A., Beversluis, M., Hartschuh, A. & Novotny, L. Near-field second-harmonic generation induced by local field enhancement. Phys. Rev. Lett. 90, 013903 (2003).
Neacsu, C. C., Reider, G. A. & Raschke, M. B. Second-harmonic generation from nanoscopic metal tips: symmetry selection rules for single asymmetric nanostructures. Phys. Rev. B 71, 201402 (2005).
Nahata, A., Linke, R. A., Ishi, T. & Ohashi, K. Enhanced nonlinear optical conversion from a periodically nanostructured metal film. Opt. Lett. 28, 423–425 (2003).
Danckwerts, M. & Novotny, L. Optical frequency mixing at coupled gold nanoparticles. Phys. Rev. Lett. 98, 026104 (2007).
Marinica, D. C., Kazansky, A. K., Nordlander, P., Aizpurua, J. & Borisov, A. G. Quantum plasmonics: nonlinear effects in the field enhancement of a plasmonic nanoparticle dimer. Nano Lett. 12, 1333–1339 (2012).
Hanke, T. et al. Tailoring spatiotemporal light confinement in single plasmonic nanoantennas. Nano Lett. 12, 992–996 (2012).
Zhang, Y., Grady, N. K., Ayala-Orozco, C. & Halas, N. J. Three-dimensional nanostructures as highly efficient generators of second harmonic light. Nano Lett. 11, 5519–5523 (2011).
Cai, W., Vasudev, A. P. & Brongersma, M. L. Electrically controlled nonlinear generation of light with plasmonics. Science 333, 1720–1723 (2011).
Pu, Y., Grange, R., Hsieh, C-L. & Psaltis, D. Nonlinear optical properties of core-shell nanocavities for enhanced second-harmonic generation. Phys. Rev. Lett. 104, 207402 (2010).
Park, I-Y. et al. Plasmonic generation of ultrashort extreme-ultraviolet light pulses. Nature Photon. 5, 677–681 (2011).
Reinisch, R. & Nevière, M. Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects. Phys. Rev. B 28, 1870–1885 (1983).
Coutaz, J. L., Nevière, M., Pic, E. & Reinisch, R. Experimental study of surface-enhanced second-harmonic generation on silver gratings. Phys. Rev. B 32, 2227–2232 (1985).
Lamprecht, B., Leitner, A. & Aussenegg, F. R. Femtosecond decay-time measurement of electron-plasma oscillation in nanolithographically designed silver particles. Appl. Phys. B 64, 269–272 (1997).
Tuovinen, H. et al. Linear and second-order nonlinear optical properties of arrays of noncentrosymmetric gold nanoparticles. J. Nonlin. Opt. Phys. Mater. 11, 421–432 (2002).
Canfield, B. K. et al. Linear and nonlinear optical responses influenced by broken symmetry in an array of gold nanoparticles. Opt. Express 12, 5418–5423 (2004).
Linden, S. et al. Collective effects in second-harmonic generation from split-ring-resonator arrays. Phys. Rev. Lett. 109, 015502 (2012).
Klein, M. W., Enkrich, C., Wegener, M. & Linden, S. Second-harmonic generation from magnetic meta-materials. Science 313, 502–504 (2006).
Feth, N. et al. Second-harmonic generation from complementary split-ring resonators. Opt. Lett. 33, 1975–1977 (2008).
McMahon, M. D., Lopez, R., Haglund, R. F. Jr, Ray, E. A. & Bunton, P. H. Second-harmonic generation from arrays of symmetric gold nanoparticles. Phys. Rev. B 73, 041401 (2006).
Xu, T., Jiao, X., Zhang, G. P. & Blair, S. Second-harmonic emission from sub-wavelength apertures: effects of aperture symmetry and lattice arrangement. Opt. Express 15, 13894–13906 (2006).
Lesuffleur, A., Swaroop Kumar, L. K. & Gordon, R. Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film. Appl. Phys. Lett. 88, 261104 (2006).
van Nieuwstadt, J. A. H. et al. Strong modification of the nonlinear optical response of metallic subwavelength hole arrays. Phys. Rev. Lett. 97, 146102 (2006).
Kujala, S., Canfield, B. K., Kauranen, M., Svirko, Y. & Turunen, J. Multipole interference in the second-harmonic optical radiation from gold nanoparticles. Phys. Rev. Lett. 98, 167403 (2007).
Czaplicki, R. et al. Dipole limit in second-harmonic generation from arrays of gold nanoparticles. Opt. Express 19, 26866–26871 (2011).
Canfield, B. K. et al. Local field asymmetry drives second-harmonic generation in noncentrosymmetric nanodimers. Nano Lett. 7, 1251–1255 (2007).
Valev, V. K. et al. Plasmonic ratchet wheels: switching circular dichroism by arranging chiral nanostructures. Nano Lett. 9, 3945–3948 (2009).
Valev, V. K. et al. Plasmons reveal the direction of magnetization in nickel nanostructures. ACS Nano 5, 91–96 (2011).
Fan, W. et al. Second harmonic generation from a nanopatterned isotropic nonlinear material. Nano Lett. 6, 1027–1030 (2006).
Niesler, F. B. P. et al. Second-harmonic generation from split-ring resonators on a GaAs substrate. Opt. Lett. 34, 1997–1999 (2009).
Chen, K., Durak, C., Heflin, J. R. & Robinson, H. D. Plasmon-enhanced second-harmonic generation from ionic self-assembled multilayer films. Nano Lett. 7, 254–258 (2007).
Belardini, A. et al. Tailored second harmonic generation from self-organized metal nano-wires arrays. Opt. Express 17, 3603–3609 (2009).
Genevet, P. et al. Large enhancement of nonlinear optical phenomena by plasmonic nanocavity gratings. Nano Lett. 10, 4880–4883 (2010).
Steuwe, C., Kaminski, C. F., Baumberg, J. J. & Mahajan, S. Surface enhanced coherent anti-Stokes Raman scattering on nanostructured gold surfaces. Nano Lett. 11, 5339–5343 (2011).
Kim, S. et al. High-harmonic generation by resonant plasmon field enhancement. Nature 453, 757–760 (2008).
Ko, K. D. et al. Nonlinear optical response from arrays of Au bowtie nanoantennas. Nano Lett. 11, 61–65 (2011).
Husu, H. et al. Metamaterials with tailored nonlinear optical response. Nano Lett. 12, 673–677 (2012).
Link, S. & El-Sayed, M. A. Spectral properties and relaxation dynamics of surface plasmon electronic oscillations in gold and silver nanodots and nanorods. J. Phys. Chem. 103, 8410–8426 (1999).
Baida, H. et al. Ultrafast nonlinear optical response of a single gold nanorod near its surface plasmon resonance. Phys. Rev. Lett. 107, 057402 (2011).
Piredda, G., Smith, D. D., Wendling, B. & Boyd, R. W. Nonlinear optical properties of a gold-silica composite with high gold fill fraction and the sign change of its nonlinear absorption coefficient. J. Opt. Soc. Am. B 25, 945–950 (2008).
Halonen, M., Lipovskii, A. A. & Svirko, Yu. P. Femtosecond absorption dynamics in glass-metal nanocomposites. Opt. Express 15, 6840–6845 (2007).
Ma, G. et al. Size and dielectric dependence of the third-order nonlinear optical response of Au nanocrystals embedded in matrices. Opt. Lett. 27, 1043–1045 (2002).
Sipe, J. E. & Boyd, R. W. Nonlinear susceptibility of composite optical materials in the Maxwell-Garnett model. Phys. Rev. A 46, 1614–1629 (1992).
Kohlgraf-Owens, D. C. & Kik, P. G. Numerical study of surface plasmon enhanced nonlinear absorption and refraction. Opt. Express 16, 16823–16834 (2008).
Dickson, W. et al. Dielectric-loaded plasmonic nano-antenna arrays: a metamaterial with tuneable optical properties. Phys. Rev. B 76, 115411 (2007).
Fu, M. et al. Resonantly enhanced optical nonlinearity in hybrid semiconductor quantum dot – metal nanoparticle structures. Appl. Phys. Lett. 100, 063117 (2012).
Abb, M., Albella, P., Aizpurua, J. & Muskens, O. L. All-optical control of a single plasmonic nanoantenna-ITO hybrid. Nano Lett. 11, 2457–2463 (2011).
Smolyaninov, I. I., Zayats, A. V., Gungor, A. & Davis, C. C. Single-photon tunneling via localized surface plasmons. Phys. Rev. Lett. 88, 187402 (2002).
Smolyaninov, I. I., Davis, C. C. & Zayats, A. V. Light-controlled photon tunnelling. Appl. Phys. Lett. 81, 3314–3316 (2002).
Innes, R. A. & Sambles, J. R. Optical non-linearity in liquid crystals using surface plasmon-polaritons. J. Phys. Condens. Matter 1, 6231–6260 (1989).
Rotenberg, N., Betz, M. & van Driel, H. M. Ultrafast all-optical coupling of light to surface plasmon polaritons on plain metal surfaces. Phys. Rev. Lett. 105, 017402 (2010).
Krasavin, A. V. & Zheludev, N. I. Active plasmonics: controlling signals in Au/Ga waveguide using nanoscale structural transformations. Appl. Phys. Lett. 84, 1416–1418 (2004).
Krasavin, A. V., MacDonald, K. F., Zheludev, N. I. & Zayats, A. V. High-contrast modulation of light with light by control of surface plasmon polariton wave coupling. Appl. Phys. Lett. 85, 3369–3371 (2004).
Pacifici, D., Lezec, H. J. & Atwater, H. A. All-optical modulation by plasmonic excitation of CdSe quantum dots. Nature Photon. 1, 402–406 (2007).
Pala, R. A., Shimizu, K. T., Melosh, N. A. & Brongersma, M. L. A nonvolatile plasmonic switch employing photochromic molecules. Nano Lett. 8, 1506–1510 (2008).
Krasavin, A. V. et al. All-plasmonic modulation via stimulated emission of co-propagating surface plasmon polaritons on a substrate with gain. Nano Lett. 11, 2231–2235 (2011).
MacDonald, K. F., Samson, Z. L., Stockman, M. I. & Zheludev, M. I. Ultrafast active plasmonics. Nature Photon. 3, 55–58 (2009).
Krasavin, A. V. et al. Optically-programmable nonlinear photonic component for dielectric-loaded plasmonic circuitry. Opt. Express 19, 25222–25229 (2011).
Krasavin, A. V. & Zayats, A. V. Electro-optic switching element for dielectric-loaded surface plasmon polariton waveguides. Appl. Phys. Lett. 97, 041107 (2010).
Wurtz, G. A. & Zayats, A. V. Nonlinear surface plasmon polaritonic crystals. Laser Photon. Rev. 2, 125–135 (2008).
Rotenberg, N., Caspers, J. N. & van Driel, H. M. Tunable ultrafast control of plasmonic coupling to gold films. Phys. Rev. B 80, 245420 (2009).
Smolyaninov, I. I., Zayats, A. V., Stanishevsky, A. & Davis, C. C. Optical control of photon tunneling through an array of nanometer-scale cylindrical channels. Phys. Rev. B 66, 205414 (2002).
Wurtz, G. A., Pollard, R. & Zayats, A. V. Optical bistability in nonlinear surface plasmon polaritonic crystals. Phys. Rev. Lett. 97, 057402 (2006).
Minovich, A. et al. Liquid crystal based nonlinear fishnet metamaterials. Appl. Phys. Lett. 100, 121113 (2012).
Dykhne, A. M., Sarychev, A. K. & Shalaev, V. M. Resonant transmittance through metal films with fabricated and light-induced modulation. Phys. Rev. B 67, 195402 (2003).
Min, C. et al. All-optical switching in subwavelength metallic grating structure containing nonlinear optical materials. Opt. Lett. 33, 869–871 (2008).
Porto, J. A., Martín-Moreno, L. & García-Vidal, F. J. Optical bistability in subwavelength slit apertures containing nonlinear media. Phys. Rev. B 70, 081402 (2004).
Nikolaenko, A. E. et al. Carbon nanotubes in a photonic metamaterial. Phys. Rev. Lett. 104, 153902 (2010).
Ren, M. et al. Nanostructured plasmonic medium for terahertz bandwidth all-optical switching. Adv. Mater. 23, 5540–5544 (2011).
Argyropoulos, C., Chen, P.Y., D'Aguano, G., Engheta, N. & Alu, A. Boosting optical nonlinearities in epsilon-near-zero plasmonic channels. Phys. Rev. B 85, 045129 (2012).
Wurtz, G. A. et al. Designed ultrafast optical nonlinearity in a plasmonic nanorod metamaterial enhanced by nonlocality. Nature Nanotech. 6, 107–111 (2011).
Wurtz, G. A. et al. Molecular plasmonics with tunable exciton-plasmon coupling strength in J-aggregate hybridized Au nanorod assemblies. Nano Lett. 7, 1297–1303 (2007).
Vasa, P. et al. Ultrafast manipulation of strong coupling in metal-molecular aggregate hybrid nanostructures. ACS Nano 4, 7759–7765 (2010).
Agranovich, V. M., Babichenko, V. S. & Chernyak, Y. Ya. Nonlinear surface polaritons. JETP Lett. 32, 512–515 (1980).
Stegeman, G. I., Seaton, C. T., Ariyasu, J., Wallis, R. F. & Maradudin, A. A. Nonlinear electromagnetic waves guided by a single interface. J. Appl. Phys. 58, 2453–2459 (1985).
Boardman, A. D., Cooper, G. S., Maradudin, A. A. & Shen, T. P. Surface-polariton solitons. Phys. Rev. B 34, 8273–8278 (1986).
Davoyan, A. R., Shadrirov, I. V. & Kivshar, Yu. S. Nonlinear plasmonic slot waveguides. Opt. Express 16, 21209–21214 (2008).
Feigenbaum, E. & Orenstein, M. Plasmon-soliton. Opt. Lett. 32, 674–676 (2007).
Noskov, R. E., Belov, P. A. & Kivshar, Yu. S. Subwavelength modulational instability and plasmon oscillons in nanoparticle arrays. Phys. Rev. Lett. 108, 093901 (2012).
Davoyan, A. R., Shadrirov, I. V. & Kivshar, Yu. S. Self-focusing and spatial plasmon-polariton solitons. Opt. Express 17, 21732–21737 (2009).
Marini, A., Skryabin, D. V. & Malomed, B. Stable spatial plasmon solitons in a dielectric-metal-dielectric geometry with gain and loss. Opt. Express 19, 6616–6622 (2011).
Ye, F., Mihalache, D., Hu, B. & Panoiu, N. C. Subwavelength plasmonic lattice solitons in arrays of metallic nanowires. Phys. Rev. Lett. 104, 106802 (2010).
Liu, Y., Bartal, G., Genov, D. A. & Zhang, X. Subwavelength discrete solitons in nonlinear metamaterials. Phys. Rev. Lett. 99, 153901 (2007).
Zeng, Y., Hoyer, W., Liu, J., Koch, S. W. & Moloney, J. V. Classical theory for second-harmonic generation from metallic nanoparticles. Phys. Rev. B 79, 235109 (2009).
Benedetti, A., Centini, M., Bertolotti, M. & Sibilia, C. Second harmonic generation from 3D nanoantennas: on the surface and bulk contributions by far-field pattern analysis. Opt. Express 19, 26752–26767 (2011).
Ciracì, C., Poutrina, E., Scalora, M. & Smith, D. R. Origin of second-harmonic generation enhancement in optical split-ring resonators. Phys. Rev. B 85, 201403 (2012).
Esteban, R., Borisov, A. G., Nordlander, P. & Aizpurua, J. Bridging quantum and classical plasmonics with a quantum-corrected model. Nature Commun. 3, 825 (2012).
García de Abajo, F. J. Nonlocal effects in the plasmons of strongly interacting nanoparticles, dimers, and waveguides. J. Phys. Chem. C 112, 17983–17987 (2008).
Kim, E., Wang, F., Wu, W., Yu, Z. & Shen, Y. R. Nonlinear optical spectroscopy of photonic metamaterials. Phys. Rev. B 78, 113102 (2008).
Hentschel, M., Utikal, T., Giessen, H. & Lippitz, M. Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas. Nano Lett. 12, 3778–3782 (2012).
Thyagarajan, K., Rivier, S., Lovera, A. & Martin, O. J. F. Enhanced second-harmonic generation from double resonant plasmonic antennae. Opt. Express 20, 12860–12865 (2012).
Harutyunyan, H., Volpe, G., Quidant, R. & Novotny, L. Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas. Phys. Rev. Lett. 108, 217403 (2012).
Author information
Authors and Affiliations
Corresponding authors
Rights and permissions
About this article
Cite this article
Kauranen, M., Zayats, A. Nonlinear plasmonics. Nature Photon 6, 737–748 (2012). https://doi.org/10.1038/nphoton.2012.244
Published:
Issue Date:
DOI: https://doi.org/10.1038/nphoton.2012.244
This article is cited by
-
Three-dimensional nonlinear optical materials from twisted two-dimensional van der Waals interfaces
Nature Photonics (2024)
-
Ultra-Fast All-Optical Plasmonic Dual-Band Nonlinear Off–On and Two-Port Switches
Plasmonics (2024)
-
Nonlinear plasmonics: second-harmonic generation and multiphoton photoluminescence
PhotoniX (2023)
-
A whispering-gallery scanning microprobe for Raman spectroscopy and imaging
Light: Science & Applications (2023)
-
A multi-mode super-fano mechanism for enhanced third harmonic generation in silicon metasurfaces
Light: Science & Applications (2023)