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Approaching the quantum limit for nanoplasmonics

  • Emily Townsend (a1), Alex Debrecht (a2) and Garnett W. Bryant (a3)


The character of optical excitations in nanoscale and atomic-scale materials is often strongly mixed, having contributions from both single-particle transitions and collective, plasmon-like response. This complicates the quantum description of these excitations, because there is no clear way to define their quantization. To move toward a quantum theory for these optical excitations, they must first be characterized so that single-particle-like and collective, plasmon-like excitations can be identified. We show that time-dependent density functional theory can be used to make that characterization if both the charge densities induced by the excitation and the transitions that make up the excitation are analyzed. Density functional theory predicts that single-particle-like and collective excitations can coexist. Exact calculations for small nanosystems predict that single-particle excitations evolve into collective excitations as the electron–electron interaction is turned on with no indication that they coexist. These different predictions present a challenge that must be resolved to develop an understanding for quantum excitations in nanoplasmonic materials.

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1.Pelton, M. and Bryant, G.: Introduction to Metal-Nanoparticle Plasmonics (Wiley, Hoboken, New Jersey, 2013).
2.Bernadotte, S., Evers, F., and Jacob, C.R.: Plasmons in molecules. J. Phys. Chem. C 117, 1863 (2013).
3.Gao, B., Ruud, K., and Luo, Y.: Plasmon resonances in linear noble-metal chains. J. Chem. Phys. 137, 194307 (2012).
4.Wallis, T.M., Nilius, N., and Ho, W.: Electronic density oscillations in gold atomic chains assembled atom by atom. Phys. Rev. Lett. 89, 236802 (2002).
5.Yan, J., Yuan, Z., and Gao, S.: End and central plasmon resonances in linear atomic chains. Phys. Rev. Lett. 98, 216602 (2007).
6.Perez, R. and Que, W.: Plasmons in isolated single-walled carbon nanotubes. J. Phys.: Condens. Matter 18, 3197 (2006).
7.Thongrattanasiri, S., Silveiro, I., and García de Abajo, F.J.: Plasmons in electrostatically doped graphene. Appl. Phys. Lett. 100, 201105 (2012).
8.Manjavacas, A., Marchesin, F., Thongrattanasiri, S., Koval, P., Nordlander, P., Sánchez-Portal, D., and García de Abajo, F.J.: Tunable molecular plasmons in polycyclic aromatic hydrocarbons. ACS Nano 7, 3635 (2013).
9.Raether, H.: Surface Plasmons on Smooth and Rough Surfaces and on Gratings (Springer-Verlag, New York, 1988).
10.Kalkbrenner, T., Håkanson, U., Schädle, A., Burger, S., Henkel, C., and Sandoghdar, V.: Optical microscopy via spectral modifications of a nanoantenna. Phys. Rev. Lett. 95, 200801 (2005).
11.Anger, P., Bharadwaj, P., and Novotny, L.: Enhancement and quenching of single-molecule fluorescence. Phys. Rev. Lett. 96, 113002 (2006).
12.Pendry, J.B.: Negative refraction makes a perfect lens. Phys. Rev. Lett. 85, 3966 (2000).
13.Shalaev, V.M.: Optical negative-index metamaterials. Nat. Photonics 1, 41 (2007).
14.Murray, W.A. and Barnes, W.L.: Plasmonic materials. Adv. Mater. 19, 3771 (2007).
15.Catchpole, K.R. and Polman, A.: Plasmonic solar cells. Opt. Express. 16, 21793 (2008).
16.Coppens, Z.J., Li, W., Walker, D.G., and Valentine, J.G.: Probing and controlling photothermal heat generation in plasmonic nanostructures. Nano Lett. 13, 1023 (2013).
17.Hirsch, L.R., Stafford, R.J., Bankson, J.A., Sershen, S., Rivera, B., Price, R.E., Hazle, J.D., Halas, N.J., and West, J.: Nanoshell-mediated near-infrared thermal therapy of tumors under magnetic resonance guidance. Proc. Natl. Acad. Sci. USA 100, 13549 (2003).
18.Tame, M.S., McEnery, K.R., Özdemir, S.K., Lee, J., Maier, S.A., and Kim, M.S.: Quantum plasmonics. Nat. Phys. 9, 329 (2013).
19.Bryant, G.W., Waks, E., and Krenn, J.R.: Plasmonics: The rise of quantum effects. Opt. Photonics News 25, 50 (2014).
20.Esteban, R., Borisov, A.G., Nordlander, P., and Aizpurua, J.: Bridging quantum and classical plasmonics with a quantum-corrected model. Nat. Commun. 3, 825 (2012).
21.Townsend, E. and Bryant, G.W.: Plasmonic properties of metallic nanoparticles: The effects of size quantization. Nano Lett. 12, 429 (2012).
22.Townsend, E. and Bryant, G.W.: Which resonances in small metallic nanoparticles are plasmonic? J. Opt. 16, 114022 (2014).
23.Altewischer, E., van Exter, M.P., and Woerdman, J.P.: Plasmon-assisted transmission of entangled photons. Nature 418, 304 (2002).
24.Fasel, S., Robin, F., Moreno, E., Erni, D., Gisin, N., and Zbinden, H.: Energy–time entanglement preservation in plasmon-assisted light transmission. Phys. Rev. Lett. 94, 110501 (2005).
25.Huck, A., Smolka, S., Lodahl, P., Sørensen, A.S., Boltasseva, A., Janousek, J., and Andersen, U.L.: Demonstration of quadrature-squeezed surface plasmons in a gold waveguide. Phys. Rev. Lett. 102, 246802 (2009).
26.Hong, C.K., Ou, Z.Y., and Mandel, L.: Measurement of subpicosecond time intervals between two photons by interference. Phys. Rev. Lett. 59, 2044 (1987).
27.Heeres, R.W., Kouwenhoven, L.P., and Zwiller, V.: Quantum interference in plasmonic circuits. Nat. Nanotechnol. 8, 719 (2013).
28.Fakonas, J.S., Lee, H., Kelaita, Y.A., and Atwater, H.A.: Two-plasmon quantum interference. Nat. Photonics 8, 317 (2014).
29.Dadosh, T., Sperling, J., Bryant, G.W., Breslow, R., Shegai, T., Dyshel, M., Haran, G., and Bar-Joseph, I.: Plasmonic control of the shape of the Raman spectrum of a single molecule in.a silver nanoparticle dimer. ACS Nano 3, 1988 (2009).
30.Cohen-Hoshen, E., Bryant, G.W., Pinkas, I., Sperling, J., and Bar-Joseph, I.: Exciton−plasmon interactions in quantum dot−gold nanoparticle structures. Nano Lett. 12, 4260 (2012).
31.Zhang, W., Govorov, A.O., and Bryant, G.W.: Semiconductor-metal nanoparticle molecules: Hybrid excitons and the nonlinear Fano effect. Phys. Rev. Lett. 97, 146804 (2006).
32.Yan, J-Y., Zhang, W., Duan, S., Zhao, X-G., and Govorov, A.O.: Optical properties of coupled metal-semiconductor and metal-molecule nanocrystal complexes: Role of multipole effects. Phys. Rev. B 77, 165301 (2008).
33.Artuso, R.D. and Bryant, G.W.: Optical response of strongly coupled quantum dot-metal nanoparticle systems: Double peaked Fano structure and bistability. Nano Lett. 8, 2106 (2009).
34.Artuso, R.D. and Bryant, G.W.: Strongly coupled quantum dot metal nanoparticle systems: Exciton-induced transparency, discontinuous response, and suppression as driven quantum oscillator effects. Phys. Rev. B 82, 195419 (2010).
35.Artuso, R.D., Bryant, G.W., García-Etxarri, A., and Aizpurua, J.: Using local fields to tailor hybrid quantum-dot/metal nanoparticle systems. Phys. Rev. B 83, 235406 (2011).
36.Artuso, R.D. and Bryant, G.W.: Quantum dot–quantum dot interactions mediated by a metal nanoparticle: Towards a fully quantum model. Phys. Rev. B 87, 125423 (2013).
37.Sadeghi, S.M.: Plasmonic metaresonances: Molecular resonances in quantum dot-metallic nanoparticle conjugates. Phys. Rev. B 79, 233309 (2009).
38.Malyshev, A.V. and Malyshev, V.A.: Optical bistability and hysteresis of a hybrid metal-semiconductor nanodimer. Phys. Rev. B 84, 035314 (2011).
39.Waks, E. and Sridharan, D.: Cavity QED treatment of interactions between a metal nanoparticle and a dipole emitter. Phys. Rev. A 82, 043845 (2010).
40.Ridolfo, A., Di Stefano, O., Fina, N., Saija, R., and Savasta, S.: Quantum plasmonics with quantum dot-metal nanoparticle molecules: Influence of the Fano effect on photon statistics. Phys. Rev. Lett. 105, 263601 (2010).
41.Esteban, R., Aizpurua, J., and Bryant, G.W.: Strong coupling of single emitters interacting with phononic infrared antennae. New J. Phys. 16, 013052 (2014).
42.Trugler, A. and Hohenester, U.: Strong coupling between a metallic nanoparticle and a single molecule. Phys. Rev. B 77, 115403 (2008).
43.Zhang, W. and Govorov, A.O.: Quantum theory of the nonlinear Fano effect in hybrid metal-semiconductor nanostructures: The case of strong nonlinearity. Phys. Rev. B 84, 081405 (2011).
44.Gonzalez-Tudela, A., Martin-Cano, D., Moreno, E., Martin-Moreno, L., Tejedor, C., and García-Vidal, F.J.: Entanglement of two qubits mediated by one-dimensional plasmonic waveguides. Phys. Rev. Lett. 106, 020501 (2011).
45.Chen, X-W., Sandoghdar, V., and Agio, M.: Coherent interaction of light with a metallic structure coupled to a single quantum emitter: From superabsorption to cloaking. Phys. Rev. Lett. 110, 153605 (2013).
46.Sadeghi, S.M. and West, R.G.: Coherent control of Forster energy transfer in nanoparticle molecules: Energy nanogates and plasmonic heat pulses. J. Phys: Condens. Matter 23, 425302 (2011).
47.Sadeghi, S.M.: Tunable nanoswitches based on nanoparticle meta-molecules. Nanotechnology 21, 355501 (2010).
48.Sadeghi, S.M.: Optical routing and switching of energy flow in nanostructure systems. Appl. Phys. Lett. 99, 113113 (2011).
49.Bohm, D. and Pines, D.: A collective description of electron interactions. I. Magnetic interactions. Phys. Rev. 82, 625 (1951).
50.Crowell, J. and Ritchie, R.H.: Radiative decay of Coulomb-stimulated plasmons in spheres. Phys. Rev. 172, 436 (1968).
51.Castro, A., Appel, H., Oliveira, M., Rozzi, C.A., Andrade, X., Lorenzen, F., Marques, M., Gross, E., and Rubio, A.: Octopus: A tool for the application of time-dependent density functional theory. Phys. Status Solidi B 243, 2465 (2006).
52.Prodan, E. and Nordlander, P.: Exchange and correlation effects in small metallic nanoshells. Chem. Phys. Lett. 349, 153 (2001).
53.Zuloaga, J., Prodan, E., and Nordlander, P.: Quantum description of the plasmon resonances of a nanoparticle dimer. Nano Lett. 9, 887 (2009).
54.Zhang, P., Feist, J., Rubio, A., García-González, P., and García-Vidal, F.J.: Ab initio nanoplasmonics: The impact of atomic structure. Phys. Rev. B 90, 161407(R) (2014).


Approaching the quantum limit for nanoplasmonics

  • Emily Townsend (a1), Alex Debrecht (a2) and Garnett W. Bryant (a3)


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