Abstract

Multishell nanospheres have been proposed as a class of layered alternating metal-dielectric probes (LAMPs) that can greatly enhance sensitivity and multiplexing capabilities of optical molecular imaging . Here we theoretically demonstrate that the interplasmonic coupling within these spheres and hence their spectral responses can be tuned by a rational selection of layer thicknesses. As a proof-of-concept, layered Mie theory calculations of near- and far-field characteristics followed by a genetic algorithm-based selection are presented for gold-silica, silver-silica and copper-silica LAMPs. The results demonstrate that the optical tunability available allows for design of application (excitation wavelength)-specific probes of different sizes. The tunability further increases with number of layers and within a particular allowable probe size provides for structures with distinct resonances at longer wavelengths. The concept of scaling internal field resonances is also shown theoretically and the range over which the magnitudes can be tuned are presented.

© 2010 OSA

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2010 (2)

R. Bardhan, S. Mukerjee, N. A. Mirin, S. D. Levit, P. Nordlander, and N. J. Halas, “Nanosphere-in-a-nanoshell: a simple nanomatryushka,” J. Phys. Chem. C 114(16), 7378–7383 (2010).
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[CrossRef] [PubMed]

2009 (1)

B. Sepúlveda, P. C. Angelome, L. M. Lechuga, and L. M. Liz-Marzan, “LSPR-based nanobiosensors,” Nano Today 4(3), 244–251 (2009).
[CrossRef]

2008 (8)

A. M. Dennis and G. Bao, “Quantum dot-fluorescent protein pairs as novel fluorescence resonance energy transfer probes,” Nano Lett. 8(5), 1439–1445 (2008).
[CrossRef] [PubMed]

C. McDonagh, C. S. Burke, and B. D. MacCraith, “Optical chemical sensors,” Chem. Rev. 108(2), 400–422 (2008).
[CrossRef] [PubMed]

U. Resch-Genger, M. Grabolle, S. Cavaliere-Jaricot, R. Nitschke, and T. Nann, “Quantum dots versus organic dyes as fluorescent labels,” Nat. Methods 5(9), 763–775 (2008).
[CrossRef] [PubMed]

J. Kundu, F. Le, P. Nordlander, and N. J. Halas, “Surface enhanced infrared absorption (SEIRA) spectroscopy on nanoshell aggregate substrates,” Chem. Phys. Lett. 452(1-3), 115–119 (2008).
[CrossRef]

A. K. Kodali and R. Bhargava, “Tunable multilayered nanospheres as probes for surface-enahnced Raman spectroscopy,” Proc. SPIE 7032, 70320V (2008).
[CrossRef]

Y. Hu, R. C. Fleming, and R. A. Drezek, “Optical properties of gold-silica-gold multilayer nanoshells,” Opt. Express 16(24), 19579–19591 (2008).
[CrossRef] [PubMed]

Y. Fang, N. H. Seong, and D. D. Dlott, “Measurement of the distribution of site enhancements in surface-enhanced Raman scattering,” Science 321(5887), 388–392 (2008).
[CrossRef] [PubMed]

X. Qian, X. H. Peng, D. O. Ansari, Q. Yin-Goen, G. Z. Chen, D. M. Shin, L. Yang, A. N. Young, M. D. Wang, and S. Nie, “In vivo tumor targeting and spectroscopic detection with surface-enhanced Raman nanoparticle tags,” Nat. Biotechnol. 26(1), 83–90 (2008).
[CrossRef]

2007 (2)

P. K. Jain, X. Huang, I. H. El-Sayed, and M. A. El-Sayed, “Review of some interesting surface plasmon resonance-enhanced properties of noble metal nanoparticles and their applications to biosystems,” Plasmonics 2(3), 107–118 (2007).
[CrossRef]

Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
[CrossRef] [PubMed]

2006 (4)

L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
[CrossRef] [PubMed]

B. Khlebtsov and N. Khlebtsov, “Ultrasharp light-scattering resonances of structured nanospheres: effects of size-dependent dielectric functions,” J. Biomed. Opt. 11(4), 044002 (2006).
[CrossRef] [PubMed]

X. Xia, Y. Liu, V. Backman, and G. A. Ameer, “Engineering sub-100 nm multi-layer nanoshells,” Nanotechnology 17(21), 5435–5440 (2006).
[CrossRef]

B. D. Chithrani, A. A. Ghazani, and W. C. W. Chan, “Determining the size and shape dependence of gold nanoparticle uptake into mammalian cells,” Nano Lett. 6(4), 662–668 (2006).
[CrossRef] [PubMed]

2005 (7)

C. Eggeling, A. Volkmer, and C. A. M. Seidel, “Molecular photobleaching kinetics of Rhodamine 6G by one- and two-photon induced confocal fluorescence microscopy,” ChemPhysChem 6(5), 791–804 (2005).
[CrossRef] [PubMed]

X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
[CrossRef] [PubMed]

H. Xu, “Multilayered metal core-shell nanostructures for inducing a large and tunable local optical field,” Phys. Rev. B 72(7), 0734051–0734054 (2005).
[CrossRef]

K. Chen, Y. Liu, G. Ameer, and V. Backman, “Optimal design of structured nanospheres for ultrasharp light-scattering resonances as molecular imaging multilabels,” J. Biomed. Opt. 10(2), 024005 (2005).
[CrossRef] [PubMed]

C. Loo, A. Lowery, N. J. Halas, J. L. West, and R. Drezek, “Immunotargeted nanoshells for integrated cancer imaging and therapy,” Nano Lett. 5(4), 709–711 (2005).
[CrossRef] [PubMed]

J. Zhang, J. Malicka, I. Gryczynski, and J. R. Lakowicz, “Surface-enhanced fluorescence of fluorescein-labeled oligonucleotides capped on silver nanoparticles,” J. Phys. Chem. B 109(16), 7643–7648 (2005).
[CrossRef]

M. Moskovits, “Surface-enhanced Raman spectroscopy: a brief retrospective,” J. Raman Spectrosc. 36(6-7), 485–496 (2005).
[CrossRef]

2004 (6)

A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

C. L. Nehl, N. K. Grady, G. P. Goodrich, F. Tam, N. J. Halas, and J. H. Hafner, “Scattering spectra of single gold nanoshells,” Nano Lett. 4(12), 2355–2359 (2004).
[CrossRef]

V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
[CrossRef]

H. Xu, X. H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, “Unified treatment of fluorescence and raman scattering processes near metal surfaces,” Phys. Rev. Lett. 93(24), 243002 (2004).
[CrossRef]

W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
[CrossRef] [PubMed]

C. Radloff and N. J. Halas, “Plasmonic properties of concentric nanoshells,” Nano Lett. 4(7), 1323–1327 (2004).
[CrossRef]

2003 (8)

W. E. Doering and S. Nie, “Spectroscopic tags using dye-embedded nanoparticles and surface-enhanced Raman scattering,” Anal. Chem. 75(22), 6171–6176 (2003).
[CrossRef] [PubMed]

R. Weissleder and V. Ntziachristos, “Shedding light onto live molecular targets,” Nat. Med. 9(1), 123–128 (2003).
[CrossRef] [PubMed]

J. K. Jaiswal, H. Mattoussi, J. M. Mauro, and S. M. Simon, “Long-term multiple color imaging of live cells using quantum dot bioconjugates,” Nat. Biotechnol. 21(1), 47–51 (2003).
[CrossRef]

K. L. Kelly, E. Coronado, L. L. Zhao, and G. C. Schatz, “The optical properties of metal nanoparticles: the influence of size, shape and dielectric environment,” J. Phys. Chem. B 107(3), 668–677 (2003).
[CrossRef]

B. R. Cuenya, S. H. Baeck, T. F. Jaramillo, and E. W. McFarland, “Size- and support-dependent electronic and catalytic properties of Au0/Au3+ nanoparticles synthesized from block copolymer micelles,” J. Am. Chem. Soc. 125(42), 12928–12934 (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]

J. L. West and N. J. Halas, “Engineered nanomaterials for biophotonics applications: improving sensing, imaging, and therapeutics,” Annu. Rev. Biomed. Eng. 5(1), 285–292 (2003).
[CrossRef] [PubMed]

J. B. Jackson, S. L. Westcott, L. R. Hirsch, J. L. West, and N. J. Halas, “Controlling the surface enhanced Raman effect via the nanoshell geometry,” Appl. Phys. Lett. 82(2), 257–259 (2003).
[CrossRef]

2002 (2)

O. Kulakovich, N. Strekal, A. Yaroshevich, S. Maskevich, S. Gaponenko, I. Nabiev, U. Woggon, and M. Artemyev, “Enhanced luminescence of CdSe quantum dots on gold colloids,” Nano Lett. 2(12), 1449–1452 (2002).
[CrossRef]

T. A. Taton, “Nanostructures as tailored biological probes,” Trends Biotechnol. 20(7), 277–279 (2002).
[CrossRef] [PubMed]

2001 (1)

M. Y. Han, X. H. Gao, J. Z. Su, and S. M. Nie, “Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules,” Nat. Biotechnol. 19(7), 631–635 (2001).
[CrossRef] [PubMed]

2000 (2)

S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, “Single-target molecule detection with nonbleaching multicolor optical immunolabels,” Proc. Natl. Acad. Sci. U.S.A. 97(3), 996–1001 (2000).
[CrossRef] [PubMed]

M. B. Mohamed, V. Volkov, S. Link, and M. A. El-Sayed, “The ‘lightning’ gold nanorods: fluorescence enhancement of over a million compared to the gold metal,” Chem. Phys. Lett. 317(6), 517–523 (2000).
[CrossRef]

1999 (1)

R. D. Averitt, S. L. Westcott, and N. J. Halas, “Linear optical properties of gold nanoshells,” J. Opt. Soc. Am. A 16(10), 1824–1832 (1999).
[CrossRef]

1998 (1)

S. J. Oldenburg, R. D. Averitt, S. L. Westcott, and N. J. Halas, “Nanoengineering of optical resonances,” Chem. Phys. Lett. 288(2-4), 243–247 (1998).
[CrossRef]

1997 (1)

J. B. Randolph and A. S. Waggoner, “Stability, specificity and fluorescence brightness of multiply-labeled fluorescent DNA probes,” Nucleic Acids Res. 25(14), 2923–2929 (1997).
[CrossRef] [PubMed]

1996 (1)

1985 (1)

M. Moskovits, “Surface-enhanced spectroscopy,” Rev. Mod. Phys. 57(3), 783–826 (1985).
[CrossRef]

1980 (1)

1951 (1)

A. L. Aden and M. Kerker, “Scattering of electromagnetic waves from two concentric spheres,” J. Appl. Phys. 22(10), 1242–1246 (1951).
[CrossRef]

Aden, A. L.

A. L. Aden and M. Kerker, “Scattering of electromagnetic waves from two concentric spheres,” J. Appl. Phys. 22(10), 1242–1246 (1951).
[CrossRef]

Ameer, G.

K. Chen, Y. Liu, G. Ameer, and V. Backman, “Optimal design of structured nanospheres for ultrasharp light-scattering resonances as molecular imaging multilabels,” J. Biomed. Opt. 10(2), 024005 (2005).
[CrossRef] [PubMed]

Ameer, G. A.

X. Xia, Y. Liu, V. Backman, and G. A. Ameer, “Engineering sub-100 nm multi-layer nanoshells,” Nanotechnology 17(21), 5435–5440 (2006).
[CrossRef]

Angelome, P. C.

B. Sepúlveda, P. C. Angelome, L. M. Lechuga, and L. M. Liz-Marzan, “LSPR-based nanobiosensors,” Nano Today 4(3), 244–251 (2009).
[CrossRef]

Ansari, D. O.

X. Qian, X. H. Peng, D. O. Ansari, Q. Yin-Goen, G. Z. Chen, D. M. Shin, L. Yang, A. N. Young, M. D. Wang, and S. Nie, “In vivo tumor targeting and spectroscopic detection with surface-enhanced Raman nanoparticle tags,” Nat. Biotechnol. 26(1), 83–90 (2008).
[CrossRef]

Arbouet, A.

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[CrossRef] [PubMed]

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A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

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O. Kulakovich, N. Strekal, A. Yaroshevich, S. Maskevich, S. Gaponenko, I. Nabiev, U. Woggon, and M. Artemyev, “Enhanced luminescence of CdSe quantum dots on gold colloids,” Nano Lett. 2(12), 1449–1452 (2002).
[CrossRef]

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R. D. Averitt, S. L. Westcott, and N. J. Halas, “Linear optical properties of gold nanoshells,” J. Opt. Soc. Am. A 16(10), 1824–1832 (1999).
[CrossRef]

S. J. Oldenburg, R. D. Averitt, S. L. Westcott, and N. J. Halas, “Nanoengineering of optical resonances,” Chem. Phys. Lett. 288(2-4), 243–247 (1998).
[CrossRef]

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X. Xia, Y. Liu, V. Backman, and G. A. Ameer, “Engineering sub-100 nm multi-layer nanoshells,” Nanotechnology 17(21), 5435–5440 (2006).
[CrossRef]

K. Chen, Y. Liu, G. Ameer, and V. Backman, “Optimal design of structured nanospheres for ultrasharp light-scattering resonances as molecular imaging multilabels,” J. Biomed. Opt. 10(2), 024005 (2005).
[CrossRef] [PubMed]

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B. R. Cuenya, S. H. Baeck, T. F. Jaramillo, and E. W. McFarland, “Size- and support-dependent electronic and catalytic properties of Au0/Au3+ nanoparticles synthesized from block copolymer micelles,” J. Am. Chem. Soc. 125(42), 12928–12934 (2003).
[CrossRef] [PubMed]

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W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
[CrossRef] [PubMed]

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A. M. Dennis and G. Bao, “Quantum dot-fluorescent protein pairs as novel fluorescence resonance energy transfer probes,” Nano Lett. 8(5), 1439–1445 (2008).
[CrossRef] [PubMed]

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R. Bardhan, S. Mukerjee, N. A. Mirin, S. D. Levit, P. Nordlander, and N. J. Halas, “Nanosphere-in-a-nanoshell: a simple nanomatryushka,” J. Phys. Chem. C 114(16), 7378–7383 (2010).
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X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
[CrossRef] [PubMed]

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A. K. Kodali, X. Llora, and R. Bhargava, “Optimally designed nanolayered metal-dielectric particles as probes for massively multiplexed and ultrasensitive molecular assays,” Proc. Natl. Acad. Sci. U.S.A. 107(31), 13620–13625 (2010).
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A. K. Kodali and R. Bhargava, “Tunable multilayered nanospheres as probes for surface-enahnced Raman spectroscopy,” Proc. SPIE 7032, 70320V (2008).
[CrossRef]

A. K. Kodali, X. Llora, and R. Bhargava, University of Illinois at Urbana Champaign, 405 N Mathews Ave, Urbana, IL are preparing a manuscript to be called “Engineering analytical volumes in and around multilayered nanoshells,”

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A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

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V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
[CrossRef]

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L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
[CrossRef] [PubMed]

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A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
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C. McDonagh, C. S. Burke, and B. D. MacCraith, “Optical chemical sensors,” Chem. Rev. 108(2), 400–422 (2008).
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V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
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U. Resch-Genger, M. Grabolle, S. Cavaliere-Jaricot, R. Nitschke, and T. Nann, “Quantum dots versus organic dyes as fluorescent labels,” Nat. Methods 5(9), 763–775 (2008).
[CrossRef] [PubMed]

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B. D. Chithrani, A. A. Ghazani, and W. C. W. Chan, “Determining the size and shape dependence of gold nanoparticle uptake into mammalian cells,” Nano Lett. 6(4), 662–668 (2006).
[CrossRef] [PubMed]

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Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
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X. Qian, X. H. Peng, D. O. Ansari, Q. Yin-Goen, G. Z. Chen, D. M. Shin, L. Yang, A. N. Young, M. D. Wang, and S. Nie, “In vivo tumor targeting and spectroscopic detection with surface-enhanced Raman nanoparticle tags,” Nat. Biotechnol. 26(1), 83–90 (2008).
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K. Chen, Y. Liu, G. Ameer, and V. Backman, “Optimal design of structured nanospheres for ultrasharp light-scattering resonances as molecular imaging multilabels,” J. Biomed. Opt. 10(2), 024005 (2005).
[CrossRef] [PubMed]

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B. D. Chithrani, A. A. Ghazani, and W. C. W. Chan, “Determining the size and shape dependence of gold nanoparticle uptake into mammalian cells,” Nano Lett. 6(4), 662–668 (2006).
[CrossRef] [PubMed]

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A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

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Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
[CrossRef] [PubMed]

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K. L. Kelly, E. Coronado, L. L. Zhao, and G. C. Schatz, “The optical properties of metal nanoparticles: the influence of size, shape and dielectric environment,” J. Phys. Chem. B 107(3), 668–677 (2003).
[CrossRef]

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B. R. Cuenya, S. H. Baeck, T. F. Jaramillo, and E. W. McFarland, “Size- and support-dependent electronic and catalytic properties of Au0/Au3+ nanoparticles synthesized from block copolymer micelles,” J. Am. Chem. Soc. 125(42), 12928–12934 (2003).
[CrossRef] [PubMed]

Del Fatti, N.

A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

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A. M. Dennis and G. Bao, “Quantum dot-fluorescent protein pairs as novel fluorescence resonance energy transfer probes,” Nano Lett. 8(5), 1439–1445 (2008).
[CrossRef] [PubMed]

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L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
[CrossRef] [PubMed]

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Y. Fang, N. H. Seong, and D. D. Dlott, “Measurement of the distribution of site enhancements in surface-enhanced Raman scattering,” Science 321(5887), 388–392 (2008).
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W. E. Doering and S. Nie, “Spectroscopic tags using dye-embedded nanoparticles and surface-enhanced Raman scattering,” Anal. Chem. 75(22), 6171–6176 (2003).
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X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
[CrossRef] [PubMed]

Drake, T.

W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
[CrossRef] [PubMed]

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C. Loo, A. Lowery, N. J. Halas, J. L. West, and R. Drezek, “Immunotargeted nanoshells for integrated cancer imaging and therapy,” Nano Lett. 5(4), 709–711 (2005).
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[CrossRef]

El-Sayed, M. A.

P. K. Jain, X. Huang, I. H. El-Sayed, and M. A. El-Sayed, “Review of some interesting surface plasmon resonance-enhanced properties of noble metal nanoparticles and their applications to biosystems,” Plasmonics 2(3), 107–118 (2007).
[CrossRef]

M. B. Mohamed, V. Volkov, S. Link, and M. A. El-Sayed, “The ‘lightning’ gold nanorods: fluorescence enhancement of over a million compared to the gold metal,” Chem. Phys. Lett. 317(6), 517–523 (2000).
[CrossRef]

Fang, Y.

Y. Fang, N. H. Seong, and D. D. Dlott, “Measurement of the distribution of site enhancements in surface-enhanced Raman scattering,” Science 321(5887), 388–392 (2008).
[CrossRef] [PubMed]

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L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
[CrossRef] [PubMed]

Fleming, R. C.

Gambhir, S. S.

X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
[CrossRef] [PubMed]

Gao, X. H.

M. Y. Han, X. H. Gao, J. Z. Su, and S. M. Nie, “Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules,” Nat. Biotechnol. 19(7), 631–635 (2001).
[CrossRef] [PubMed]

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O. Kulakovich, N. Strekal, A. Yaroshevich, S. Maskevich, S. Gaponenko, I. Nabiev, U. Woggon, and M. Artemyev, “Enhanced luminescence of CdSe quantum dots on gold colloids,” Nano Lett. 2(12), 1449–1452 (2002).
[CrossRef]

Geschwender, A. S-.

V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
[CrossRef]

Ghazani, A. A.

B. D. Chithrani, A. A. Ghazani, and W. C. W. Chan, “Determining the size and shape dependence of gold nanoparticle uptake into mammalian cells,” Nano Lett. 6(4), 662–668 (2006).
[CrossRef] [PubMed]

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C. L. Nehl, N. K. Grady, G. P. Goodrich, F. Tam, N. J. Halas, and J. H. Hafner, “Scattering spectra of single gold nanoshells,” Nano Lett. 4(12), 2355–2359 (2004).
[CrossRef]

Grabolle, M.

U. Resch-Genger, M. Grabolle, S. Cavaliere-Jaricot, R. Nitschke, and T. Nann, “Quantum dots versus organic dyes as fluorescent labels,” Nat. Methods 5(9), 763–775 (2008).
[CrossRef] [PubMed]

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C. L. Nehl, N. K. Grady, G. P. Goodrich, F. Tam, N. J. Halas, and J. H. Hafner, “Scattering spectra of single gold nanoshells,” Nano Lett. 4(12), 2355–2359 (2004).
[CrossRef]

Gryczynski, I.

J. Zhang, J. Malicka, I. Gryczynski, and J. R. Lakowicz, “Surface-enhanced fluorescence of fluorescein-labeled oligonucleotides capped on silver nanoparticles,” J. Phys. Chem. B 109(16), 7643–7648 (2005).
[CrossRef]

Hafner, J. H.

C. L. Nehl, N. K. Grady, G. P. Goodrich, F. Tam, N. J. Halas, and J. H. Hafner, “Scattering spectra of single gold nanoshells,” Nano Lett. 4(12), 2355–2359 (2004).
[CrossRef]

Halas, N. J.

R. Bardhan, S. Mukerjee, N. A. Mirin, S. D. Levit, P. Nordlander, and N. J. Halas, “Nanosphere-in-a-nanoshell: a simple nanomatryushka,” J. Phys. Chem. C 114(16), 7378–7383 (2010).
[CrossRef]

J. Kundu, F. Le, P. Nordlander, and N. J. Halas, “Surface enhanced infrared absorption (SEIRA) spectroscopy on nanoshell aggregate substrates,” Chem. Phys. Lett. 452(1-3), 115–119 (2008).
[CrossRef]

C. Loo, A. Lowery, N. J. Halas, J. L. West, and R. Drezek, “Immunotargeted nanoshells for integrated cancer imaging and therapy,” Nano Lett. 5(4), 709–711 (2005).
[CrossRef] [PubMed]

C. Radloff and N. J. Halas, “Plasmonic properties of concentric nanoshells,” Nano Lett. 4(7), 1323–1327 (2004).
[CrossRef]

C. L. Nehl, N. K. Grady, G. P. Goodrich, F. Tam, N. J. Halas, and J. H. Hafner, “Scattering spectra of single gold nanoshells,” Nano Lett. 4(12), 2355–2359 (2004).
[CrossRef]

J. B. Jackson, S. L. Westcott, L. R. Hirsch, J. L. West, and N. J. Halas, “Controlling the surface enhanced Raman effect via the nanoshell geometry,” Appl. Phys. Lett. 82(2), 257–259 (2003).
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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).
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J. L. West and N. J. Halas, “Engineered nanomaterials for biophotonics applications: improving sensing, imaging, and therapeutics,” Annu. Rev. Biomed. Eng. 5(1), 285–292 (2003).
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R. D. Averitt, S. L. Westcott, and N. J. Halas, “Linear optical properties of gold nanoshells,” J. Opt. Soc. Am. A 16(10), 1824–1832 (1999).
[CrossRef]

S. J. Oldenburg, R. D. Averitt, S. L. Westcott, and N. J. Halas, “Nanoengineering of optical resonances,” Chem. Phys. Lett. 288(2-4), 243–247 (1998).
[CrossRef]

Han, M. Y.

M. Y. Han, X. H. Gao, J. Z. Su, and S. M. Nie, “Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules,” Nat. Biotechnol. 19(7), 631–635 (2001).
[CrossRef] [PubMed]

He, X.

W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
[CrossRef] [PubMed]

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J. B. Jackson, S. L. Westcott, L. R. Hirsch, J. L. West, and N. J. Halas, “Controlling the surface enhanced Raman effect via the nanoshell geometry,” Appl. Phys. Lett. 82(2), 257–259 (2003).
[CrossRef]

Hu, Y.

Huang, X.

P. K. Jain, X. Huang, I. H. El-Sayed, and M. A. El-Sayed, “Review of some interesting surface plasmon resonance-enhanced properties of noble metal nanoparticles and their applications to biosystems,” Plasmonics 2(3), 107–118 (2007).
[CrossRef]

Huntzinger, J. R.

A. Arbouet, D. Christofilos, N. Del Fatti, F. Vallée, J. R. Huntzinger, L. Arnaud, P. Billaud, and M. Broyer, “Direct measurement of the single-metal-cluster optical absorption,” Phys. Rev. Lett. 93(12), 127401 (2004).
[CrossRef] [PubMed]

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J. B. Jackson, S. L. Westcott, L. R. Hirsch, J. L. West, and N. J. Halas, “Controlling the surface enhanced Raman effect via the nanoshell geometry,” Appl. Phys. Lett. 82(2), 257–259 (2003).
[CrossRef]

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P. K. Jain, X. Huang, I. H. El-Sayed, and M. A. El-Sayed, “Review of some interesting surface plasmon resonance-enhanced properties of noble metal nanoparticles and their applications to biosystems,” Plasmonics 2(3), 107–118 (2007).
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J. K. Jaiswal, H. Mattoussi, J. M. Mauro, and S. M. Simon, “Long-term multiple color imaging of live cells using quantum dot bioconjugates,” Nat. Biotechnol. 21(1), 47–51 (2003).
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B. R. Cuenya, S. H. Baeck, T. F. Jaramillo, and E. W. McFarland, “Size- and support-dependent electronic and catalytic properties of Au0/Au3+ nanoparticles synthesized from block copolymer micelles,” J. Am. Chem. Soc. 125(42), 12928–12934 (2003).
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K. L. Kelly, E. Coronado, L. L. Zhao, and G. C. Schatz, “The optical properties of metal nanoparticles: the influence of size, shape and dielectric environment,” J. Phys. Chem. B 107(3), 668–677 (2003).
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B. Khlebtsov and N. Khlebtsov, “Ultrasharp light-scattering resonances of structured nanospheres: effects of size-dependent dielectric functions,” J. Biomed. Opt. 11(4), 044002 (2006).
[CrossRef] [PubMed]

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A. K. Kodali, X. Llora, and R. Bhargava, “Optimally designed nanolayered metal-dielectric particles as probes for massively multiplexed and ultrasensitive molecular assays,” Proc. Natl. Acad. Sci. U.S.A. 107(31), 13620–13625 (2010).
[CrossRef] [PubMed]

A. K. Kodali and R. Bhargava, “Tunable multilayered nanospheres as probes for surface-enahnced Raman spectroscopy,” Proc. SPIE 7032, 70320V (2008).
[CrossRef]

A. K. Kodali, X. Llora, and R. Bhargava, University of Illinois at Urbana Champaign, 405 N Mathews Ave, Urbana, IL are preparing a manuscript to be called “Engineering analytical volumes in and around multilayered nanoshells,”

Kong, K. Y.

Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
[CrossRef] [PubMed]

Kulakovich, O.

O. Kulakovich, N. Strekal, A. Yaroshevich, S. Maskevich, S. Gaponenko, I. Nabiev, U. Woggon, and M. Artemyev, “Enhanced luminescence of CdSe quantum dots on gold colloids,” Nano Lett. 2(12), 1449–1452 (2002).
[CrossRef]

Kundu, J.

J. Kundu, F. Le, P. Nordlander, and N. J. Halas, “Surface enhanced infrared absorption (SEIRA) spectroscopy on nanoshell aggregate substrates,” Chem. Phys. Lett. 452(1-3), 115–119 (2008).
[CrossRef]

Lakowicz, J. R.

J. Zhang, J. Malicka, I. Gryczynski, and J. R. Lakowicz, “Surface-enhanced fluorescence of fluorescein-labeled oligonucleotides capped on silver nanoparticles,” J. Phys. Chem. B 109(16), 7643–7648 (2005).
[CrossRef]

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J. Kundu, F. Le, P. Nordlander, and N. J. Halas, “Surface enhanced infrared absorption (SEIRA) spectroscopy on nanoshell aggregate substrates,” Chem. Phys. Lett. 452(1-3), 115–119 (2008).
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R. Bardhan, S. Mukerjee, N. A. Mirin, S. D. Levit, P. Nordlander, and N. J. Halas, “Nanosphere-in-a-nanoshell: a simple nanomatryushka,” J. Phys. Chem. C 114(16), 7378–7383 (2010).
[CrossRef]

Li, J. J.

X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
[CrossRef] [PubMed]

Link, S.

M. B. Mohamed, V. Volkov, S. Link, and M. A. El-Sayed, “The ‘lightning’ gold nanorods: fluorescence enhancement of over a million compared to the gold metal,” Chem. Phys. Lett. 317(6), 517–523 (2000).
[CrossRef]

Liotta, L. A.

V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
[CrossRef]

Liu, Y.

X. Xia, Y. Liu, V. Backman, and G. A. Ameer, “Engineering sub-100 nm multi-layer nanoshells,” Nanotechnology 17(21), 5435–5440 (2006).
[CrossRef]

K. Chen, Y. Liu, G. Ameer, and V. Backman, “Optimal design of structured nanospheres for ultrasharp light-scattering resonances as molecular imaging multilabels,” J. Biomed. Opt. 10(2), 024005 (2005).
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L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
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S. Schultz, D. R. Smith, J. J. Mock, and D. A. Schultz, “Single-target molecule detection with nonbleaching multicolor optical immunolabels,” Proc. Natl. Acad. Sci. U.S.A. 97(3), 996–1001 (2000).
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Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
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X. Qian, X. H. Peng, D. O. Ansari, Q. Yin-Goen, G. Z. Chen, D. M. Shin, L. Yang, A. N. Young, M. D. Wang, and S. Nie, “In vivo tumor targeting and spectroscopic detection with surface-enhanced Raman nanoparticle tags,” Nat. Biotechnol. 26(1), 83–90 (2008).
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J. K. Jaiswal, H. Mattoussi, J. M. Mauro, and S. M. Simon, “Long-term multiple color imaging of live cells using quantum dot bioconjugates,” Nat. Biotechnol. 21(1), 47–51 (2003).
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Y. Xing, Q. Chaudry, C. Shen, K. Y. Kong, H. E. Zhau, L. W. Chung, J. A. Petros, R. M. O’Regan, M. V. Yezhelyev, J. W. Simons, M. D. Wang, and S. Nie, “Bioconjugated quantum dots for multiplexed and quantitative immunohistochemistry,” Nat. Protoc. 2(5), 1152–1165 (2007).
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M. Y. Han, X. H. Gao, J. Z. Su, and S. M. Nie, “Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules,” Nat. Biotechnol. 19(7), 631–635 (2001).
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W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
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W. Tan, K. Wang, X. He, X. J. Zhao, T. Drake, L. Wang, and R. P. Bagwe, “Bionanotechnology based on silica nanoparticles,” Med. Res. Rev. 24(5), 621–638 (2004).
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X. Qian, X. H. Peng, D. O. Ansari, Q. Yin-Goen, G. Z. Chen, D. M. Shin, L. Yang, A. N. Young, M. D. Wang, and S. Nie, “In vivo tumor targeting and spectroscopic detection with surface-enhanced Raman nanoparticle tags,” Nat. Biotechnol. 26(1), 83–90 (2008).
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H. Xu, X. H. Wang, M. P. Persson, H. Q. Xu, M. Käll, and P. Johansson, “Unified treatment of fluorescence and raman scattering processes near metal surfaces,” Phys. Rev. Lett. 93(24), 243002 (2004).
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L. A. Swafford, L. A. Weigand, M. J. Bowers, J. R. McBride, J. L. Rapaport, T. L. Watt, S. K. Dixit, L. C. Feldman, and S. J. Rosenthal, “Homogeneously alloyed CdSxSe1-x nanocrystals: synthesis, characterization, and composition/size-dependent band gap,” J. Am. Chem. Soc. 128(37), 12299–12306 (2006).
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O. Kulakovich, N. Strekal, A. Yaroshevich, S. Maskevich, S. Gaponenko, I. Nabiev, U. Woggon, and M. Artemyev, “Enhanced luminescence of CdSe quantum dots on gold colloids,” Nano Lett. 2(12), 1449–1452 (2002).
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X. Michalet, F. F. Pinaud, L. A. Bentolila, J. M. Tsay, S. Doose, J. J. Li, G. Sundaresan, A. M. Wu, S. S. Gambhir, and S. Weiss, “Quantum dots for live cells, in vivo imaging, and diagnostics,” Science 307(5709), 538–544 (2005).
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V. S. Calvert, Y. Tang, V. Boveia, J. Wulfkuhle, A. S-. Geschwender, D. M. Olive, L. A. Liotta, and E. F. Petricoin III, “Development of multiplexed protein profiling and detection using near infrared detection of reverse-phase protein microarrays,” Clin. Proteomics 1, 81–89 (2004).
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Figures (6)

Fig. 1
Fig. 1

Probe Structure, far-field and near-field characteristics of nano-LAMPs. (a) LAMPs with linkers can label analyte molecules and the response of the probe to an incident electro-magnetic field can be used for detection. (b) Mid-sectional view of odd- and even-layered LAMP configurations (c) Extinction efficiencies for gold-silica LAMPs consisting of 5 layers ({r1, r2, r3, r4, r5} = {5, 15, 30, 44, 50 nm}) and 6 layers ({r1, r2, r3, r4, r5, r6} = {5, 10, 26, 34, 44, 50 nm}). (d) Internal intensity distribution in the incident plane for 5-layered (top) and 6-layered (bottom) LAMPs in (c) when illuminated by plane waves at resonant wavelengths. The boundaries of different layers are indicated using black circles.

Fig. 2
Fig. 2

Odd-layered Silver-Silica LAMPs of 100 nm size with distinct extinction spectra in 200-1200 nm excitation range. (a) 3-layered LAMPs (b) 5-layered LAMPs.

Fig. 3
Fig. 3

Even-layered Silver-Silica LAMPs of 100 nm size with extinction spectra in 200-1200 nm excitation range. (a) 4-layered LAMPs (b) 6-layered LAMPs.

Fig. 4
Fig. 4

The tunability of enhancement in the internal fields in dielectric layers using 100 nm sized six-layered gold-silica LAMPs of various layer thicknesses when illuminated by a plane wave of wavelength 785 nm. The distributions are shown in the indicent plane with incident field polarized horizontally. The structures shown have radii (a) 5,14,16,17,48,50 nm, (b) 7,17,20,21,44,50 nm, (c) 8,23,25,26,35,50 nm (d) 6,18,23,26,31,50 nm (e) 15,25,32,36,40,50 nm (f)13,20,25,35,40,50 nm (g) 10,14,22,32,41,50 nm (h) 18,22,33,38,41,50 nm (i) 14,16,28,34,46,50 nm (j) 7,8,26,38,48,50 nm. The boundaries of different layers are depicted using black lines.

Fig. 5
Fig. 5

Internal field distributions in 60 nm sized six-layered Gold-Silica LAMPs ((a) and (b)) and Copper-Silica LAMPs((c) and (d)) designed for minimal and maximal enhancements at excitation wavelengths 532 nm ((a) and (c)) and 785 nm ((b) and (d)). The distributions are shown in the incident plane with incident field polarized horizontally. The structures shown have radii (a) minimal-left:{5,7,9,10,12,30 nm}, maximal-right: {5,9,13,17,28,30 nm} (b) minimal-left: {5,11,13,14,26,30 nm}, maximal-right: {7,8,18,24,29,30 nm} (c) minimal-left: {5,6,8,10,12,30 nm}, maximal-right: {6,7,13,19,29,30 nm} (d) minimal-left: {6,12,14,15,27,30 nm}, maximal-right: {7,8,18,24,29,30 nm}. The boundaries of different layers are depicted using black circles.

Fig. 6
Fig. 6

Dynamic range of achievable Raman Net Enhancement Factors using Gold-Silica and Copper-Silica LAMPs of different sizes over different number of layers for excitation wavelengths (a) 532 nm and (b) 785 nm. The data points plotted are connected by smooth piece-wise cubic interpolation.

Equations (1)

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N E F = | E l o c ( λ + δ λ ) | 2 | E l o c ( λ ) | 2 c r d V

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