Abstract

We present a method to perform hyper Rayleigh scattering from aqueous solutions and second harmonic scattering measurements from unlabeled interfaces of liposomes and nanoparticles in dilute solutions. The water and interfacial response can be measured on a millisecond timescale, thus opening up the possibility to measure label-free time dependent transport processes in biological (membrane) systems.

©2013 Optical Society of America

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  1. J. E. Rothman, “Mechanisms of intracellular protein transport,” Nature 372(6501), 55–63 (1994).
    [Crossref] [PubMed]
  2. S. M. Butterfield and H. A. Lashuel, “Amyloidogenic Protein-Membrane Interactions: Mechanistic Insight from Model Systems,” Angew. Chem. Int. Ed. Engl. 49(33), 5628–5654 (2010).
    [Crossref] [PubMed]
  3. D. S. Peterka, H. Takahashi, and R. Yuste, “Imaging Voltage in Neurons,” Neuron 69(1), 9–21 (2011).
    [Crossref] [PubMed]
  4. T. F. Heinz, C. K. Chen, D. Ricard, and Y. Shen, “Spectroscopy of Molecular Monolayers by Resonant Second-Harmonic Generation,” Phys. Rev. Lett. 48(7), 478–481 (1982).
    [Crossref]
  5. S. Roke, “Nonlinear optical spectroscopy of soft matter interfaces,” ChemPhysChem 10(9-10), 1380–1388 (2009).
    [Crossref] [PubMed]
  6. R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14(17), 681–684 (1965).
    [Crossref]
  7. R. Bersohn, Y. H. Pao, and H. L. Frisch, “Double-Quantum Light Scattering by Molecules,” J. Chem. Phys. 45(9), 3184–3198 (1966).
    [Crossref]
  8. M. Kauranen and A. Persoons, “Theory of polarization measurements of second-order nonlinear light scattering,” J. Chem. Phys. 104(10), 3445–3456 (1996).
    [Crossref]
  9. D. P. Shelton, “Polarization and angle dependence for hyper-Rayleigh scattering from local and nonlocal modes of isotropic fluids,” J. Opt. Soc. Am. B 17(12), 2032–2036 (2000).
    [Crossref]
  10. D. P. Shelton, “Accurate hyper-Rayleigh scattering polarization measurements,” Rev. Sci. Instrum. 82(11), 113103 (2011).
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  11. K. Clays, M. J. Therien, and G. Hennrich, “Hyper-Rayleigh scattering for solution phase structure determination,” Linear and Nonlinear Optics of Organic Materials Viii 7049 (2008).
  12. S. Roke and G. Gonella, “Nonlinear Light Scattering and Spectroscopy of Particles and Droplets in Liquids,” Annu. Rev. Phys. Chem. 63(1), 353–378 (2012).
    [Crossref] [PubMed]
  13. H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, “Second harmonic generation from the surface of centrosymmetric particles in bulk solution,” Chem. Phys. Lett. 259(1-2), 15–20 (1996).
    [Crossref]
  14. K. B. Eisenthal, “Second harmonic spectroscopy of aqueous nano- and microparticle interfaces,” Chem. Rev. 106(4), 1462–1477 (2006).
    [Crossref] [PubMed]
  15. L. Schneider, H. J. Schmid, and W. Peukert, “Influence of particle size and concentration on the second-harmonic signal generated at colloidal surfaces,” Appl. Phys. B 87(2), 333–339 (2007).
    [Crossref]
  16. S. Roke, W. G. Roeterdink, J. E. G. J. Wijnhoven, A. V. Petukhov, A. W. Kleyn, and M. Bonn, “Vibrational sum frequency scattering from a submicron suspension,” Phys. Rev. Lett. 91(25), 258302 (2003).
    [Crossref] [PubMed]
  17. S. H. Jen, G. Gonella, and H. L. Dai, “The Effect of Particle Size in Second Harmonic Generation from the Surface of Spherical Colloidal Particles. I: Experimental Observations,” J. Phys. Chem. A 113(16), 4758–4762 (2009).
    [Crossref] [PubMed]
  18. J. I. Dadap, J. Shan, and T. F. Heinz, “Theory of optical second-harmonic generation from a sphere of centrosymmetric material: small-particle limit,” J. Opt. Soc. Am. B 21(7), 1328–1347 (2004).
    [Crossref]
  19. A. G. F. de Beer, S. Roke, and J. I. Dadap, “Theory of optical second-harmonic and sum-frequency scattering from arbitrarily shaped particles,” J. Opt. Soc. Am. B 28(6), 1374–1384 (2011).
    [Crossref]
  20. G. Gonella and H. L. Dai, “Determination of adsorption geometry on spherical particles from nonlinear Mie theory analysis of surface second harmonic generation,” Phys. Rev. B 84(12), 121402 (2011).
    [Crossref]
  21. H. Husu, R. Siikanen, J. Mäkitalo, J. Lehtolahti, J. Laukkanen, M. Kuittinen, and M. Kauranen, “Metamaterials with Tailored Nonlinear Optical Response,” Nano Lett. 12(2), 673–677 (2012).
    [Crossref] [PubMed]
  22. J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
    [Crossref] [PubMed]
  23. Y. Liu, C. Y. Yan, X. L. Zhao, and K. B. Eisenthal, “Surface potential of charged liposomes determined by second harmonic generation,” Langmuir 17(7), 2063–2066 (2001).
    [Crossref]
  24. M. Subir, J. Liu, and K. B. Eisenthal, “Protonation at the Aqueous Interface of Polymer Nanoparticles with Second Harmonic Generation,” J. Phys. Chem. C 112(40), 15809–15812 (2008).
    [Crossref]
  25. B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
    [Crossref]
  26. S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
    [Crossref]
  27. H. F. Wang, T. Troxler, A. G. Yeh, and H. L. Dai, “In Situ, Nonlinear Optical Probe of Surfactant Adsorption on the Surface of Microparticles in Colloids,” Langmuir 16(6), 2475–2481 (2000).
    [Crossref]
  28. H. M. Eckenrode and H. L. Dai, “Nonlinear optical probe of biopolymer adsorption on colloidal particle surface: poly-L-lysine on polystyrene sulfate microspheres,” Langmuir 20(21), 9202–9209 (2004).
    [Crossref] [PubMed]
  29. H. M. Eckenrode, S. H. Jen, J. Han, A. G. Yeh, and H. L. Dai, “Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: Effect of surface charge and composition probed by second harmonic generation,” J. Phys. Chem. B 109(10), 4646–4653 (2005).
    [Crossref] [PubMed]
  30. J. I. Dadap, X. Hu, N. Russell, J. Ekerdt, J. Lowell, and M. Downer, “Analysis of second-harmonic generation by unamplified, high-repetition-rate, ultrashort laser pulses at Si(001) interfaces,” IEEE J. Sel. Top. Quantum Electron. 1(4), 1145–1155 (1995).
    [Crossref]
  31. Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
    [Crossref] [PubMed]
  32. D. P. Shelton, “Slow polarization relaxation in water observed by hyper-Rayleigh scattering,” Phys. Rev. B 72(2), 020201 (2005).
    [Crossref]
  33. L. Haber, S. J. J. Kwok, M. Semeraro, and K. B. Eisenthal, “Probing the colloidal gold nanoparticle/aqueous interface with second harmonic generation,” Chem. Phys. Lett. 507(1-3), 11–14 (2011).
    [Crossref]
  34. J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
    [Crossref] [PubMed]
  35. Handbook of Biomedical Nonlinear Optical Microscopy (Oxford Univeristy Press, Oxford, 2008).
  36. K. Kuetemeyer, R. Rezgui, H. Lubatschowski, and A. Heisterkamp, “Influence of laser parameters and staining on femtosecond laser-based intracellular nanosurgery,” Biomed. Opt. Express 1(2), 587–597 (2010).
    [Crossref] [PubMed]
  37. D. O. Lapotko and E. Y. Lukianova, “Influence of Physiological Conditions on Laser Damage Thresholds for Blood, Heart, and Liver Cells,” Lasers Surg. Med. 36(1), 13–21 (2005).
    [Crossref] [PubMed]
  38. K. König, “Multiphoton microscopy in life sciences,” J. Microsc. 200(2), 83–104 (2000).
    [Crossref] [PubMed]
  39. A. Vogel, N. Linz, S. Freidank, and G. Paltauf, “Femtosecond-Laser-Induced Nanocavitation in Water: Implications for Optical Breakdown Threshold and Cell Surgery,” Phys. Rev. Lett. 100(3), 038102 (2008).
    [Crossref] [PubMed]
  40. D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
    [Crossref] [PubMed]

2012 (4)

S. Roke and G. Gonella, “Nonlinear Light Scattering and Spectroscopy of Particles and Droplets in Liquids,” Annu. Rev. Phys. Chem. 63(1), 353–378 (2012).
[Crossref] [PubMed]

H. Husu, R. Siikanen, J. Mäkitalo, J. Lehtolahti, J. Laukkanen, M. Kuittinen, and M. Kauranen, “Metamaterials with Tailored Nonlinear Optical Response,” Nano Lett. 12(2), 673–677 (2012).
[Crossref] [PubMed]

J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
[Crossref] [PubMed]

Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
[Crossref] [PubMed]

2011 (5)

L. Haber, S. J. J. Kwok, M. Semeraro, and K. B. Eisenthal, “Probing the colloidal gold nanoparticle/aqueous interface with second harmonic generation,” Chem. Phys. Lett. 507(1-3), 11–14 (2011).
[Crossref]

D. P. Shelton, “Accurate hyper-Rayleigh scattering polarization measurements,” Rev. Sci. Instrum. 82(11), 113103 (2011).
[Crossref] [PubMed]

G. Gonella and H. L. Dai, “Determination of adsorption geometry on spherical particles from nonlinear Mie theory analysis of surface second harmonic generation,” Phys. Rev. B 84(12), 121402 (2011).
[Crossref]

D. S. Peterka, H. Takahashi, and R. Yuste, “Imaging Voltage in Neurons,” Neuron 69(1), 9–21 (2011).
[Crossref] [PubMed]

A. G. F. de Beer, S. Roke, and J. I. Dadap, “Theory of optical second-harmonic and sum-frequency scattering from arbitrarily shaped particles,” J. Opt. Soc. Am. B 28(6), 1374–1384 (2011).
[Crossref]

2010 (3)

K. Kuetemeyer, R. Rezgui, H. Lubatschowski, and A. Heisterkamp, “Influence of laser parameters and staining on femtosecond laser-based intracellular nanosurgery,” Biomed. Opt. Express 1(2), 587–597 (2010).
[Crossref] [PubMed]

S. M. Butterfield and H. A. Lashuel, “Amyloidogenic Protein-Membrane Interactions: Mechanistic Insight from Model Systems,” Angew. Chem. Int. Ed. Engl. 49(33), 5628–5654 (2010).
[Crossref] [PubMed]

B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
[Crossref]

2009 (2)

S. Roke, “Nonlinear optical spectroscopy of soft matter interfaces,” ChemPhysChem 10(9-10), 1380–1388 (2009).
[Crossref] [PubMed]

S. H. Jen, G. Gonella, and H. L. Dai, “The Effect of Particle Size in Second Harmonic Generation from the Surface of Spherical Colloidal Particles. I: Experimental Observations,” J. Phys. Chem. A 113(16), 4758–4762 (2009).
[Crossref] [PubMed]

2008 (3)

M. Subir, J. Liu, and K. B. Eisenthal, “Protonation at the Aqueous Interface of Polymer Nanoparticles with Second Harmonic Generation,” J. Phys. Chem. C 112(40), 15809–15812 (2008).
[Crossref]

J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
[Crossref] [PubMed]

A. Vogel, N. Linz, S. Freidank, and G. Paltauf, “Femtosecond-Laser-Induced Nanocavitation in Water: Implications for Optical Breakdown Threshold and Cell Surgery,” Phys. Rev. Lett. 100(3), 038102 (2008).
[Crossref] [PubMed]

2007 (1)

L. Schneider, H. J. Schmid, and W. Peukert, “Influence of particle size and concentration on the second-harmonic signal generated at colloidal surfaces,” Appl. Phys. B 87(2), 333–339 (2007).
[Crossref]

2006 (1)

K. B. Eisenthal, “Second harmonic spectroscopy of aqueous nano- and microparticle interfaces,” Chem. Rev. 106(4), 1462–1477 (2006).
[Crossref] [PubMed]

2005 (4)

D. P. Shelton, “Slow polarization relaxation in water observed by hyper-Rayleigh scattering,” Phys. Rev. B 72(2), 020201 (2005).
[Crossref]

D. O. Lapotko and E. Y. Lukianova, “Influence of Physiological Conditions on Laser Damage Thresholds for Blood, Heart, and Liver Cells,” Lasers Surg. Med. 36(1), 13–21 (2005).
[Crossref] [PubMed]

H. M. Eckenrode, S. H. Jen, J. Han, A. G. Yeh, and H. L. Dai, “Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: Effect of surface charge and composition probed by second harmonic generation,” J. Phys. Chem. B 109(10), 4646–4653 (2005).
[Crossref] [PubMed]

S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
[Crossref]

2004 (2)

H. M. Eckenrode and H. L. Dai, “Nonlinear optical probe of biopolymer adsorption on colloidal particle surface: poly-L-lysine on polystyrene sulfate microspheres,” Langmuir 20(21), 9202–9209 (2004).
[Crossref] [PubMed]

J. I. Dadap, J. Shan, and T. F. Heinz, “Theory of optical second-harmonic generation from a sphere of centrosymmetric material: small-particle limit,” J. Opt. Soc. Am. B 21(7), 1328–1347 (2004).
[Crossref]

2003 (1)

S. Roke, W. G. Roeterdink, J. E. G. J. Wijnhoven, A. V. Petukhov, A. W. Kleyn, and M. Bonn, “Vibrational sum frequency scattering from a submicron suspension,” Phys. Rev. Lett. 91(25), 258302 (2003).
[Crossref] [PubMed]

2001 (1)

Y. Liu, C. Y. Yan, X. L. Zhao, and K. B. Eisenthal, “Surface potential of charged liposomes determined by second harmonic generation,” Langmuir 17(7), 2063–2066 (2001).
[Crossref]

2000 (3)

H. F. Wang, T. Troxler, A. G. Yeh, and H. L. Dai, “In Situ, Nonlinear Optical Probe of Surfactant Adsorption on the Surface of Microparticles in Colloids,” Langmuir 16(6), 2475–2481 (2000).
[Crossref]

K. König, “Multiphoton microscopy in life sciences,” J. Microsc. 200(2), 83–104 (2000).
[Crossref] [PubMed]

D. P. Shelton, “Polarization and angle dependence for hyper-Rayleigh scattering from local and nonlocal modes of isotropic fluids,” J. Opt. Soc. Am. B 17(12), 2032–2036 (2000).
[Crossref]

1999 (1)

D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
[Crossref] [PubMed]

1996 (2)

H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, “Second harmonic generation from the surface of centrosymmetric particles in bulk solution,” Chem. Phys. Lett. 259(1-2), 15–20 (1996).
[Crossref]

M. Kauranen and A. Persoons, “Theory of polarization measurements of second-order nonlinear light scattering,” J. Chem. Phys. 104(10), 3445–3456 (1996).
[Crossref]

1995 (1)

J. I. Dadap, X. Hu, N. Russell, J. Ekerdt, J. Lowell, and M. Downer, “Analysis of second-harmonic generation by unamplified, high-repetition-rate, ultrashort laser pulses at Si(001) interfaces,” IEEE J. Sel. Top. Quantum Electron. 1(4), 1145–1155 (1995).
[Crossref]

1994 (1)

J. E. Rothman, “Mechanisms of intracellular protein transport,” Nature 372(6501), 55–63 (1994).
[Crossref] [PubMed]

1982 (1)

T. F. Heinz, C. K. Chen, D. Ricard, and Y. Shen, “Spectroscopy of Molecular Monolayers by Resonant Second-Harmonic Generation,” Phys. Rev. Lett. 48(7), 478–481 (1982).
[Crossref]

1966 (1)

R. Bersohn, Y. H. Pao, and H. L. Frisch, “Double-Quantum Light Scattering by Molecules,” J. Chem. Phys. 45(9), 3184–3198 (1966).
[Crossref]

1965 (1)

R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14(17), 681–684 (1965).
[Crossref]

Benichou, E.

J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
[Crossref] [PubMed]

Bersohn, R.

R. Bersohn, Y. H. Pao, and H. L. Frisch, “Double-Quantum Light Scattering by Molecules,” J. Chem. Phys. 45(9), 3184–3198 (1966).
[Crossref]

Bonn, M.

S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
[Crossref]

S. Roke, W. G. Roeterdink, J. E. G. J. Wijnhoven, A. V. Petukhov, A. W. Kleyn, and M. Bonn, “Vibrational sum frequency scattering from a submicron suspension,” Phys. Rev. Lett. 91(25), 258302 (2003).
[Crossref] [PubMed]

Borguet, E.

H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, “Second harmonic generation from the surface of centrosymmetric particles in bulk solution,” Chem. Phys. Lett. 259(1-2), 15–20 (1996).
[Crossref]

Brevet, P. F.

J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
[Crossref] [PubMed]

Buitenhuis, J.

S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
[Crossref]

Butet, J.

J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
[Crossref] [PubMed]

Butterfield, S. M.

S. M. Butterfield and H. A. Lashuel, “Amyloidogenic Protein-Membrane Interactions: Mechanistic Insight from Model Systems,” Angew. Chem. Int. Ed. Engl. 49(33), 5628–5654 (2010).
[Crossref] [PubMed]

Cain, C. P.

D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
[Crossref] [PubMed]

Chen, C. K.

T. F. Heinz, C. K. Chen, D. Ricard, and Y. Shen, “Spectroscopy of Molecular Monolayers by Resonant Second-Harmonic Generation,” Phys. Rev. Lett. 48(7), 478–481 (1982).
[Crossref]

Dadap, J. I.

Dai, H. L.

G. Gonella and H. L. Dai, “Determination of adsorption geometry on spherical particles from nonlinear Mie theory analysis of surface second harmonic generation,” Phys. Rev. B 84(12), 121402 (2011).
[Crossref]

S. H. Jen, G. Gonella, and H. L. Dai, “The Effect of Particle Size in Second Harmonic Generation from the Surface of Spherical Colloidal Particles. I: Experimental Observations,” J. Phys. Chem. A 113(16), 4758–4762 (2009).
[Crossref] [PubMed]

H. M. Eckenrode, S. H. Jen, J. Han, A. G. Yeh, and H. L. Dai, “Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: Effect of surface charge and composition probed by second harmonic generation,” J. Phys. Chem. B 109(10), 4646–4653 (2005).
[Crossref] [PubMed]

H. M. Eckenrode and H. L. Dai, “Nonlinear optical probe of biopolymer adsorption on colloidal particle surface: poly-L-lysine on polystyrene sulfate microspheres,” Langmuir 20(21), 9202–9209 (2004).
[Crossref] [PubMed]

H. F. Wang, T. Troxler, A. G. Yeh, and H. L. Dai, “In Situ, Nonlinear Optical Probe of Surfactant Adsorption on the Surface of Microparticles in Colloids,” Langmuir 16(6), 2475–2481 (2000).
[Crossref]

de Beer, A. G. F.

Downer, M.

J. I. Dadap, X. Hu, N. Russell, J. Ekerdt, J. Lowell, and M. Downer, “Analysis of second-harmonic generation by unamplified, high-repetition-rate, ultrashort laser pulses at Si(001) interfaces,” IEEE J. Sel. Top. Quantum Electron. 1(4), 1145–1155 (1995).
[Crossref]

Eckenrode, H. M.

H. M. Eckenrode, S. H. Jen, J. Han, A. G. Yeh, and H. L. Dai, “Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: Effect of surface charge and composition probed by second harmonic generation,” J. Phys. Chem. B 109(10), 4646–4653 (2005).
[Crossref] [PubMed]

H. M. Eckenrode and H. L. Dai, “Nonlinear optical probe of biopolymer adsorption on colloidal particle surface: poly-L-lysine on polystyrene sulfate microspheres,” Langmuir 20(21), 9202–9209 (2004).
[Crossref] [PubMed]

Eilert, B. G.

D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
[Crossref] [PubMed]

Eisenthal, K. B.

L. Haber, S. J. J. Kwok, M. Semeraro, and K. B. Eisenthal, “Probing the colloidal gold nanoparticle/aqueous interface with second harmonic generation,” Chem. Phys. Lett. 507(1-3), 11–14 (2011).
[Crossref]

J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
[Crossref] [PubMed]

M. Subir, J. Liu, and K. B. Eisenthal, “Protonation at the Aqueous Interface of Polymer Nanoparticles with Second Harmonic Generation,” J. Phys. Chem. C 112(40), 15809–15812 (2008).
[Crossref]

K. B. Eisenthal, “Second harmonic spectroscopy of aqueous nano- and microparticle interfaces,” Chem. Rev. 106(4), 1462–1477 (2006).
[Crossref] [PubMed]

Y. Liu, C. Y. Yan, X. L. Zhao, and K. B. Eisenthal, “Surface potential of charged liposomes determined by second harmonic generation,” Langmuir 17(7), 2063–2066 (2001).
[Crossref]

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R. Bersohn, Y. H. Pao, and H. L. Frisch, “Double-Quantum Light Scattering by Molecules,” J. Chem. Phys. 45(9), 3184–3198 (1966).
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J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
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L. Haber, S. J. J. Kwok, M. Semeraro, and K. B. Eisenthal, “Probing the colloidal gold nanoparticle/aqueous interface with second harmonic generation,” Chem. Phys. Lett. 507(1-3), 11–14 (2011).
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J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
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H. Husu, R. Siikanen, J. Mäkitalo, J. Lehtolahti, J. Laukkanen, M. Kuittinen, and M. Kauranen, “Metamaterials with Tailored Nonlinear Optical Response,” Nano Lett. 12(2), 673–677 (2012).
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A. Vogel, N. Linz, S. Freidank, and G. Paltauf, “Femtosecond-Laser-Induced Nanocavitation in Water: Implications for Optical Breakdown Threshold and Cell Surgery,” Phys. Rev. Lett. 100(3), 038102 (2008).
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M. Subir, J. Liu, and K. B. Eisenthal, “Protonation at the Aqueous Interface of Polymer Nanoparticles with Second Harmonic Generation,” J. Phys. Chem. C 112(40), 15809–15812 (2008).
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J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
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Y. Liu, C. Y. Yan, X. L. Zhao, and K. B. Eisenthal, “Surface potential of charged liposomes determined by second harmonic generation,” Langmuir 17(7), 2063–2066 (2001).
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J. I. Dadap, X. Hu, N. Russell, J. Ekerdt, J. Lowell, and M. Downer, “Analysis of second-harmonic generation by unamplified, high-repetition-rate, ultrashort laser pulses at Si(001) interfaces,” IEEE J. Sel. Top. Quantum Electron. 1(4), 1145–1155 (1995).
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Lukianova, E. Y.

D. O. Lapotko and E. Y. Lukianova, “Influence of Physiological Conditions on Laser Damage Thresholds for Blood, Heart, and Liver Cells,” Lasers Surg. Med. 36(1), 13–21 (2005).
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R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14(17), 681–684 (1965).
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H. Husu, R. Siikanen, J. Mäkitalo, J. Lehtolahti, J. Laukkanen, M. Kuittinen, and M. Kauranen, “Metamaterials with Tailored Nonlinear Optical Response,” Nano Lett. 12(2), 673–677 (2012).
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Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
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J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
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D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
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D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
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M. Kauranen and A. Persoons, “Theory of polarization measurements of second-order nonlinear light scattering,” J. Chem. Phys. 104(10), 3445–3456 (1996).
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B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
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B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
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Ricard, D.

T. F. Heinz, C. K. Chen, D. Ricard, and Y. Shen, “Spectroscopy of Molecular Monolayers by Resonant Second-Harmonic Generation,” Phys. Rev. Lett. 48(7), 478–481 (1982).
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D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
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J. Butet, I. Russier-Antoine, C. Jonin, N. Lascoux, E. Benichou, and P. F. Brevet, “Sensing with Multipolar Second Harmonic Generation from Spherical Metallic Nanoparticles,” Nano Lett. 12(3), 1697–1701 (2012).
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B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
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R. W. Terhune, P. D. Maker, and C. M. Savage, “Measurements of nonlinear light scattering,” Phys. Rev. Lett. 14(17), 681–684 (1965).
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L. Schneider, H. J. Schmid, and W. Peukert, “Influence of particle size and concentration on the second-harmonic signal generated at colloidal surfaces,” Appl. Phys. B 87(2), 333–339 (2007).
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L. Schneider, H. J. Schmid, and W. Peukert, “Influence of particle size and concentration on the second-harmonic signal generated at colloidal surfaces,” Appl. Phys. B 87(2), 333–339 (2007).
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B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
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L. Haber, S. J. J. Kwok, M. Semeraro, and K. B. Eisenthal, “Probing the colloidal gold nanoparticle/aqueous interface with second harmonic generation,” Chem. Phys. Lett. 507(1-3), 11–14 (2011).
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H. Husu, R. Siikanen, J. Mäkitalo, J. Lehtolahti, J. Laukkanen, M. Kuittinen, and M. Kauranen, “Metamaterials with Tailored Nonlinear Optical Response,” Nano Lett. 12(2), 673–677 (2012).
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Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
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D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
[Crossref] [PubMed]

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J. Liu, M. Subir, K. Nguyen, and K. B. Eisenthal, “Second Harmonic Studies of Ions Crossing Liposome Membranes in Real Time,” J. Phys. Chem. B 112(48), 15263–15266 (2008).
[Crossref] [PubMed]

M. Subir, J. Liu, and K. B. Eisenthal, “Protonation at the Aqueous Interface of Polymer Nanoparticles with Second Harmonic Generation,” J. Phys. Chem. C 112(40), 15809–15812 (2008).
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D. S. Peterka, H. Takahashi, and R. Yuste, “Imaging Voltage in Neurons,” Neuron 69(1), 9–21 (2011).
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D. J. Payne, R. A. Hopkins, B. G. Eilert, G. D. Noojin, D. J. Stolarski, R. J. Thomas, C. P. Cain, G. T. Hengst, P. K. Kennedy, T. R. Jost, and B. A. Rockwell, “Comparative Study of Laser Damage Threshold Energies in the Artificial Retina,” J. Biomed. Opt. 4(3), 337–344 (1999).
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S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
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S. Roke, J. Buitenhuis, J. C. van Miltenburg, M. Bonn, and A. van Blaaderen, “Interface-solvent effects during colloidal phase transitions,” J. Phys. Condens. Matter 17(45), S3469–S3479 (2005).
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A. Vogel, N. Linz, S. Freidank, and G. Paltauf, “Femtosecond-Laser-Induced Nanocavitation in Water: Implications for Optical Breakdown Threshold and Cell Surgery,” Phys. Rev. Lett. 100(3), 038102 (2008).
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H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, “Second harmonic generation from the surface of centrosymmetric particles in bulk solution,” Chem. Phys. Lett. 259(1-2), 15–20 (1996).
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H. F. Wang, T. Troxler, A. G. Yeh, and H. L. Dai, “In Situ, Nonlinear Optical Probe of Surfactant Adsorption on the Surface of Microparticles in Colloids,” Langmuir 16(6), 2475–2481 (2000).
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Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
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Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
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S. Roke, W. G. Roeterdink, J. E. G. J. Wijnhoven, A. V. Petukhov, A. W. Kleyn, and M. Bonn, “Vibrational sum frequency scattering from a submicron suspension,” Phys. Rev. Lett. 91(25), 258302 (2003).
[Crossref] [PubMed]

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B. Schürer, S. Wunderlich, C. Sauerbeck, U. Peschel, and W. Peukert, “Probing colloidal interfaces by angle-resolved second harmonic light scattering,” Phys. Rev. B 82(24), 241404 (2010).
[Crossref]

Yan, C. Y.

Y. Liu, C. Y. Yan, X. L. Zhao, and K. B. Eisenthal, “Surface potential of charged liposomes determined by second harmonic generation,” Langmuir 17(7), 2063–2066 (2001).
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H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, “Second harmonic generation from the surface of centrosymmetric particles in bulk solution,” Chem. Phys. Lett. 259(1-2), 15–20 (1996).
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H. M. Eckenrode, S. H. Jen, J. Han, A. G. Yeh, and H. L. Dai, “Adsorption of a cationic dye molecule on polystyrene microspheres in colloids: Effect of surface charge and composition probed by second harmonic generation,” J. Phys. Chem. B 109(10), 4646–4653 (2005).
[Crossref] [PubMed]

H. F. Wang, T. Troxler, A. G. Yeh, and H. L. Dai, “In Situ, Nonlinear Optical Probe of Surfactant Adsorption on the Surface of Microparticles in Colloids,” Langmuir 16(6), 2475–2481 (2000).
[Crossref]

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D. S. Peterka, H. Takahashi, and R. Yuste, “Imaging Voltage in Neurons,” Neuron 69(1), 9–21 (2011).
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ACS Nano (1)

Y. Wang, O. Zeiri, A. Neyman, F. Stellacci, and I. A. Weinstock, “Nucleation and Island Growth of Alkanethiolate Ligand Domains on Gold Nanoparticles,” ACS Nano 6(1), 629–640 (2012).
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Figures (4)

Fig. 1
Fig. 1 Optical setup used for SH scattering measurements. P: Polarizer, LP: long pass filter, FL: focusing lens, CL: Collimating lens, BP: band pass filter. The detection arm can be adjusted to any orientation from −120° to 120°.

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Fig. 2
Fig. 2 a)The power dependence in PP polarization of SHS from a 0.026 v.v. % solution of PS beads. The power was measured in mW before the focus. The scattered light was detected at 30° degrees with an angle of acceptance of 2° and 10 s acquisition time. (b) SH intensity as a function of particle density from aqueous solutions of PS particles with a diameter of 500 nm, recorded under the same experimental condition as in a. The best fit solid line indicates a linear dependence.

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Fig. 3
Fig. 3 HRS intensity from pure water as a function of acquisition time. The inset shows the response for a time lapse of 5 ms (1000 laser shots). The angular resolution was 5° degrees and the scattering angle was set at 90°.

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Fig. 4
Fig. 4 a) SHS spectra recorded (at a detection angle of 30°) from the surface of PS particles in water (0.026 v.v%, 500 nm diameter), and 8 nm gold nanoparticles in water. The SHS spectrum of the PS beads follows the shape of the frequency doubled laser spectrum, while the spectral response from the Au nanoparticles is broadened by the resonance of the SH light with the 520 nm centered plasmon resonance. b) Comparison of signal strengths for liposomes (100 nm, 0.075 v.v %), nanoparticles (8 nm, 12 µg/ml), and polystyrene particles (500 nm, 0.026 v.v %).

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