OSA's Digital Library

Optics Express

Optics Express

  • Editor: C. Martijn de Sterke
  • Vol. 15, Iss. 24 — Nov. 26, 2007
  • pp: 16051–16060

Defocused imaging of second harmonic generation from a single nanocrystal

N. Sandeau, L. Le Xuan, D. Chauvat, C. Zhou, J.-F. Roch, and S. Brasselet  »View Author Affiliations

Optics Express, Vol. 15, Issue 24, pp. 16051-16060 (2007)

View Full Text Article

Enhanced HTML    Acrobat PDF (461 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



We demonstrate the direct imaging of the second harmonic generation radiation from a single nonlinear nanocrystal using defocused nonlinear microscopy. This technique allows the retrieval of complete information on the 3D orientation of a nanocrystal as well as possible deviations from its purely crystalline nature, in a simple experimental implementation. The obtained images are modeled by calculation of the radiation diagram from a nonlinear dipole that accounts for the excitation beam, the crystal symmetry and the particle size. Experimental demonstrations are performed on Potassium Titanyl Phosphase (KTP) nanocrystals. The shape and structure of the radiation images show a strong dependence on both crystal orientation and field polarization state, as expected by the specific nonlinear coherent coupling between the induced dipole and the excitation field polarization state.

© 2007 Optical Society of America

OCIS Codes
(190.1900) Nonlinear optics : Diagnostic applications of nonlinear optics
(180.4315) Microscopy : Nonlinear microscopy

ToC Category:

Original Manuscript: July 26, 2007
Revised Manuscript: October 18, 2007
Manuscript Accepted: October 18, 2007
Published: November 20, 2007

Virtual Issues
Vol. 2, Iss. 12 Virtual Journal for Biomedical Optics

N. Sandeau, L. Le Xuan, D. Chauvat, C. Zhou, J.-F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007)

Sort:  Year  |  Journal  |  Reset  


  1. M. Flijrsheimer, C. Radiige, H. Salmen, M. Bösch, R. Terbrack, and H. Fuchs, "In-situ imaging of Langmuir monolayers by second-harmonic microscopy," Thin Solid Films 284, 659-662 (1996). [CrossRef]
  2. R. Gauderon, P. B. Lukins, and C. J. R. Sheppard, "Three-dimensional second-harmonic generation imaging with femtosecond laser pulses," Opt. Lett. 23, 1209-1212 (1998). [CrossRef]
  3. P. J. Campagnola, M. Wei, A. Lewis, and L. M. Loew, "High-Resolution Nonlinear Imaging of Live Cells by Second Harmonic Generation," Biophys. J. 77, 3341-3349 (1999). [CrossRef] [PubMed]
  4. L. Moreaux, O. Sandrea, and J. Mertz, "Membrane Imaging by Second Harmonic Generation Microscopy," J. Opt. Soc. Am. B 17, 1685-1689 (2000). [CrossRef]
  5. C. Anceau, S. Brasselet, and J. Zyss, "Local orientational distribution of molecular monolayers probed by nonlinear microscopy," Chem. Phys. Lett. 411, 98-102 (2005). [CrossRef]
  6. V. Le Floc’h, S. Brasselet, J.-F. Roch, and J. Zyss, "Monitoring of orientation in molecular ensembles by polarization sensitive nonlinear microscopy," J. Phys.Chem. B 107, 12403-12410 (2003). [CrossRef]
  7. P. Stoller, B. M. Kim, A. M. Rubenchik, K. M. Reiser, and L. B. Da Silva, "Polarization-dependent optical second harmonic imaging of a rat-tail tendon," J. Biomed. Opt. 7, 205-214 (2000). [CrossRef]
  8. K. Komorowska, S. Brasselet, J. Zyss, L. Pourlsen, M. Jazdzyk, H. J. Egelhaaf, J. Gierschner, and M. Hanack, "Nanometric scale investigation of the nonlinear efficiency of perhydrotriphynylene inclusion compounds," Chem. Phys. 318, 12-20 (2005). [CrossRef]
  9. R. M. Williams, W. R. Zipfel, and W. W. Webb, "Interpreting Second-Harmonic Generation Images of Collagen I Fibrils," Biophys. J. 88, 13771386 (2005). [CrossRef] [PubMed]
  10. J. Zyss, "Molecular Engineering Implications of Rotational Invariance in Quadratic Nonlinear Optics: from Dipolar to Octupolar Molecules and Materials," J. Chem. Phys. 98, 6583-6593 (1993) [CrossRef]
  11. E. Yew, and C. Sheppard, "Effects of axial field components on second harmonic generation microscopy," Opt. Express 14, 1167-1174 (2006). [CrossRef]
  12. G. Revillod, I. Russier-Antoine, E. Benichou, C. Jonin, and P-F. Brevet, "Investigating the interaction of crystal violet probe molecules on sodium dodecyl sulfate micelles with Hyper-Rayleigh scattering," J. Phys. Chem. B 109, 5383-5389 (2005). [CrossRef]
  13. S. Brasselet, V. Le Floc’h, F. Treussart, J.-F. Roch, J. Zyss, E. Botzung-Appert, and A. Ibanez, "In situ diagnostics of the crystalline nature of single organic nanocrystals by nonlinear microscopy," Phys. Rev. Lett. 92, 207401 (2004). [CrossRef] [PubMed]
  14. F. Treussart, E. Botzung-Appert, N. T. Ha-Duong, A. Ibanez, J.-F. Roch, and R. Pansu," Second harmonic generation and fluorescence of CMONS dye nanocrystals grown in a sol-gel thin film," Chem. Phys. Chem. 4, 757-760 (2003). [CrossRef] [PubMed]
  15. E. Delahaye, N. Tancrez, T. Yi, I. Ledoux, J. Zyss, S. Brasselet, and R. Clément, "Second harmonic generation from individual hybrid MnPS3-based nanoparticles investigated by nonlinear microscopy" Chem. Phys. Lett. 429, 533-537 (2006). [CrossRef]
  16. L. Le Xuan, F. Marquier, D. Chauvat, S. Brasselet, F. Treussart, S. Perruchas, C. Tard, T. Gacoin, and J.-F. Roch, "Balanced homodyne detection in second harmonic generation microscopy," Appl. Phys. Lett. 89, 121118-1-3 (2006). [CrossRef]
  17. J. P. Long, B. S. Simpkins, D. J. Rowenhorst, and P. E. Pehrsson, "Far-field Imaging of Optical Second-Harmonic Generation in Single GaN Nanowires," Nanoletters 7, 831-836 (2007). [CrossRef]
  18. L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J.-F. Roch, "Photostable blinking-free single nanocrystals for second harmonic microscopy," submitted.
  19. S. Brasselet and J. Zyss, "Nonlinear polarimetry of molecular crystals down to the nanoscale," C. R. Physique 8, 165-179 (2007). [CrossRef]
  20. M. Böhmer and J. Enderlein, "Orientation imaging of single molecules by wide-field epifluorescence microscopy," J. Opt. Soc. Am. B 20, 554-559 (2003). [CrossRef]
  21. J. Enderlein, and M. Böhmer, "Influence of interface dipole interactions on the efficiency of fluorescence light collection near surfaces," Opt. Lett. 28, 941-944 (2003). [CrossRef] [PubMed]
  22. M. A. Lieb, J. M. Zavislan, and L. Novotny, "Single-molecule orientations determined by direct emission pattern imaging," J. Opt. Soc. Am. B 21, 1210-1215 (2004). [CrossRef]
  23. X. Brokmann, M.-V. Ehrensperger, J.-P. Hermier, A. Triller, and M. Dahan, "Orientational imaging and tracking of single CdSe nanocrystals by defocused microscopy," Chem. Phys. Lett. 406, 210214 (2005). [CrossRef]
  24. J. Enderlein, "Theoretical study of detection of a dipole emitter through an objective with high numerical aperture," Opt. Lett. 25, 634-637 (2000). [CrossRef]
  25. H. Vanherzeele and J. D. Bierlein, "Magnitude of the nonlinear-optical coefficients of KTiOPO4," Opt. Lett. 17, 982-985 (1992). [CrossRef] [PubMed]
  26. B. Richards and E. Wolf, "Electromagnetic diffraction in optical systems. II. Structure of the image field in an aplanetic system," Proc. of the Royal Society of London.Series A. 153, 358-379 (1959). [CrossRef]
  27. D. Gachet, N. Sandeau, and H. Rigneault, "Far-field radiation pattern in Coherent Anti-stokes Raman Scattering (CARS) Microscopy," Biomedical Vibrational Spectroscopy III: Advances in Research and Industry, Proc SPIE 6093, 62 (2006).

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited