Second harmonic generation imaging with a kHz amplifier [Invited]

Nonlinear optical imaging is a powerful method for observing bulk and interfacial phenomena in time and space. Here, we present a stepby-step description of how to carry out second harmonic generation imaging with a kHz amplifier laser system and demonstrate its applicability for SHG microscopy studies of highly size-resolved colloidal CdSe quantum dots having radii of 1-2 nm deposited on glass slides. It is found that not all quantum dots are SHG active, which suggests that environmental effects and particle distributions are important for SHG activity of quantum dots. ©2011 Optical Society of America OCIS codes: (110.0110) Imaging systems; (120.0120) Instrumentation, measurement, and metrology; (140.0140) Lasers and laser optics; (180.0180) Microscopy; (190.0190) Nonlinear optics; (300.0300) Spectroscopy. References and links 1. R. Boyd, Nonlinear Optics, 2nd ed. (Academic Press, 2003). 2. O. A. Aktsipetrov, P. V. Elyutin, A. A. Fedyanin, A. A. Nikulin, and A. N. Rubtsov, “Second harmonic generation in metal and semiconductor low-dimensional structures,” Surf. Sci. 325(3), 343–355 (1995). 3. M. Jacobsohn and U. Banin, “Size dependence of second harmonic generation in CdSe nanocrystal quantum dots,” J. Phys. Chem. B 104(1), 1–5 (2000). 4. B. S. Santos, G. A. Pereira, D. V. Petrov, and C. D. Donega, “First hyperpolarizability of CdS nanoparticles studied by hyper-Rayleigh scattering,” Opt. Commun. 178(1-3), 187–192 (2000). 5. M. Zielinski, D. Oron, D. Chauvat, and J. Zyss, “Second-harmonic generation from a single core/shell quantum dot,” Small 5(24), 2835–2840 (2009). 6. E. Shaviv and U. Banin, “Synergistic effects on second harmonic generation of hybrid CdSe-Au nanoparticles,” ACS Nano 4(3), 1529–1538 (2010). 7. M. A. Kriech and J. C. Conboy, “Imaging chirality with surface second harmonic generation microscopy,” J. Am. Chem. Soc. 127(9), 2834–2835 (2005). 8. N. Ji, K. Zhang, H. Yang, and Y.-R. Shen, “Three-dimensional chiral imaging by sum-frequency generation,” J. Am. Chem. Soc. 128(11), 3482–3483 (2006). 9. M. Nuriya, J. Jiang, B. Nemet, K. B. Eisenthal, and R. Yuste, “Imaging membrane potential in dendritic spines,” Proc. Natl. Acad. Sci. U.S.A. 103(3), 786–790 (2006). 10. R. D. Schaller, J. C. Johnson, K. R. Wilson, L. F. Lee, L. H. Haber, and R. J. Saykally, “Nonlinear chemical imaging nanomicroscopy: from second and third harmonic generation to multiplex (broad-bandwidth) sum frequency generation near-field scanning optical microscopy,” J. Phys. Chem. B 106(20), 5143–5154 (2002). 11. K. Cimatu and S. Baldelli, “Chemical imaging of corrosion: sum frequency generation imaging microscopy of cyanide on gold at the solid-liquid interface,” J. Am. Chem. Soc. 130(25), 8030–8037 (2008). 12. R. D. Wampler, D. J. Kissick, C. J. Dehen, E. J. Gualtieri, J. L. Grey, H.-F. Wang, D. H. Thompson, J.-X. Cheng, and G. J. Simpson, “Selective detection of protein crystals by second harmonic microscopy,” J. Am. Chem. Soc. 130(43), 14076–14077 (2008). 13. P. Rechsteiner, J. Hulliger, and M. Flörsheimer, “Phase-sensitive second harmonic microscopy reveals bipolar twinning of markov-type molecular crystals,” Chem. Mater. 12(11), 3296–3300 (2000). 14. A. C. Millard, L. Jin, J. P. Wuskell, D. M. Boudreau, A. Lewis, and L. M. Loew, “Wavelengthand timedependence of potentiometric non-linear optical signals from styryl dyes,” J. Membr. Biol. 208(2), 103–111 (2005). 15. R. Jin, J. E. Jureller, H. Y. Kim, and N. F. Scherer, “Correlating second harmonic optical responses of single Ag nanoparticles with morphology,” J. Am. Chem. Soc. 127(36), 12482–12483 (2005). 16. 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,” Nano Lett. 7(3), 831–836 (2007). 17. T. Petralli-Mallow, T. M. Wong, J. D. Byers, H. I. Yee, and J. M. Hicks, “Circular dichroism spectroscopy at interfaces: a surface second harmonic generation study,” J. Phys. Chem. 97(7), 1383–1388 (1993). #142850 $15.00 USD Received 23 Feb 2011; revised 7 Mar 2011; accepted 7 Mar 2011; published 22 Apr 2011 (C) 2011 OSA 1 May 2011 / Vol. 1, No. 1 / OPTICAL MATERIALS EXPRESS 57 18. T. Verbiest, S. V. Elshocht, A. Persoons, C. Nuckolls, K. E. Phillips, and T. J. Katz, “Second-order nonlinear optical properties of highly symmetric chiral thin films,” Langmuir 17(16), 4685–4687 (2001). 19. J. M. Hicks, Chirality: Physical Chemistry, ACS Symposium Series 810 (Oxford University Press, 2002). 20. B. J. Burke, A. J. Moad, M. A. Polizzi, and G. J. Simpson, “Experimental confirmation of the importance of orientation in the anomalous chiral sensitivity of second harmonic generation,” J. Am. Chem. Soc. 125(30), 9111–9115 (2003). 21. G. J. Simpson, “Molecular origins of the remarkable chiral sensitivity of second-order nonlinear optics,” ChemPhysChem 5(9), 1301–1310 (2004). 22. N. Ji and Y. R. Shen, “Optically active sum frequency generation from molecules with a chiral center: amino acids as model systems,” J. Am. Chem. Soc. 126(46), 15008–15009 (2004). 23. Y. R. Shen, The Principles of Nonlinear Optics (John Wiley & Sons, 1984). 24. P. M. Rentzepis, J. A. Giordmaine, and K. W. Wecht, “Coherent optical mixing in optically active liquids,” Phys. Rev. Lett. 16(18), 792–794 (1966). 25. M. A. Belkin, T. A. Kulakov, K. H. Ernst, L. Yan, and Y. R. Shen, “Sum-frequency vibrational spectroscopy on chiral liquids: a novel technique to probe molecular chirality,” Phys. Rev. Lett. 85(21), 4474–4477 (2000). 26. J. A. Giordmaine, “Nonlinear optical properties of liquids,” Phys. Rev. 138(6A), A1599–A1606 (1965). 27. J. F. Nye, Physical Properties of Crystals: Their Representation by Tensors and Matrices (Oxford University Press, 1957). 28. A. J. Moad and G. J. Simpson, “Self-consistent approach for simplifying the molecular interpretation of nonlinear optical and multiphoton phenomena,” J. Phys. Chem. A 109(7), 1316–1323 (2005). 29. Y. R. Shen, “Nonlinear optical spectroscopy of molecular chirality,” in Trends and Perspectives in Modern Computational Science, G. Maroulis and T. Simos, eds. (Brill Academic Pub., 2006), pp. 461–471. 30. V. J. Hall and G. J. Simpson, “Direct observation of transient Ostwald crystallization ordering from racemic serine solutions,” J. Am. Chem. Soc. 132(39), 13598–13599 (2010). 31. J. Butet, J. Duboisset, G. Bachelier, I. Russier-Antoine, E. Benichou, C. Jonin, and P.-F. Brevet, “Optical second harmonic generation of single metallic nanoparticles embedded in a homogeneous medium,” Nano Lett. 10(5), 1717–1721 (2010). 32. V. K. Valev, N. Smisdom, A. V. Silhanek, B. De Clercq, W. Gillijns, M. Ameloot, V. V. Moshchalkov, and T. Verbiest, “Plasmonic ratchet wheels: switching circular dichroism by arranging chiral nanostructures,” Nano Lett. 9(11), 3945–3948 (2009). 33. N. J. Borys, M. J. Walter, and J. M. Lupton, “Intermittency in second-harmonic radiation from plasmonic hot spots on rough silver films,” Phys. Rev. B 80(16), 161407 (2009). 34. A. J. Morris-Cohen, M. D. Donakowski, K. E. Knowles, and E. A. Weiss, “The effect of a common purification procedure on the chemical composition of the surfaces of CdSe quantum dots synthesized with trioctylphosphine oxide,” J. Phys. Chem. C 114(2), 897–906 (2010). 35. A. J. Morris-Cohen, M. T. Frederick, G. D. Lilly, E. A. McArthur, and E. A. Weiss, “Organic surfactantcontrolled composition of the surfaces of CdSe quantum dots,” J. Phys. Chem. Lett. 1(7), 1078–1081 (2010). 36. L. Qu and X. Peng, “Control of photoluminescence properties of CdSe nanocrystals in growth,” J. Am. Chem. Soc. 124(9), 2049–2055 (2002). 37. W. W. Yu, L. Qu, W. Guo, and X. Peng, “Experimental determination of the extinction coefficient of CdTe, CdSe, and CdS nanocrystals,” Chem. Mater. 15(14), 2854–2860 (2003). 38. Y. R. Shen, The Principles of Nonlinear Optics (John Wiley & Sons, 2003). 39. M. L. Frederick, J. L. Achtyl, K. E. Knowles, E. A. Weiss, and F. M. Geiger, “Surface amplified ligand disorder in CdSe quantum dots determined by electron and coherent vibrational spectroscopy” (submitted [2010]). 40. C. J. Murphy, A. M. Gole, S. E. Hunyadi, J. W. Stone, P. N. Sisco, A. Alkilany, B. E. Kinard, and P. Hankins, “Chemical sensing and imaging with metallic nanorods,” Chem. Commun. (Camb.) 5(5), 544–557 (2008).