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Optics Express

Optics Express

  • Editor: C. Martijn de Sterke
  • Vol. 18, Iss. 22 — Oct. 25, 2010
  • pp: 23218–23225
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Evanescent-field-induced second harmonic generation by noncentrosymmetric nanoparticles

Ronja Bäumner, Luigi Bonacina, Jörg Enderlein, Jérôme Extermann, Thomas Fricke-Begemann, Gerd Marowsky, and Jean-Pierre Wolf  »View Author Affiliations


Optics Express, Vol. 18, Issue 22, pp. 23218-23225 (2010)
http://dx.doi.org/10.1364/OE.18.023218


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Abstract

We demonstrate the excitation of second harmonic radiation of noncentrosymmetric nanoparticles dispersed on a planar optical waveguide by the evanescent field of the guided mode. Polarization imaging reveals information on the orientation of the crystal axis of individual nanoparticles. Interference patterns generated from adjacent particles at the second harmonic frequency are - to the authors knowledge - observed for the first time. The actual form of the interference pattern is explained on the basis of a dipole radiation model, taking into account the nanoparticles’ orientation, surface effects, and the characteristics of the imaging optics.

© 2010 Optical Society of America

1. Introduction

Planar optical waveguides have already been used as a suitable excitation platform in a number of fluorescence analysis applications.[1

1. G. L. Duveneck, M. Pawlak, D. Neuschafer, E. Bar, W. Budach, and U. Pieles, “Novel bioaffinity sensors for trace analysis based on luminescence excitation by planar waveguides,” Sens. Actuators B 38, 88–95 (1997). [CrossRef]

, 2

2. P. N. Zeller, G. Voirin, and R. E. Kunz, “Single-pad scheme for integrated optical fluorescence sensing,” Biosens. Bioelectron. 15, 591–595 (2000). [CrossRef]

, 3

3. K. Schmitt, K. Oehse, G. Sulz, and C. Hoffmann, “Evanescent field sensors based on tantalum pentoxide waveguides - a review,” Sensors 8, 711–738 (2008). [CrossRef]

] They enable highly efficient and selective excitation of fluorescent molecules in close proximity to the waveguide surface by the evanescent field of the guided mode. Typically the waveguide is composed of a single layer of a metaloxide with high index of refraction. High intensity of the evanescent field is assured by using an appropriate film thickness for single mode operation, usually in the range of 100 – 200 nm. The strong evanescent field of such waveguide modes allows the design of highly sensitive devices and provides the possibility for two-photon fluorescence excitation on comparatively large areas.[4

4. C. Kappel, A. Selle, T. Fricke-Begemann, M. A. Bader, and G. Marowsky, “Giant enhancement of two-photon fluorescence induced by resonant double grating waveguide structures,” Appl. Phys. B: Lasers Opt. 79, 531–534 (2004). [CrossRef]

, 5

5. G. L. Duveneck, M. A. Bopp, M. Ehrat, M. Haiml, U. Keller, M. A. Bader, G. Marowsky, and S. Soria, “Evanescent-field-induced two-photon fluorescence: excitation of macroscopic areas of planar waveguides,” Appl. Phys. B: Lasers Opt. 73, 869–871 (2001). [CrossRef]

]

In this work we demonstrate non-scanning excitation of the second harmonic (SH) response of several individual SHRIMPs scattered over a large area on a planar waveguide. Although evanescent-field-induced two-photon fluorescence was already demonstrated for homogenous organic layers, this work provides for the first time the evidence of non-scanning evanescent excitation of the SH response of nanometric objects. In a similar context, it should be highlighted the experiment realized by the Prasad group on nonlinear excitation of organic nanocrystals with a photon scanning tunneling microscope.[14

14. Y. Shen, J. Swiatkiewicz, J. Winiarz, P. Markowicz, and P. N. Prasad, “Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope,” Appl. Phys. Lett. 77, 2946 (2000). [CrossRef]

] Our results are discussed in terms of efficiency and polarization properties. Further information about individual nanoparticles’ orientation and coherent emission are derived within the defined image defocusing framework first developed by Sepiol [15

15. J. Jasny and J. Sepiol, “Single molecules observed by immersion mirror objective. a novel method of finding the orientation of a radiating dipole,” Chem. Phys. Lett. 273, 439–443 (1997). [CrossRef]

] and later expanded by Enderlein and co-workers.[16

16. M. Bohmer and J. Enderlein, “Orientation imaging of single molecules by wide-field epifluorescence microscopy,” J. Opt. Soc. Am. B 20, 554–559 (2003). [CrossRef]

]

2. Experimental

The experimental setup is described in Fig. 1. The frequency-doubled output of an ultrashort-pulse Erbium doped fiber laser (Menlo Systems TC1550, central wavelength 780 nm, bandwidth 9 nm, output power 45 mW, repetition rate 80 MHz, pulse duration 150 fs) is coupled with TE polarization under the resonance angle of −48° into a tantalum pentoxide waveguide of thickness 159 nm on a 0.7 mm AF45 glass substrate by a lithographically manufactured grating structure (Balzers Optics, Liechtenstein, grating period Λ = 318 nm). The guided mode inside the plane waveguide has a lateral extension along the x-direction of 25 μm. TE laser polarization denotes an electric field vector along the x axis of the laboratory frame. The coupling efficiency into the waveguide is approximately 20%. Due to the limited spectral acceptance of the grating, the spectral bandwidth of the coupled pulses is reduced to 4 nm, leading to temporal stretching.

Fig. 1 Experimental setup. Laser radiation is coupled via grating couplers (Gr) into the tantalum pentoxide (Ta2O5) waveguide which is applied to the surface of a glass substrate. The SH as generated by the nanoparticles on the waveguide is observed by a CCD camera through a microscope objective (Obj). SF: Spectral Filter. PA: Polarization Analyzer. WD: Working Distance of the objective. def: defocusing parameter. Left: 3D view. Right: side view illustrating the geometry of substrate, waveguide, nanoparticles, incident laser beam and the intensity profile of the guided mode.

Potassium-Titanyl-Phospate (KTiOPO4, KTP) powder (Cristal Laser S.A., Messein - France) was dissolved in demineralized water. A drop (1 μl) of the solution was dispensed onto the waveguide surface at some millimeters from the grating coupler where the solvent evaporated. The histogram of naocrystals size as determined by dynamic light scattering (Malvern Zetasizer NanoZS) is given in Fig. 2(a) inset. The superimposed log-normal fit indicates an average size of 185 nm. The SH radiation emitted by individual SHRIMPs was collected by a 40× magnification objective (Nikon, Plan Fluor ELWD 40x/0.60), spectrally filtered by a multi-photon fluorescence emission filter (Semrock, FF01-750SP, 380–720 nm passband), and detected by a CCD camera (pco.1600, 1200 x 1600 pixels, pixel size 7.4 μm). For polarization analysis, a polarizing plate (Schneider-Kreuznach, AUF-MRC) located in front of the camera sensor was rotated by an angle α, where α = 0 corresponds to transmitted x-polarization. Defocused images were acquired by an accurately defined displacement, def, of the detection unit (objective, filter, CCD camera) and thus of the objective’s focal plane with respect to the waveguide surface.

Fig. 2 (a) Size distribution by number of the KTP nanocrystals suspension fitted by a log-normal function centered at 185 nm. (b) White light image of the scatterers on the waveguide. The dashed lines indicate the extension of the waveguide mode. (c) SH image of the same sample region. Note that the particles encircled in the upper plot are not present in the SH image. (d) Defocused (def = 20 μm) images of the four SH emitting particles of panel (b).

3. Imaging

Figure 2(b) presents an image of the nanoparticles spread on the waveguide under white light illumination. The differences in intensity revealed by the particles scattering, originate from the size dispersion of the sample. The lateral extension of the guided mode inside the waveguide is indicated by the two parallel dashed lines. Figure 2(c) represents the same sample region imaged at the SH frequency. The four nanoparticles appearing in this image, labeled AD, are evanescently excited by the laser radiation propagating inside the waveguide. Their positions spatially correlate with those of the nanoparticles observed in Fig. 2(b). Figure 3(a) shows the power dependence of the normalized SH signal generated by these nanoparticles. The response exhibits a clear square dependence shown by the superimposed fit (thick line). This result supports the good spectral selection of the experiment, appreciable also from the extremely high contrast in the SH response of Fig. 2(c). However, one can notice the absence in the SH image of the two nanoparticles encircled in Fig. 2(b) although they are both within the excitation region. The lack of the SH counterparts for these particles cannot be trivially ascribed to a difference in size: this becomes apparent for the right particle, which presents a higher scattering intensity than the average under white light illumination. The missing SH signal of these particles is rather owing to an unfavorable orientation of their crystal axis with respect to the excitation light polarization.

Fig. 3 (a) Normalized power dependence of the SH of nanoparticles AD of Fig. 1(b). (b) and (c) Polarization dependence of SH emission from particles D (▵) and C (□) as a function of the analyzer angle α. (d) and (e) Calculated intensity dependence of SH emission for particles D and C as a function of excitation light polarization (γ) and analyzer angle (continuous line α = 0, dashed line α = 90°). Waveguide evanescent excitation corresponds to γ = 0. Note that the α = 90° response in the upper plot is multiplied by ten for easier inspection.

4. Orientation retrieval

4.1. Polarization analysis

The polarization dependence of the nonlinear response of a nanocrystal can be calculated knowing the nonlinear susceptibility tensor of the material, χ(2), and the particle orientation with respect to the laser polarization.[17

17. 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]

] The induced nonlinear polarization components can be then defined as
Pi2ω=ɛ0jkχijk(2)EjωEkω
(1)

Where the χijk(2) tensor is expressed in the laboratory frame and can be derived from the χijk¯(2) tensor in the crystal frame by
χijk(2)=ijk¯χijk¯(2)Sii¯Sjj¯Skk¯
(2)
S being the components of the rotation matrix between the laboratory and crystal axes.[17

17. 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]

, 18

18. J. I. Dadap, “Optical second-harmonic scattering from cylindrical particles,” Phys. Rev. B 78, 205322 (2008). [CrossRef]

]

KTP presents an orthorombic crystal structure, where the χzzz¯(2) element is at least four times larger than any other tensorial contribution.[19

19. 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). [CrossRef] [PubMed]

] The particles highlighted in Fig. 2(b) very likely present an orientation of the crystal frame that leads to a vanishing result for Eq. 1, assuming an electric field vector aligned along x. For particles A – D, on the other hand, the SH response is generated quite efficiently.

4.2. Defocused imaging

As just mentioned, the fixed laser polarization of the approach presented above prevents a complete and rigorous orientation retrieval, nevertheless information about the out-of-plane angle θ of the nonlinear dipole can be derived by applying the theoretical model developed by J. Enderlein [16

16. M. Bohmer and J. Enderlein, “Orientation imaging of single molecules by wide-field epifluorescence microscopy,” J. Opt. Soc. Am. B 20, 554–559 (2003). [CrossRef]

] and already used by Sandeau et al. for analyzing the defocused images of SHRIMPs.[19

19. 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). [CrossRef] [PubMed]

] Figure 2(d) reports the images obtained for particles A – D by displacing the focal plane of the collection objective by def = 20 μm from the substrate. One can see that, while particles C and D present a radial symmetric emission structure with concentric rings of different intensity, particles A and B are characterized by the presence of weaker intensity regions in their emission patterns (the upper right zone and the bottom half respectively for particles A and B ). In addition, in the series experimental images reported in the first row of Fig. 4, measured by varying the def parameter from 0 to 70 μm, a clear asymmetry is observable for any def > 0 in the emission of the lower particle as opposed to the perfectly radial pattern of the upper one.

Fig. 4 Experimental (first row) and numerical (second row) images of two adjacent nanoparticles excited by the evanescent field and interfering at the SH frequency for different defocusing parameters: def = 0, 20, 50, and 70 μm. The third row contains the corresponding defocused images calculated for the artificial case of no inter-particles interference. The length scale is the same for all plots, the intensity scale are adjusted to facilitate the inspection of interference details but are maintained constant among second and third row for each def value. The resulting out-of-plane orientation of the emitting dipole associated to the upper particle and to the lower particle are θ1 = 90° (in-plane) and θ2 = 35°, respectively.

5. Coherent effects

One very intriguing characteristic emerging from all the images of Fig. 4 is the presence of interference fringes, occurring because of the coherent superposition of the SH emission of the two nanoparticles. Incidentally, analogous structures have been recently observed in the far-field scattering patterns generated by different portions of a micrometric rod.[21

21. S. W. Liu, H. J. Zhou, A. Ricca, R. Tian, and M. Xiao, “Far-field second-harmonic fingerprint of twinning in single ZnO rods,” Phys. Rev. B 77, 113311 (2008). [CrossRef]

] Here interferences appear for small defocusing values as stripes in the region between the two particles and then develop as a dashed motif on the concentric rings of the emission pattern. The simulations capture even the finest details observed in the experimental images. The best agreement was obtained by convoluting the numerical results with a disk of two pixels radius, accounting for the smoothing effect of the not perfectly planar waveguide surface. As an additional proof of the genuine interpretation of the observed patterns as resulting from interferences and to rule out any alternative explanation based on some critical misalignment of the optical set-up, we provide in the third row of Fig. 4 the corresponding defocused images calculated by artificially switching-off the inter-particles interference term. The false color scales for any given def value are respected in the simulations run with and without this contribution. From the comparison of both approaches with the experimental data, it immediately comes into sight that inter-particle interference plays an essential and unambiguous role in the definition of the observed pattern.

It is worth noting that - unlike the case of harmonic holography, where interferences are created with an external reference beam - we show here interferences originated directly among the nonlinear emissions of two distinct nano-objects for the first time. It should be also pointed out that the clear interference pattern of Fig. 4 is not easily observed. Most of the times, in fact, the latter presents complicated and nonsymmetric structures because of to the presence of several interfering nanoparticles and/or small aggregates. In these cases, the defocused images cannot be easily interpreted and modelled as the coherent superposition of a few, well defined, spatially separated dipoles.

6. Conclusions

This work proves the possibility to employ SHRIMP nanoparticles as molecular probes in experiments based on evanescent excitation, taking full advantage of their photostability and of their non-resonant optical response. High selective evanescent excitation at the substrate surface can be associated to nonlinear transverse resolution for imaging. In principle, for example, SHRIMPs can be used to probe the penetration of the evanescent field more efficiently than fluorescent beads for TIRF experiments.[22

22. J. Steyer and W. Almers, “Tracking single secretory granules in live chromaffin cells by evanescent-field fluorescence microscopy,” Biophys. J. 76, 2262–2271 (1999). [CrossRef] [PubMed]

] Furthermore, we demonstrated that polarization analysis can be carried out under reasonable assumptions, and the dipole moments associated to individual crystals can be prospectively used as optical probes of the local field [9

9. R. Grange, J. W. Choi, C. L. Hsieh, Y. Pu, A. Magrez, R. Smajda, L. Forro, and D. Psaltis, “Lithium niobate nanowires synthesis, optical properties, and manipulation,” Appl. Phys. Lett. 95, 143105 (2009). [CrossRef]

] in large areas of a waveguide for monitoring, for instance, cells membrane potential. Finally, and for the first time, we observed and numerically modeled the interferences generated from the nonlinear emission of distinct nanometric objects.

Acknowledgments

L. Bonacina acknowledges the financial support of the Swiss Secretary for Research (SER) in the framework of COST MP0604 actions. R. Bäumner and T. Fricke-Begemann gratefully acknowledge financial support by the German Federal Ministry of Economics and Technology (Grant no. 16IN0365). We are grateful to Ronan Le Dantec (SYMME, Université de Savoie) for the DLS measurements.

References and links

1.

G. L. Duveneck, M. Pawlak, D. Neuschafer, E. Bar, W. Budach, and U. Pieles, “Novel bioaffinity sensors for trace analysis based on luminescence excitation by planar waveguides,” Sens. Actuators B 38, 88–95 (1997). [CrossRef]

2.

P. N. Zeller, G. Voirin, and R. E. Kunz, “Single-pad scheme for integrated optical fluorescence sensing,” Biosens. Bioelectron. 15, 591–595 (2000). [CrossRef]

3.

K. Schmitt, K. Oehse, G. Sulz, and C. Hoffmann, “Evanescent field sensors based on tantalum pentoxide waveguides - a review,” Sensors 8, 711–738 (2008). [CrossRef]

4.

C. Kappel, A. Selle, T. Fricke-Begemann, M. A. Bader, and G. Marowsky, “Giant enhancement of two-photon fluorescence induced by resonant double grating waveguide structures,” Appl. Phys. B: Lasers Opt. 79, 531–534 (2004). [CrossRef]

5.

G. L. Duveneck, M. A. Bopp, M. Ehrat, M. Haiml, U. Keller, M. A. Bader, G. Marowsky, and S. Soria, “Evanescent-field-induced two-photon fluorescence: excitation of macroscopic areas of planar waveguides,” Appl. Phys. B: Lasers Opt. 73, 869–871 (2001). [CrossRef]

6.

J. Extermann, L. Bonacina, E. Cuna, C. Kasparian, Y. Mugnier, T. Feurer, and J. P. Wolf, “Nanodoublers as deep imaging markers for multi-photon microscopy,” Opt. Express 17, 15342–15349 (2009). [CrossRef] [PubMed]

7.

C. L. Hsieh, R. Grange, Y. Pu, and D. Psaltis, “Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging,” Opt. Express 17, 2880–2891 (2009). [CrossRef] [PubMed]

8.

A. V. Kachynski, A. N. Kuzmin, M. Nyk, I. Roy, and P. N. Prasad, “Zinc oxide nanocrystals for nonresonant nonlinear optical microscopy in biology and medicine,” J. Phys. Chem. C 112, 10721–10724 (2008). [CrossRef]

9.

R. Grange, J. W. Choi, C. L. Hsieh, Y. Pu, A. Magrez, R. Smajda, L. Forro, and D. Psaltis, “Lithium niobate nanowires synthesis, optical properties, and manipulation,” Appl. Phys. Lett. 95, 143105 (2009). [CrossRef]

10.

L. Le Xuan, S. Brasselet, F. Treussart, J. F. Roch, F. Marquier, D. Chauvat, S. Perruchas, C. Tard, and T. Gacoin, “Balanced homodyne detection of second-harmonic generation from isolated subwavelength emitters,” Appl. Phys. Lett. 89, 121118 (2006). [CrossRef]

11.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Galez, and J. P. Wolf, “Nano-frog: Frequency resolved optical gating by a nanometric object,” Opt. Express 16, 10405–10411 (2008). [CrossRef] [PubMed]

12.

P. Wnuk, L. Le Xuan, A. Slablab, C. Tard, S. Perruchas, T. Gacoin, J. F. Roch, D. Chauvat, and C. Radzewicz, “Coherent nonlinear emission from a single ktp nanoparticle with broadband femtosecond pulses,” Opt. Express 17, 4652–4658 (2009). [CrossRef] [PubMed]

13.

J. Extermann, P. Béjot, L. Bonacina, Y. Mugnier, R. Le Dantec, T. Mazingue, C. Galez, and J. Wolf, “An inexpensive nonlinear medium for intense ultrabroadband pulse characterization,” Appl. Phys. B 97, 537–540 (2009). [CrossRef]

14.

Y. Shen, J. Swiatkiewicz, J. Winiarz, P. Markowicz, and P. N. Prasad, “Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope,” Appl. Phys. Lett. 77, 2946 (2000). [CrossRef]

15.

J. Jasny and J. Sepiol, “Single molecules observed by immersion mirror objective. a novel method of finding the orientation of a radiating dipole,” Chem. Phys. Lett. 273, 439–443 (1997). [CrossRef]

16.

M. Bohmer and J. Enderlein, “Orientation imaging of single molecules by wide-field epifluorescence microscopy,” J. Opt. Soc. Am. B 20, 554–559 (2003). [CrossRef]

17.

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]

18.

J. I. Dadap, “Optical second-harmonic scattering from cylindrical particles,” Phys. Rev. B 78, 205322 (2008). [CrossRef]

19.

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). [CrossRef] [PubMed]

20.

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J. P. Wolf, “Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy,” Appl. Phys. B: Lasers Opt.87, 399–403 (2007). [CrossRef]

21.

S. W. Liu, H. J. Zhou, A. Ricca, R. Tian, and M. Xiao, “Far-field second-harmonic fingerprint of twinning in single ZnO rods,” Phys. Rev. B 77, 113311 (2008). [CrossRef]

22.

J. Steyer and W. Almers, “Tracking single secretory granules in live chromaffin cells by evanescent-field fluorescence microscopy,” Biophys. J. 76, 2262–2271 (1999). [CrossRef] [PubMed]

OCIS Codes
(190.2620) Nonlinear optics : Harmonic generation and mixing
(230.7370) Optical devices : Waveguides
(310.6628) Thin films : Subwavelength structures, nanostructures

ToC Category:
Nonlinear Optics

History
Original Manuscript: September 9, 2010
Revised Manuscript: September 30, 2010
Manuscript Accepted: October 1, 2010
Published: October 19, 2010

Citation
Ronja Bäumner, Luigi Bonacina, Jörg Enderlein, Jèrôme Extermann, Thomas Fricke-Begemann, Gerd Marowsky, and Jean-Pierre Wolf, "Evanescent-Field-Induced Second Harmonic Generation by Noncentrosymmetric Nanoparticles," Opt. Express 18, 23218-23225 (2010)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-18-22-23218


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References

  1. G. L. Duveneck, M. Pawlak, D. Neuschafer, E. Bar, W. Budach, and U. Pieles, “Novel bioaffinity sensors for trace analysis based on luminescence excitation by planar waveguides,” Sens. Actuators B 38, 88–95 (1997). [CrossRef]
  2. P. N. Zeller, G. Voirin, and R. E. Kunz, “Single-pad scheme for integrated optical fluorescence sensing,” Biosens. Bioelectron. 15, 591–595 (2000). [CrossRef]
  3. K. Schmitt, K. Oehse, G. Sulz, and C. Hoffmann, “Evanescent field sensors based on tantalum pentoxide waveguides- a review,” Sensors 8, 711–738 (2008). [CrossRef]
  4. C. Kappel, A. Selle, T. Fricke-Begemann, M. A. Bader, and G. Marowsky, “Giant enhancement of two-photon fluorescence induced by resonant double grating waveguide structures,” Appl. Phys. B: Lasers Opt. 79, 531–534 (2004). [CrossRef]
  5. G. L. Duveneck, M. A. Bopp, M. Ehrat, M. Haiml, U. Keller, M. A. Bader, G. Marowsky, and S. Soria, “Evanescent-field-induced two-photon fluorescence: excitation of macroscopic areas of planar waveguides,” Appl. Phys. B: Lasers Opt. 73, 869–871 (2001). [CrossRef]
  6. J. Extermann, L. Bonacina, E. Cuna, C. Kasparian, Y. Mugnier, T. Feurer, and J. P. Wolf, “Nanodoublers as deep imaging markers for multi-photon microscopy,” Opt. Express 17, 15342–15349 (2009). [CrossRef] [PubMed]
  7. C. L. Hsieh, R. Grange, Y. Pu, and D. Psaltis, “Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging,” Opt. Express 17, 2880–2891 (2009). [CrossRef] [PubMed]
  8. A. V. Kachynski, A. N. Kuzmin, M. Nyk, I. Roy, and P. N. Prasad, “Zinc oxide nanocrystals for nonresonant nonlinear optical microscopy in biology and medicine,” J. Phys. Chem. C 112, 10721–10724 (2008). [CrossRef]
  9. R. Grange, J. W. Choi, C. L. Hsieh, Y. Pu, A. Magrez, R. Smajda, L. Forro, and D. Psaltis, “Lithium niobate nanowires synthesis, optical properties, and manipulation,” Appl. Phys. Lett. 95, 143105 (2009). [CrossRef]
  10. L. Le Xuan, S. Brasselet, F. Treussart, J. F. Roch, F. Marquier, D. Chauvat, S. Perruchas, C. Tard, and T. Gacoin, “Balanced homodyne detection of second-harmonic generation from isolated subwavelength emitters,” Appl. Phys. Lett. 89, 121118 (2006). [CrossRef]
  11. J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Galez, and J. P. Wolf, “Nano-frog: Frequency resolved optical gating by a nanometric object,” Opt. Express 16, 10405–10411 (2008). [CrossRef] [PubMed]
  12. P. Wnuk, L. Le Xuan, A. Slablab, C. Tard, S. Perruchas, T. Gacoin, J. F. Roch, D. Chauvat, and C. Radzewicz, “Coherent nonlinear emission from a single ktp nanoparticle with broadband femtosecond pulses,” Opt. Express 17, 4652–4658 (2009). [CrossRef] [PubMed]
  13. J. Extermann, P. Béjot, L. Bonacina, Y. Mugnier, R. Le Dantec, T. Mazingue, C. Galez, and J. Wolf, “An inexpensive nonlinear medium for intense ultrabroadband pulse characterization,” Appl. Phys. B 97, 537–540 (2009). [CrossRef]
  14. Y. Shen, J. Swiatkiewicz, J. Winiarz, P. Markowicz, and P. N. Prasad, “Second-harmonic and sum-frequency imaging of organic nanocrystals with photon scanning tunneling microscope,” Appl. Phys. Lett. 77, 2946 (2000). [CrossRef]
  15. J. Jasny and J. Sepiol, “Single molecules observed by immersion mirror objective. a novel method of finding the orientation of a radiating dipole,” Chem. Phys. Lett. 273, 439–443 (1997). [CrossRef]
  16. M. Bohmer and J. Enderlein, “Orientation imaging of single molecules by wide-field epifluorescence microscopy,” J. Opt. Soc. Am. B 20, 554–559 (2003). [CrossRef]
  17. 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]
  18. J. I. Dadap, “Optical second-harmonic scattering from cylindrical particles,” Phys. Rev. B 78, 205322 (2008). [CrossRef]
  19. 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). [CrossRef] [PubMed]
  20. L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J. P. Wolf, “Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy,” Appl. Phys. B: Lasers Opt. 87, 399–403 (2007). [CrossRef]
  21. S. W. Liu, H. J. Zhou, A. Ricca, R. Tian, and M. Xiao, “Far-field second-harmonic fingerprint of twinning in single ZnO rods,” Phys. Rev. B 77, 113311 (2008). [CrossRef]
  22. J. Steyer and W. Almers, “Tracking single secretory granules in live chromaffin cells by evanescent-field fluorescence microscopy,” Biophys. J. 76, 2262–2271 (1999). [CrossRef] [PubMed]

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