Electro-optical Pockels scattering from a single nanocrystal.

The electro-optical Pockels response from a single non-centrosymmetric nanocrystal is reported. High sensitivity to the weak electric-field dependent nonlinear scattering is achieved through a dedicated imaging interferometric microscope and the linear dependence of electro-optical signal upon the applied field is checked. Using different incident light polarization states, a priori random spatial orientation of the crystal can be inferred. The electro-optical response from a nanocrystal provides local subwavelength sensor of quasi-static electric fields with potential applications in physics and biology. It also leads to a new sub-wavelength microscopy towards the nanoscale investigation of interesting phenomena such as nanoferroelectricity.

Nanoengineering the second order susceptibility in semiconductor quantum dot heterostructures.

We study second-harmonic generation from single CdTe/CdS core/shell rod-on-dot nanocrystals with different geometrical parameters, which allow to fine tune the nonlinear properties of the nanostructure. These hybrid semiconductor-semiconductor nanoparticles exhibit extremely strong and stable second-harmonic emission, although the size of CdTe core is still within the strong quantum confinement regime. The orientation sensitive polarization response is analyzed by means of a pointwise additive model of the third-order tensors associated to the nanoparticle components. These findings prove that engineering of semiconducting complex heterostructures at the single nanoparticle scale can lead to extremely bright nanometric nonlinear light sources.

Enhanced detection of fluorescent nanospheres using two-channel radially polarized surface plasmon microscopy.

We detected single dye-stained latex nanospheres as small as 20 nm using a two-detection channel modified surface plasmon microscope. We found that a radially polarized incident beam leading to excitation of well-focused surface plasmons induces both fluorescence and elastic linear scattering from the spheres. The two complementary emitted signals were detected in parallel by the two separated channels, leading to well-colocalized images. We obtained high spatial resolutions for both channels down to 250 nm in the lateral direction and 300 nm along the longitudinal axis. We believe this multimodal microscope can be useful to track nano objects and to compensate for intermittent fluorescence, thanks to a permanently activated parallel scattering detection channel.

Polarization-sensitive two-photon microscopy study of the organization of liquid-crystalline DNA.

Highly concentrated DNA solutions exhibit self-ordering properties such as the generation of liquid-crystalline phases. Such organized domains may play an important role in the global chromatin topology but can also be used as a simple model for the study of more complex 3D DNA structures. In this work, using polarized two-photon fluorescence microscopy, we report on the orientation of DNA molecules in liquid-crystalline phases. For this purpose, we analyze the signal emitted by fluorophores that are noncovalently bound to DNA strands. In nonlinear processes, excitation occurs exclusively in the focal volume, which offers advantages such as the reduction of photobleaching of out-of-focus molecules and intrinsic 3D sectioning capability. Propidium iodide and Hoechst, two fluorophores with different DNA binding modes, have been considered. Polarimetric measurements show that the dyes follow the alignment with respect to the DNA strands and allow the determination of the angles between the emission dipoles and the longitudinal axis of the DNA double strand. These results provide a useful starting point toward the application of two-photon polarimetry techniques to determine the local orientation of condensed DNA in physiological conditions.

Electro-optical imaging microscopy of dye-doped artificial lipidic membranes.

Artificial lipidic bilayers are widely used as a model for the lipid matrix in biological cell membranes. We use the Pockels electro-optical effect to investigate the properties of an artificial lipidic membrane doped with nonlinear molecules in the outer layer. We report here what is believed to be the first electro-optical Pockels signal and image from such a membrane. The electro-optical dephasing distribution within the membrane is imaged and the signal is shown to be linear as a function of the applied voltage. A theoretical analysis taking into account the statistical orientation distribution of the inserted dye molecules allows us to estimate the doped membrane nonlinearity. Ongoing extensions of this work to living cell membranes are discussed.

Second-harmonic generation from a single core/shell quantum dot.

Nanoparticles emitting two-photon luminescence are broadly used as photostable emitters for nonlinear microscopy. Second-harmonic generation (SHG) as another two-photon mechanism offers complementary optical properties but the reported sizes of nanoparticles are still large, of a few tens of nanometers. Herein, coherent SHG from single core/shell CdTe/CdS nanocrystals with a diameter of 10 to 15 nm is reported. The nanocrystal excitation spectrum reveals resonances in the nonlinear efficiency with an overall maximum at about 970 nm. Polarization analysis of the second-harmonic emission confirms the expected zinc blende symmetry, and allows extraction of the three-dimensional nanocrystal orientation. The small size of these nonlinearly active quantum dots, together with the intrinsic coherence and orientation sensitivity of the SHG process, are well adapted for ultrafast probing of optical near-fields with high resolution as well as for orientation tracking for bioimaging applications.

Coherent nonlinear emission from a single KTP nanoparticle with broadband femtosecond pulses.

We demonstrate that the intensity of the second harmonic (SH) generated in KTiOPO(4) nanoparticles excited with femtosecond laser pulses increases with decreasing duration of the infrared pump pulses. The SH intensity scales, approximately, as the inverse of the laser pulse duration ranging between 13 fs and 200 fs. The SH intensity enhancement requires careful compensation of the high-order spectral phase, being achieved with a genetic algorithm. Using ultrashort laser pulses improves the signal-to-noise ratio and will allow the detection of 10-nm size particles. Finally, we demonstrate that the spectrum of broadband (100 nm) pulses can be shaped to generate non-degenerate sum-frequency mixing. This opens up access to the polarization degrees of freedom of this second-order nonlinear process at the nanoscale.

Single KTP nanocrystals as second-harmonic generation biolabels in cortical neurons.

We report an efficient colloidal synthesis of KTiOPO4 (KTP) nanocrystals with excellent crystallinity and the direct observation of optical second-harmonic generation (SHG) from discrete KTP nanocrystals in neurons cultured from mammalian brain cortex. Direct internalization and monitoring of these nanoparticles was successfully achieved without limitations from cytotoxicity, bleaching and blinking emission.

Liquid crystal phases of DNA: evaluation of DNA organization by two-photon fluorescence microscopy and polarization analysis.

We report on the investigation of the structure of DNA liquid crystal (LC) phases by means of polarization sensitive two-photon microscopy (PSTPM). DNA was stained with fluorescent dyes, an intercalator propidium iodide, or a groove binder Hoechst 3342, and the angular dependence of the intensity of two-photon excited fluorescence emitted by the dye was collected. The local orientation of DNA molecules in cholesteric and columnar LC phases was established on the basis of the relative angle between the transition dipole of the dye and the long axis of DNA helix. Three-dimensional images of the cholesteric phase were obtained making use of the intrinsic 3D resolving ability of two-photon microscopy. We also discuss the influence of dyes on the parameters of DNA LC phases and comment on advantages and limitations of the PSTPM technique in comparison with other LC characterization techniques.

Nonequivalence of spatial shifts and Wigner delays at interfaces.

We isolate spatial shifts and Wigner delays for reflection at the same interface and demonstrate that they can carry different information. The spatial shifts associated with Wood anomalies on gratings can be either positive or negative, while the corresponding delays are both positive. In the standard case of total reflection at a glass-air interface, a differential two-photon absorption correlation technique allows us to measure for the first time a delay of up to 35 fs in agreement with the associated 10.5 microm spatial shift. The method also allows us to isolate giant Wigner delays. The existence of similar delays in different areas of physics is discussed.

Continuous-wave tunnel ring fiber laser.

The continuous-wave oscillation of a tunnel ring fiber laser is demonstrated. The high losses encountered in tunneling systems are compensated for by a high-gain amplifying medium from barrier widths for 0 to lambda/2. The experimental observations are in good agreement with a simple theoretical model. This near-field probe system allows one to detect small displacements in the picometer range.

Jamin Fabry-Perot interferometer.

A novel type of interferometer was designed and tested experimentally. It combines the advantages of the spatial path separation used in the two-wave polarized Jamin interferometer and the high sensitivity that characterizes the multiwave Fabry-Perot interferometer. Furthermore, when it is sandwiched between crossed polarizers it shows a sensitivity to intracavity anisotropies that is proportional to the square of the Fabry-Perot interferometer's finesse.