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Wavefront shaping is a powerful method to refocus light through a scattering medium. Its application to large spectral bandwidths or multiple wavelengths refocusing for nonlinear bio-imaging in-depth is however limited by spectral decorrelations. In this work, we demonstrate ways to access a large spectral memory of a refocus in thin scattering media and thick forward-scattering biological tissues. First, we show that the accessible spectral bandwidth through a scattering medium involves an axial spatio-spectral coupling, which can be minimized when working in a confocal geometry. Second, we show that this bandwidth can be further enlarged when working in a broadband excitation regime. These results open important prospects for multispectral nonlinear imaging through scattering media. more...

We report a detailed investigation on the second harmonic generation (SHG) emission from single 150 nm diameter non-centrosymmetric gold nanoparticles. Polarization-resolved analysis together with scanning electron microscopy images shows that these nanostructures exhibit a unique polarization-sensitive SHG that depends strongly on the particle's shape. An analytical approach based on multipolar analysis is introduced to link SHG properties to the nanoparticles' shape. Those multipolar modes can be probed using polarization-resolved SHG. This multipolar analysis offers a physical picture of the relation between shape (size, symmetries, defects, etc.) and nonlinear polarized optical efficiency. more...

Fluorescence microscopy is widely used in biological imaging, however scattering from tissues strongly limits its applicability to a shallow depth. In this work we adapt a methodology inspired from stellar speckle interferometry, and exploit the optical memory effect to enable fluorescence microscopy through a turbid layer. We demonstrate efficient reconstruction of micrometer-size fluorescent objects behind a scattering medium in epi-microscopy, and study the specificities of this imaging modality (magnification, field of view, resolution) as compared to traditional microscopy. Using a modified phase retrieval algorithm to reconstruct fluorescent objects from speckle images, we demonstrate robust reconstructions even in relatively low signal to noise conditions. This modality is particularly appropriate for imaging in biological media, which are known to exhibit relatively large optical memory ranges compatible with tens of micrometers size field of views, and large spectral bandwidths compatible with emission fluorescence spectra of tens of nanometers widths. more...

Polarization resolved nonlinear microscopy (PRNM) is a powerful technique to gain microscopic structural information in biological media. However, deep imaging in a variety of biological specimens is hindered by light scattering phenomena, which not only degrades the image quality but also affects the polarization state purity. In order to quantify this phenomenon and give a framework for polarization resolved microscopy in thick scattering tissues, we develop a characterization methodology based on four wave mixing (FWM) process. More specifically, we take advantage of two unique features of FWM, meaning its ability to produce an intrinsic in-depth local coherent source and its capacity to quantify the presence of light depolarization in isotropic regions inside a sample. By exploring diverse experimental layouts in phantoms with different scattering properties, we study systematically the influence of scattering on the nonlinear excitation and emission processes. The results show that depolarization mechanisms for the nonlinearly generated photons are highly dependent on the scattering center size, the geometry used (epi/forward) and, most importantly, on the thickness of the sample. We show that the use of an un-analyzed detection makes the polarization-dependence read-out highly robust to scattering effects, even in regimes where imaging might be degraded. The effects are illustrated in polarization resolved imaging of myelin lipid organization in mouse spinal cords. more...

We report spatial and vectorial imaging of local fields' confinement properties in metal nanoparticles with branched shapes, using Second Harmonic Generation (SHG) microscopy. Taking advantage of the coherent nature of this nonlinear process, the technique provides a direct evidence of the coupling between the excitation polarization and both localization and polarization specificities of local fields at the sub-diffraction scale. These combined features, which are governed by the nanoparticles' symmetry, are not accessible using other contrasts such as linear optical techniques or two-photon luminescence. more...

We present theoretical and experimental demonstrations of the electro-optic activity in crystalline molecular thin films with octupolar D(3h) symmetry. Applying a longitudinal electric field modulation within the molecular plane, we analyze the induced refractive index change relative to the orientation of the octupoles in their plane, and show that a maximum value is reached when one octupolar branch lies along the direction of the modulating field. These characteristics, as well as their electric field dependence, are drastically different from more traditional one-dimensional symmetry samples, bringing additional advantages related to electro-optic coupling possibilities. more...

We present a global analysis of experimental factors affecting polarization responses in two-photon inverted microscopy. The role of reflection optics and high numerical aperture focusing is investigated in two-photon fluorescence, which can be extended to other nonlinear processes. We show that both effects strongly distort polarization responses and can lead to misleading extraction of molecular order information from polarimetric measurements. We describe a model accounting for these effects and develop a calibration technique for the determination of polarization parameters in the sample plane using two-photon fluorescence polarimetry in liquids. more...

We demonstrate spatially resolved polarization encoding of nonlinear information by all-optical poling of photoisomerizable and nonlinear molecules in polymer films. The second harmonic generation (SHG)polarization responses of the photo-induced patterns are imaged by a nonlinear microscope with 2 microm lateral resolution. The strong SHG dependence to the poling fields polarizations is applied to information encoding, with a potential in high density optical data storage. In addition, the imprinted local nonlinear susceptibilities of multipolar symmetries cannot be deciphered by more traditional one-photon holography techniques. more...