SearcharxivSearch

arXiv subjects

Sophie Brasselet

Publications and source records attributed to Sophie Brasselet.

18 recordsLinked to original sources

3D Stokes polarimetric imaging at nanoscales

Optical fields polarized along three dimensions are frequent in optical microscopy and nanophotonics, and yet retrieving their polarization distribution is challenging. We present the experimental implementation of three-dimensional (3D) Stokes polarimetric imaging of nonparaxial optical fields with nanoscale spatial resolution. This approach extends classical Stokes polarimetry (traditionally limited to paraxial fields) into the nonparaxial regime. We use an array of gold nanospheres, each acting as a localized electric dipolar scatterer, to probe 3D polarization states over a field of view of tens of micrometers. The scattered signal is collected by a high numerical aperture objective lens and separated into its circular polarization components, providing a very simple imaging system. We introduce a computational algorithm to efficiently extract the physical parameters from the generated dipole spread functions with a high throughput across the whole field of view. Finally, we show that this method can also be applied to single-molecule localization and orientation fluorescence microscopy.

physics.optics

Periodic skyrmionic textures via conformal cartographic projections

We find periodic skyrmionic textures via conformal cartographic projections that map either an entire spherical parameter space or a hemisphere onto every regular polygon that provides regular tessellations of the plane. These textures minimize the energy inherent to the mapping and preserve the sign of the Skyrme density throughout the entire space. We show that 2D spinor fields (e.g., 2D polarization) that present periodic textures preserving the sign of the Skyrme density, unavoidably exhibit zeros. We implement these textures in the polarization state of a laser beam.

physics.optics

Propagation-invariant optical meron lattices

We introduce and produce experimentally optical beams exhibiting periodic skyrmionic polarization lattices at each transverse plane of propagation. These textures are meron lattices formed by tiles mapping hemispheres of the Poincaré sphere. All presented fields are combinations of a small number of plane waves. Firstly, we propose square lattices with a Skyrme density (the Jacobian of the mapping between the Poincaré sphere and physical space) that oscillates in sign but whose intensity distribution is constant. Secondly, we present triangular lattices preserving the Skyrme density's sign. Both lattices are invariant under propagation. Finally, we introduce a family of lattices with uniform Skyrme density sign, composed of square tiles that map to the same hemisphere of the Poincaré sphere. In these lattices, the polarization state undergoes a uniform local periodic rotation during propagation, thus preserving the texture's Skyrme density distribution.

physics.optics

Vectorial phase retrieval in super-resolution polarization microscopy

In single molecule orientation localization microscopy, valuable information about the orientation and longitudinal position of each molecule is often encoded in the shape of the point spread function (PSF). This shape, though, can be affected significantly by aberrations and other imperfections in the imaging system, leading to erroneous estimation of the measured parameters. A basic solution is to model the aberrations as a scalar mask in the pupil plane that is characterized through phase retrieval algorithms. However, this approach is not suitable for cases involving polarization-dependent aberrations, introduced either through unintentional anisotropy in the elements or by using birefringent masks for PSF shaping. Here, this problem is addressed by introducing a fully vectorial model in which the polarization aberrations are represented via a spatially-dependent Jones matrix, commonly used to describe polarization-dependent elements. It is then shown that these aberrations can be characterized from a set of PSF measurements at varying focal planes and for various polarization projections. This PZ-stack of PSFs, which contains both phase and polarization projection diversity, is used in a phase retrieval algorithm based on nonlinear optimization to determine the aberrations. This methodology is demonstrated with numerical simulations and experimental measurements. The pyPSFstack software developed for the modeling and characterization is made freely available.

physics.optics

Using fluorescent beads to emulate single flurophores

In this work, we study the conditions under which fluorescent beads can be used to emulate single fluorescent molecules in the calibration of optical microscopes. Although beads are widely used due to their brightness and easy manipulation, there can be notable differences between the point spread functions (PSFs) they produce and those for single-molecule fluorophores, caused by their different emission pattern and their size. We study theoretically these differences for various scenarios, e.g. with or without polarization channel splitting, to determine the conditions under which the use of beads as a model for single molecules is valid. We also propose methods to model the blurring due to the size difference and compensate for it to produce PSFs that are more similar to those for single molecules.

physics.optics

DNA self-assembly of single molecules with deterministic position and orientation

An ideal nanofabrication method should allow the organization of nanoparticles and molecules with nanometric positional precision, stoichiometric control and well-defined orientation. The DNA origami technique has evolved into a highly versatile bottom-up nanofabrication methodology that fulfils almost all of these features. It enables the nanometric positioning of molecules and nanoparticles with stoichiometric control, and even the orientation of asymmetrical nanoparticles along predefined directions. However, orienting individual molecules has been a standing challenge, mainly due to unspecific electrostatic interactions. Here, we show how single molecules, namely Cy5 and Cy3 fluorophores, can be incorporated in a DNA origami with controlled orientation by doubly linking them to oligonucleotide strands that are hybridized while leaving enough unpaired bases to induce a stretching force. Particularly, we explore the effects of leaving 0, 2, 4, 6, and 8 unpaired bases and find extreme orientations for 0 and 8 unpaired bases, corresponding to the molecules being perpendicular and parallel to the DNA double helix, respectively. We foresee that these results will expand the application field of DNA origami towards the fabrication of nanodevices involving a wide range of orientation-dependent molecular interactions, such as energy transfer, intermolecular electron transport, catalysis, exciton delocalization, or the electromagnetic coupling of a molecule to specific resonant nano-antennas modes.

cond-mat.soft

Roadmap on Wavefront Shaping and deep imaging in complex media

The last decade has seen the development of a wide set of tools, such as wavefront shaping, computational or fundamental methods, that allow to understand and control light propagation in a complex medium, such as biological tissues or multimode fibers. A vibrant and diverse community is now working on this field, that has revolutionized the prospect of diffraction-limited imaging at depth in tissues. This roadmap highlights several key aspects of this fast developing field, and some of the challenges and opportunities ahead.

physics.optics

Birefringent Fourier filtering for single molecule Coordinate and Height super-resolution Imaging with Dithering and Orientation

Super-resolution imaging based on single molecule localization allows accessing nanometric-scale information in biological samples with high precision. However, complete measurements including molecule orientation are still challenging. Orientation is intrinsically coupled to position in microscopy imaging, and molecular wobbling during the image integration time can bias orientation measurements. Providing 3D molecular orientation and orientational fluctuations can offer new ways to assess the degree of alignment of protein structures, which cannot be monitored by pure localization. Here we demonstrate that by adding polarization control to phase control in the Fourier plane of the imaging path, all parameters can be determined unambiguously from single molecules: 3D spatial position, 3D orientation and wobbling or dithering angle. The method, applied to fluorescent labels attached to single actin filaments, provides precisions within tens of nanometers in position and few degrees in direction.

physics.optics

Coherent anti-Stokes Raman scattering through thick biological tissues by single wavefront shaping

Coherent Anti Stokes Raman Scattering (CARS) offers many advantages for nonlinear bio-imaging, thanks to its sub-cellular spatial resolution and unique chemical specificity. Its working principle requires two incident pulsed laser beams with distinct frequencies to be focused in space and time, which focus quality however rapidly deteriorates when propagating at large depths in biological tissues. The depth limits of CARS and the capability of wavefront correction to overcome these limits are currently unknown. In this work we exploit the spectral correlation properties of the transmission matrix of a scattering medium in a pulsed regime, to recover coherent focusing for two distant incident CARS wavelengths which propagation is initially uncorrelated. Using wavefront shaping with a single spatial light modulator, we recover CARS generation through thick mice spinal cord tissues where initially no signal is measurable due to scattering, and demonstrate point scanning over large field of views of tens of micrometers.

physics.optics

Focusing large spectral bandwidths through scattering media

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.

physics.optics

Manipulating the transmission matrix of scattering media for nonlinear imaging beyond the memory effect

The measurement of the Transmission Matrix (TM) of a scattering medium is of great interest for imaging. It can be acquired directly by interferometry using an internal reference wavefront. Unfortunately, internal reference fields are scattered by the medium which results in a speckle that makes the TM measurement heterogeneous across the output field of view. We demonstrate how to correct for this effect using the intrinsic properties of the TM. For thin scattering media, we exploit the memory effect of the medium and the reference speckle to create a corrected TM. For highly scattering media where the memory effect is negligible, we use complementary reference speckles to compose a new TM, not compromised by the speckled reference anymore. Using this correction, we demonstrate large field of view second harmonic generation imaging through thick biological media.

physics.optics

Wide field fluorescence epi-microscopy behind a scattering medium enabled by speckle correlations

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.

physics.optics

Enhanced nonlinear imaging through scattering media using transmission matrix based wavefront shaping

Despite the tremendous progresses in wavefront control through or inside complex scattering media, several limitations prevent reaching practical feasibility for nonlinear imaging in biological tissues. While the optimization of nonlinear signals might suffer from low signal to noise conditions and from possible artifacts at large penetration depths, it has nevertheless been largely used in the multiple scattering regime since it provides a guide star mechanism as well as an intrinsic compensation for spatiotemporal distortions. Here, we demonstrate the benefit of Transmission Matrix (TM) based approaches under broadband illumination conditions, to perform nonlinear imaging. Using ultrashort pulse illumination with spectral bandwidth comparable but still lower than the spectral width of the scattering medium, we show strong nonlinear enhancements of several orders of magnitude, through thicknesses of a few transport mean free paths, which corresponds to millimeters in biological tissues. Linear TM refocusing is moreover compatible with fast scanning nonlinear imaging and potentially with acoustic based methods, which paves the way for nonlinear microscopy deep inside scattering media.

physics.optics

Direct imaging of molecular symmetry by coherent anti-Stokes Raman scattering

Nonlinear optical methods, such as coherent anti-Stokes Raman scattering (CARS) and stimulated Raman scattering (SRS), are able to perform label free imaging, with chemical bonds specificity. Here, we demonstrate that the use of circularly polarized light allows to retrieve not only the chemical nature but also the symmetry of the probed sample, in a single shot measurement. Our symmetry-resolved scheme offers simple access to the local organization of vibrational bonds and as a result provides enhanced image contrast for anisotropic samples as well as an improved chemical selectivity. We quantify the local organization of vibrational bonds on crystalline and biological samples, thus providing new information not accessible by spontaneous Raman and SRS techniques. This work stands for a novel symmetry-resolved contrast in vibrational microscopy, with potential application in biological diagnostic.

physics.optics

Polarization-resolved microscopy through scattering media via wavefront shaping

Wavefront shaping has revolutionized imaging deep in scattering media, being able to spatially and temporally refocus light through or inside the medium. However, wavefront shaping is not compatible yet with polarization-resolved microscopy given the need of polarizing optics to refocus light with a controlled polarization state. Here, we show that wavefront shaping is not only able to restore a focus, but it can also recover the injected polarization state without using any polarizing optics at the detection. This counter-intuitive effect occurs up to several transport mean free path thick samples, which exhibit a speckle with a completely scrambled state. Remarkably, an arbitrary rotation of the input polarization does not degrade the quality of the focus. This unsupervised re-polarization - out of the originally scrambled polarization state - paves the way for polarization-resolved structural microscopy at unprecedented depths. We exploit this phenomenon and demonstrate second harmonic generation (SHG) structural imaging of collagen fibers in tendon tissues behind a scattering medium.

physics.optics

Balanced homodyne detection in second-harmonic generation microscopy

We demonstrate the association of two-photon nonlinear microscopy with balanced homodyne detection for investigating second harmonic radiation properties at nanoscale dimensions. Variation of the relative phase between second-harmonic and fundamental beams is retrieved, as a function of the absolute orientation of the nonlinear emitters. Sensitivity down to approximately 3.2 photon/s in the spatio-temporal mode of the local oscillator is obtained. This value is high enough to efficiently detect the coherent second-harmonic emission from a single KTiOPO4 crystal of sub-wavelength size.

physics.optics

In-situ diagnostics of the crystalline nature of single organic nanocrystals by nonlinear microscopy

We elucidate the crystalline nature and the three-dimensional orientation of isolated organic nanocrystals embedded in a sol-gel matrix, using a polarized nonlinear microscopy technique that combines two-photon fluorescence and second harmonic generation. This technique allows the distinction between mono-crystalline structures and nano-scale poly-crystalline aggregates responsible for incoherent second harmonic signals.

cond-mat.mtrl-sci

Monitoring of Orientation in Molecular Ensembles by Polarization Sensitive Nonlinear Microscopy

We present high resolution two-photon excitation microscopy studies combining two-photon fluorescence (TPF) and second harmonic generation (SHG) in order to probe orientational distributions of molecular ensembles at room temperature. A detailed polarization analysis of TPF and SHG signals is used in order to unravel the parameters of the molecular orientational statistical distribution, using a technique which can be extended and generalized to a broad variety of molecular arrangements. A polymer film containing molecules active for TPF and/or SHG emission is studied as a model system. Polarized TPF is shown to provide information on specific properties pertaining to incoherent emission in molecular media, such as excitation transfer. SHG, being highly sensitive to a slight departure from centrosymmetry such as induced by an external electric field in the medium, complements TPF. The response of each signal to a variable excitation polarization allows investigation of molecular behavior in complex environments which affect their orientations and interactions.

cond-mat.soft