On the maximization of entropy in the process of thermalization of highly multimode nonlinear beams.

We present a direct experimental confirmation of the maximization of entropy which accompanies the thermalization of a highly multimode light beam, upon its nonlinear propagation in standard graded-index (GRIN) optical fibers.

Single-Photon Level Dispersive Fourier Transform: Ultrasensitive Characterization of Noise-Driven Nonlinear Dynamics.

Dispersive Fourier transform is a characterization technique that allows directly extracting an optical spectrum from a time domain signal, thus providing access to real-time characterization of the signal spectrum. However, these techniques suffer from sensitivity and dynamic range limitations, hampering their use for special applications in, e.g., high-contrast characterizations and sensing. Here, we report on a novel approach to dispersive Fourier transform-based characterization using single-photon detectors. In particular, we experimentally develop this approach by leveraging mutual information analysis for signal processing and hold a performance comparison with standard dispersive Fourier transform detection and statistical tools. We apply the comparison to the analysis of noise-driven nonlinear dynamics arising from well-known modulation instability processes. We demonstrate that with this dispersive Fourier transform approach, mutual information metrics allow for successfully gaining insight into the fluctuations associated with modulation instability-induced spectral broadening, providing qualitatively similar signatures compared to ultrafast photodetector-based dispersive Fourier transform but with improved signal quality and spectral resolution (down to 53 pm). The technique presents an intrinsically unlimited dynamic range and is extremely sensitive, with a sensitivity reaching below the femtowatt (typically 4 orders of magnitude better than ultrafast dispersive Fourier transform detection). We show that this method can not only be implemented to gain insight into noise-driven (spontaneous) frequency conversion processes but also be leveraged to characterize incoherent dynamics seeded by weak coherent optical fields.

GaAs-chip-based mid-infrared supercontinuum generation.

The mid-infrared spectral region opens up new possibilities for applications such as molecular spectroscopy with high spatial and frequency resolution. For example, the mid-infrared light provided by synchrotron sources has helped for early diagnosis of several pathologies. However, alternative light sources at the table-top scale would enable better access to these state-of-the-art characterizations, eventually speeding up research in biology and medicine. Mid-infrared supercontinuum generation in highly nonlinear waveguides pumped by compact fiber lasers represents an appealing alternative to synchrotrons. Here, we introduce orientation-patterned gallium arsenide waveguides as a new versatile platform for mid-infrared supercontinuum generation. Waveguides and fiber-based pump lasers are optimized in tandem to allow for the group velocities of the signal and the idler waves to match near the degeneracy point. This configuration exacerbates supercontinuum generation from 4 to 9 µm when waveguides are pumped at 2750 nm with few-nanojoule energy pulses. The brightness of the novel mid-infrared source exceeds that of the third-generation synchrotron source by a factor of 20. We also show that the nonlinear dynamics is strongly influenced by the choice of waveguide and laser parameters, thus offering an additional degree of freedom in tailoring the spectral profile of the generated light. Such an approach then opens new paths for high-brightness mid-infrared laser sources development for high-resolution spectroscopy and imaging. Furthermore, thanks to the excellent mechanical and thermal properties of the waveguide material, further power scaling seems feasible, allowing for the generation of watt-level ultra-broad frequency combs in the mid-infrared.

High-temperature wave thermalization spoils beam self-cleaning in nonlinear multimode GRIN fibers.

In our experiments, we reveal a so-far unnoticed power limitation of beam self-cleaning in graded-index nonlinear multimode optical fibers. As the optical pulse power is progressively increased, we observed that the initial Kerr-induced improvement of the spatial beam quality is eventually lost. Based on a holographic mode decomposition of the output field, we show that beam spoiling is associated with high-temperature wave thermalization, which depletes the fundamental mode in favor of a highly multimode power distribution.

Modal phase-locking in multimode nonlinear optical fibers.

Spatial beam self-cleaning, a manifestation of the Kerr effect in graded-index multimode fibers, involves a nonlinear transfer of power among modes, which leads to robust bell-shaped output beams. The resulting mode power distribution can be described by statistical mechanics arguments. Although the spatial coherence of the output beam was experimentally demonstrated, there is no direct study of modal phase evolutions. Based on a holographic mode decomposition method, we reveal that nonlinear spatial phase-locking occurs between the fundamental and its neighboring low-order modes, in agreement with theoretical predictions. As such, our results dispel the current belief that the spatial beam self-cleaning effect is the mere result of a wave thermalization process.

Efficient second-harmonic generation through cascaded optically poled fibers.

We report the experimental demonstration of efficient second-harmonic generation by splicing optically poled fiber segments. A device made from five segments each 20 cm-long exhibits, at a fundamental average power of 4.2 mW, a maximum increase of 5.5 in the conversion efficiency with respect to a single 20 cm poled fiber, corresponding to a conversion efficiency of 5.4%. For any considered fundamental power, the conversion efficiency at the output of a five-segment device is larger than the efficiency of a single poled fiber having the same length.

Multimode solitons in step-index fibers.

We experimentally generate multimode solitons in step-index fibers, where nonlinearity compensates for both chromatic and modal dispersion. These solitons are subject to Raman self-frequency shift, and their energy is gradually transfered to the fundamental fiber mode. We compare multimode soliton dynamics in both step-index and graded index fibers, in excellent agreement with numerical predictions.

Spatial beam reshaping and large-band nonlinear conversion in rectangular-core phosphate glass fibers.

Here we present the ability of Nd3+-doped zinc-phosphate glasses to be shaped into rectangular core fibers. At first, the physico-chemical properties of the developed P2O5-based materials are investigated for different concentrations of neodymium oxide and core and cladding glass compositions are selected for further fiber development. A modified stack-and-draw technique is used to produce multimode large rectangular-core optical fibers. Self-guided nonlinear effects acting as spatial beam reshaping processes occurring in these newly-developed photonic structures lead to the generation of spectral broadenings in the visible and near-infrared spectral domains.

Spatiotemporal beam self-cleaning for high-resolution nonlinear fluorescence imaging with multimode fiber.

Beam self-cleaning (BSC) in graded-index (GRIN) multimode fibers (MMFs) has been recently reported by different research groups. Driven by the interplay between Kerr effect and beam self-imaging, BSC counteracts random mode coupling, and forces laser beams to recover a quasi-single mode profile at the output of GRIN fibers. Here we show that the associated self-induced spatiotemporal reshaping allows for improving the performances of nonlinear fluorescence (NF) microscopy and endoscopy using multimode optical fibers. We experimentally demonstrate that the beam brightness increase, induced by self-cleaning, enables two and three-photon imaging of biological samples with high spatial resolution. Temporal pulse shortening accompanying spatial beam clean-up enhances the output peak power, hence the efficiency of nonlinear imaging. We also show that spatiotemporal supercontinuum (SC) generation is well-suited for large-band NF imaging in visible and infrared domains. We substantiated our findings by multiphoton fluorescence imaging in both microscopy and endoscopy configurations.

Scaling of average power in sub-MW peak power Yb-doped tapered fiber picosecond pulse amplifiers.

Prospects for average power scaling of sub-MW output peak power picosecond fiber lasers by utilization of a Yb-doped tapered fiber at the final amplification stage were studied. In this paper, it was shown experimentally that a tapered fiber allows the achievement of an average power level of 150 W (limited by the available pump power) with a peak power of 0.74 MW for 22 ps pulses with no signs of transverse mode instability. Measurements of the mode content using the S2 technique showed a negligible level of high order modes (less than 0.3%) in the output radiation even for the maximum output power level. Our reliability tests predict no thermal issues during long-term operation (105 hours) of the developed tapered fiber laser up to kilowatt output average power levels.

Visualizing intra-medulla lipids in human hair using ultra-multiplex CARS, SHG, and THG microscopy.

We performed label-free imaging of human-hair medulla using multi-modal nonlinear optical microscopy. Intra-medulla lipids (IMLs) were clearly visualized by ultra-multiplex coherent anti-Stokes Raman scattering (CARS) spectroscopic imaging. Two groups of IMLs were found: second harmonic generation (SHG) active and inactive. By combining SHG analysis with CARS, the two groups were identified as free fatty acids and wax esters, respectively.

Coherent combining of self-cleaned multimode beams.

A low intensity light beam emerges from a graded-index, highly multimode optical fibre with a speckled shape, while at higher intensity the Kerr nonlinearity may induce a spontaneous spatial self-cleaning of the beam. Here, we reveal that we can generate two self-cleaned beams with a mutual coherence large enough to produce a clear stable fringe pattern at the output of a nonlinear interferometer. The two beams are pumped by the same input laser, yet are self-cleaned into independent multimode fibres. We thus prove that the self-cleaning mechanism preserves the beams' mutual coherence via a noise-free parametric process. While directly related to the initial pump coherence, the emergence of nonlinear spatial coherence is achieved without additional noise, even for self-cleaning obtained on different modes, and in spite of the fibre structural disorder originating from intrinsic imperfections or external perturbations. Our discovery may impact theoretical approaches on wave condensation, and open new opportunities for coherent beam combining.

Multiplex coherent anti-Stokes Raman scattering microspectroscopy detection of lipid droplets in cancer cells expressing TrkB.

For many years, scientists have been looking for specific biomarkers associated with cancer cells for diagnosis purposes. These biomarkers mainly consist of proteins located at the cell surface (e.g. the TrkB receptor) whose activation is associated with specific metabolic modifications. Identification of these metabolic changes usually requires cell fixation and specific dye staining. MCARS microspectroscopy is a label-free, non-toxic, and minimally invasive method allowing to perform analyses of live cells and tissues. We used this method to follow the formation of lipid droplets in three colorectal cancer cell lines expressing TrkB. MCARS images of cells generated from signal integration of CH2 stretching modes allow to discriminate between lipid accumulation in the endoplasmic reticulum and the formation of cytoplasmic lipid droplets. We found that the number of the latter was related to the TrkB expression level. This result was confirmed thanks to the creation of a HEK cell line which over-expresses TrkB. We demonstrated that BDNF-induced TrkB activation leads to the formation of cytoplasmic lipid droplets, which can be abolished by K252a, an inhibitor of TrkB. So, MCARS microspectroscopy proved useful in characterizing cancer cells displaying an aberrant lipid metabolism.

Nonlinear beam self-imaging and self-focusing dynamics in a GRIN multimode optical fiber: theory and experiments.

Beam self-imaging in nonlinear graded-index multimode optical fibers is of interest for many applications, such as implementing a fast saturable absorber mechanism in fiber lasers via multimode interference. We obtain a new exact solution for the nonlinear evolution of first and second order moments of a laser beam of arbitrary transverse shape carried by a graded-index multimode fiber. We have experimentally directly visualized the longitudinal evolution of beam self-imaging by means of femtosecond laser pulse propagation in both the anomalous and the normal dispersion regime of a standard telecom graded-index multimode optical fiber. Light scattering out of the fiber core via visible photo-luminescence emission permits us to directly measure the self-imaging period and the beam dynamics. Spatial shift and splitting of the self-imaging process under the action of self-focusing are also revealed.

Highly Transparent Fluorotellurite Glass-Ceramics: Structural Investigations and Luminescence Properties.

Crystallization from glass can lead to the stabilization of metastable crystalline phases, which offers an interesting way to unveil novel compounds and control the optical properties of resulting glass-ceramics. Here, we report on a crystallization study of the ZrF4-TeO2 glass system and show that under specific synthesis conditions, a previously unreported Te0.47Zr0.53OxFy zirconium oxyfluorotellurite antiglass phase can be selectively crystallized at the nanometric scale within the 65TeO2-35ZrF4 amorphous matrix. This leads to highly transparent glass-ceramics in both the visible and near-infrared ranges. Under longer heat treatment, the stable cubic ZrTe3O8 phase crystallizes in addition to the previous unreported antiglass phase. The structure, microstructure, and optical properties of 65TeO2-35ZrF4Tm3+-doped glass-ceramics, were investigated in detail by means of X-ray diffraction, scanning and transmission electron microscopies, and 19F, 91Zr, and 125Te NMR, Raman, and photoluminescence spectroscopies. The crystal chemistry study of several single crystals samples by X-ray diffraction evidence that the novel phase, derived from α-UO3 type, corresponds in terms of long-range ordering inside this basic hexagonal/trigonal disordered phase (antiglass) to a complex series of modulated microphases rather than a stoichiometric compound with various superstructures analogous to those observed in the UO3-U3O8 subsystem. These results highlight the peculiar disorder-order phenomenon occurring in tellurite materials.

Multiplex coherent anti-Stokes Raman scattering highlights state of chromatin condensation in CH region.

Coherent Raman microscopy has become a powerful tool in label-free, non-destructive and fast cell imaging. Here we apply high spectral resolution multiplex coherent anti-Stokes Raman scattering (MCARS) microspectroscopy in the high wavenumber region to the study of the cell cycle. We show that heterochromatin - the condensed state of chromatin - can be visualised by means of the vibrational signature of proteins taking part in its condensation. Thus, we are able to identify chromosomes and their movement during mitosis, as well as structures like nucleoli and nuclear border in interphase. Furthermore, the specific organization of the endoplasmic reticulum during mitosis is highlighted. Finally, we stress that MCARS can reveal the biochemical impact of the fixative method at the cellular level. Beyond the study of the cell cycle, this work introduces a label-free imaging approach that enables the visualization of cellular processes where chromatin undergoes rearrangements.

Characterization of Intra/Extracellular Water States Probed by Ultrabroadband Multiplex Coherent Anti-Stokes Raman Scattering (CARS) Spectroscopic Imaging.

Detailed knowledge of the water status in living organisms is crucial for understanding their physiology and pathophysiology. Here, we developed a technique to spectroscopically image water at high resolution using ultrabroadband multiplex coherent anti-Stokes Raman scattering (CARS) microscopy equipped with a supercontinuum light source. This system allows for the visualization of a wide spectrum of CARS signals from the fingerprint to the end of O-H stretching at a spectral resolution of ∼10 cm-1. Application of the system to living mammalian cells revealed a spectral red shift of the O-H stretching vibrational band inside compared to outside the cells, suggesting the existence of stronger hydrogen bonds inside the cells. Furthermore, potential changes in spectra were examined by adding mannitol to the extracellular solution, which increases the osmolality outside the cells and thereby induces dehydration of the cells. Under this treatment, the red shift of the O-H stretching band was further enhanced, revealing the effects of mannitol on water states inside the cells. The methodology developed here should serve as a powerful tool for the chemical imaging of water in living cells in various biological and medical contexts.

Nonlinear polarization dynamics of Kerr beam self-cleaning in a graded-index multimode optical fiber.

We experimentally study polarization dynamics of Kerr beam self-cleaning in a graded-index multimode optical fiber. We show that spatial beam cleaning is accompanied by nonlinear polarization rotation and a significant increase of the degree of linear polarization.

Nd3+-doped transparent tellurite ceramics bulk lasers.

We report on the laser emission of the polycrystalline ceramic obtained from the full and congruent crystallization of the parent glass 1Nd3+:75TeO2-12.5Bi2O3-12.5Nb2O5 composition. In particular, the current work underlines the importance of carefully controlling the heat treatment in order to solely crystallize the Bi0.8Nb0.8Te2.4O8 cubic phase and consequently avoid the formation of the BiNbTe2O8 orthorhombic phase that would be detrimental for optical purpose. The structure, microstructure and photoluminescence properties of the resulting transparent tellurite ceramics are characterized. The continuous-wave and gain-switching laser performances reveal that the emission remains perfectly single transversal mode in the range of pump powers explored. The maximum output power achieved was ~28.5 mW, for a pump power threshold of ~67 mW, and with associated efficiency and slope efficiency of ~22.5% and ~50%, respectively. These data definitely stand among the best results obtained so far for bulk laser tellurite materials and thus demonstrate the potential of such polycrystalline transparent ceramics as optically active materials. Finally, the laser emission characteristics in pulsed regime, at low and high repetition rates, are also provided: more than 6.5 W of peak power at a repetition rate of 728 kHz can be obtained.

Fast epi-detected broadband multiplex CARS and SHG imaging of mouse skull cells.

We present a bimodal imaging system able to obtain epi-detected mutiplex coherent anti-Stokes Raman scattering (M-CARS) and second harmonic generation (SHG) signals coming from biological samples. We studied a fragment of mouse parietal bone and could detect broadband anti-Stokes and SHG responses originating from bone cells and collagen respectively. In addition we compared two post-processing methods to retrieve the imaginary part of the third-order nonlinear susceptibility related to the spontaneous Raman scattering.