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Hilton B. de Aguiar

Publications and source records attributed to Hilton B. de Aguiar.

At least 19 recordsLinked to original sources
arXiv2026

High-resolution scanning fluorescence imaging through scattering via speckle replica alignment and variance computation

Fluorescence imaging is an essential diagnostic tool in many fields, but diffraction-limited optical imaging at depth is limited by scattering. Here, we present a method based on multiple random illuminations, combined with a computational framework that retrieves high-resolution images by aligning local speckle replicas and computing their pixel-wise variance. We demonstrate its versatility in two regimes: linear wide-field one-photon (1P) fluorescence imaging and nonlinear two-photon (2P) fluorescence imaging where the object is excited by a scanned speckle field and detected with a single-pixel detector. This approach outperforms standard autocorrelation techniques in terms of resolution and convergence.

physics.optics↗
arXiv2025

Three-dimensional holographic imaging of incoherent objects through scattering media

Three-dimensional (3D) high-resolution imaging is essential in microscopy, yet light scattering poses significant challenges in achieving it. Here, we present an approach to holographic imaging of spatially incoherent objects through scattering media, utilizing a virtual medium that replicates the scattering effects of the actual medium. This medium is constructed by retrieving mutually incoherent fields from the object, and exploiting the spatial correlations between them. By numerically propagating the incoherent fields through the virtual medium, we non-invasively compensate for scattering, achieving accurate 3D reconstructions of hidden objects. Experimental validation with fluorescent and synthetic incoherent objects confirms the effectiveness of this approach, opening new possibilities for advanced 3D high-resolution microscopy in scattering environments.

physics.optics↗
arXiv2024

Replica-assisted super-resolution fluorescence imaging in scattering media

Far-field super-resolution fluorescence microscopy has been rapidly developed for applications ranging from cell biology to nanomaterials. However, it remains a significant challenge to achieve super-resolution imaging at depth in opaque materials. In this study, we present a super-resolution microscopy technique for imaging hidden fluorescent objects through scattering media, started by exploiting the inherent object replica generation arising from the memory effect, i.e. the seemingly informationless emission speckle can be regarded as a random superposition of multiple object copies. Inspired by the concept of super-resolution optical fluctuation imaging, we use temporally-fluctuating speckles to excite fluorescent signals and perform high-order cumulant analysis on the fluctuation, which can not only improve the image resolution, but also increase the speckle contrast to isolate only the bright object replicas. A super-resolved image can be finally retrieved by simply unmixing the sparsely distributed replicas with their location map. This methodology allows to overcome scattering and achieve robust super-resolution fluorescence imaging, circumventing the need of heavy computational steps.

physics.optics↗
arXiv2023

Phase conjugation with spatially incoherent light in complex media

Shaping light deep inside complex media, such as biological tissue, is critical to many research fields. Although the coherent control of scattered light via wavefront shaping has made significant advances in addressing this challenge, controlling light over extended or multiple targets without physical access inside a medium remains elusive. Here we present a phase conjugation method for spatially incoherent light, which enables the non-invasive light control based on incoherent emission from multiple target positions. Our method characterizes the scattering responses of hidden sources by retrieving mutually incoherent scattered fields from speckle patterns. By time-reversing scattered fluorescence with digital phase conjugation, we experimentally demonstrate focusing of light on individual and multiple targets. We also demonstrate maximum energy delivery to an extended target through a scattering medium by exploiting transmission eigenchannels. This paves the way to control light propagation in complex media using incoherent contrasts mechanisms.

physics.optics↗
arXiv2023

Single-pixel transmission matrix recovery via 2-photon fluorescence

Imaging at depth in opaque materials has long been a challenge. Recently, wavefront shaping has enabled significant advance for deep imaging. Nevertheless, most non-invasive wavefront shaping methods require cameras, lack the sensitivity for deep imaging under weak optical signals, or can only focus on a single "guidestar". Here, we retrieve the transmission matrix (TM) non-invasively using two-photon fluorescence exploiting a general single-pixel detection framework, allowing to achieve single-target focus on multiple guidestars spread beyond the memory effect range. In addition, if we assume memory effect correlations exist in the transmission matrix, we are able to significantly reduce the number of measurements needed.

physics.optics↗
arXiv2022

Competing oxygen evolution reaction mechanisms revealed by high-speed compressive Raman imaging

Transition metal oxides are state-of-the-art materials for catalysing the oxygen evolution reaction (OER), whose slow kinetics currently limit the efficiency of water electrolysis. However, microscale physicochemical heterogeneity between particles, dynamic reactions both in the bulk and at the surface, and an interplay between particle reactivity and electrolyte makes probing the OER challenging. Here, we overcome these limitations by applying state-of-the-art compressive Raman imaging to uncover competing bias-dependent mechanisms for the OER in a solid electrocatalyst, α-Li2IrO3. By spatially and temporally tracking changes in the in- and out-of-plane Ir-O stretching modes - identified by density functional theory calculations - we follow catalytic activation and charge accumulation following ion exchange under a variety of electrolytes, particle compositions and cycling conditions. We extract velocities of phase fronts and demonstrate that at low overpotentials oxygen is evolved by the combination of an electrochemical-chemical mechanism and a classical electrocatalytic adsorbate mechanism, whereas at high overpotentials only the latter occurs. These results provide strategies to promote mechanisms for enhanced OER performances, and highlight the power of compressive Raman imaging for low-cost, chemically specific tracking of microscale reaction dynamics in a broad range of systems where ion and electron exchange can be coupled to structural changes, i.e. catalysts, battery materials, memristors, etc.

cond-mat.mtrl-sci↗
arXiv2022

Three-dimensional operando optical imaging of single particle and electrolyte heterogeneities inside Li-ion batteries

Understanding (de)lithiation heterogeneities in battery materials is key to ensuring optimal electrochemical performance and developing better energy storage devices. However, this remains challenging due to the complex three dimensional morphology of microscopic electrode particles, the involvement of both solid and liquid phase reactants, and range of relevant timescales (seconds to hours). Here, we overcome this problem and demonstrate the use of bench-top laser scanning confocal microscopy for simultaneous three-dimensional operando measurement of lithium ion dynamics in single particles, and the electrolyte, in batteries. We examine two technologically important cathode materials that are known to suffer from intercalation heterogeneities: LixCoO2 and LixNi0.8Mn0.1Co0.1O2. The single-particle surface-to-core transport velocity of Li-phase fronts, and volume changes - as well as their inter-particle heterogeneity - are captured as a function of C-rate, and benchmarked to previous ensemble measurements. Additionally, we visualise heterogeneities in the bulk and at the surface of particles during cycling, and image the formation of spatially non-uniform concentration gradients within the liquid electrolyte. Importantly, the conditions under which optical imaging can be performed inside absorbing and multiply scattering materials such as battery intercalation compounds are outlined.

cond-mat.mtrl-sci↗
arXiv2022

Scattering correcting wavefront shaping for three-photon microscopy

Three-photon (3P) microscopy is getting traction due to its superior performance in deep tissues. Yet, aberrations and light scattering still pose one of the main limitations in the attainable depth ranges for high-resolution imaging. Here, we show scattering correcting wavefront shaping with a simple continuous optimization algorithm, guided by the integrated 3P fluorescence signal. We demonstrate focusing and imaging behind scattering layers and investigate convergence trajectories for different sample geometries and feedback non-linearities. Furthermore, we show imaging through a mouse skull and demonstrate a novel fast phase estimation scheme that substantially increases the speed at which the optimal correction can be found.

physics.optics↗
arXiv2022

Non-invasive chemically selective energy delivery and focusing inside a scattering medium guided by Raman scattering

Raman scattering is a chemically selective probing mechanism with diverse applications in industry and clinical settings. Yet, most samples are optically opaque limiting the applicability of Raman probing at depth. Here, we demonstrate chemically selective energy deposition behind a scattering medium by combining prior information on the chemical's spectrum with the measurement of a spectrally resolved Raman speckle as a feedback mechanism for wavefront shaping. We demonstrate unprecedented six-fold signal enhancement in an epi-geometry, realizing targeted energy deposition and focusing on selected Raman active particles.

physics.optics↗
arXiv2021

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↗
arXiv2021

Large field-of-view non-invasive imaging through scattering layers using fluctuating random illumination

On-invasive optical imaging techniques are essential diagnostic tools in many fields. Although various recent methods have been proposed to utilize and control light in multiple scattering media, non-invasive optical imaging through and inside scattering layers across a large field of view remains elusive due to the physical limits set by the optical memory effect, especially without wavefront shaping techniques. Here, we demonstrate an approach that enables non-invasive fluorescence imaging behind scattering layers with field-of-views extending well beyond the optical memory effect. The method consists in demixing the speckle patterns emitted by a fluorescent object under variable unknown random illumination, using matrix factorization and a novel fingerprint-based reconstruction. Experimental validation shows the efficiency and robustness of the method with various fluorescent samples, covering a field of view up to three times the optical memory effect range. Our non-invasive imaging technique is simple, neither requires a spatial light modulator nor a guide star, and can be generalized to a wide range of incoherent contrast mechanisms and illumination schemes.

physics.optics↗
arXiv2020

Spectrally-resolved point-spread-function engineering using a complex medium

Propagation of an ultrashort pulse of light through strongly scattering media generates an intricate spatio-spectral speckle that can be described by means of the multi-spectral transmission matrix (MSTM). In conjunction with a spatial light modulator, the MSTM enables the manipulation of the pulse leaving the medium; in particular focusing it at any desired spatial position and/or time. Here, we demonstrate how to engineer the point-spread-function of the focused beam both spatially and spectrally, from the measured MSTM. It consists in numerically filtering the spatial content at each wavelength of the matrix prior to focusing. We experimentally report on the versatility of the technique through several examples, in particular as an alternative to simultaneous spatial and temporal focusing, with potential applications in multiphoton microscopy.

physics.optics↗
arXiv2019

Interface-Sensitive Raman Microspectroscopy of Water via Confinement with a Multimodal Miniature Surface Forces Apparatus

Modern interfacial science is increasingly multi-disciplinary. Unique insight into interfacial interactions requires new multimodal techniques for interrogating surfaces with simultaneous complementary physical and chemical measurements. We describe here the design and testing of a microscope that incorporates a miniature Surface Forces Apparatus (μSFA) in sphere vs. flat mode for force-distance measurements, while simultaneously acquiring Raman spectra of the confined zone. The microscope uses a simple optical setup that isolates independent optical paths for (i) the illumination and imaging of Newton's Rings and (ii) Raman-mode excitation and efficient signal collection. We benchmark the methodology by examining Teflon thin films in asymmetric (Teflon-water-glass) and symmetric (Teflon-water-Teflon) configurations. Water is observed near the Teflon-glass interface with nanometer-scale sensitivity in both the distance and Raman signals. We perform chemically-resolved, label-free imaging of confined contact regions between Teflon and glass surfaces immersed in water. Remarkably, we estimate that the combined approach enables vibrational spectroscopy with single water monolayer sensitivity within minutes. Altogether, the Raman-μSFA allows exploration of molecular confinement between surfaces with chemical selectivity and correlation with interaction forces.

physics.ins-det↗
arXiv2019

A Multi-Modal Miniature Surface Forces Apparatus (uSFA) for Interfacial Science Measurements

Advances in the research of intermolecular and surface interactions result from the development of new and improved measurement techniques and combinations of existing techniques. Here, we present a new miniature version of the Surface Force Apparatus (the uSFA) that has been designed for ease of use and multi-modal capabilities with retention of the capabilities of other SFA models including accurate measurement of surface separation distance and physical characterization of dynamic and static physical forces (i.e., normal, shear, and friction) and interactions (e.g., van der Waals, electrostatic, hydrophobic, steric, biospecific). The small physical size of the uSFA, compared to previous SFA models, makes it portable and suitable for integration into commercially available optical and fluorescence light microscopes, as demonstrated here. The large optical path entry and exit ports make it ideal for concurrent force measurements and spectroscopy studies. Examples of the use of the uSFA in combination with surface plasmon resonance (SPR) and Raman spectroscopy measurements are presented. Due to the short working distance constraints associated with Raman spectroscopy, an interferometric technique was developed and applied for calculating the inter-surface separation distance based on Newtons rings. The introduction of the \muSFA will mark a transition in SFA usage from primarily physical characterization to concurrent physical characterization with in situ chemical and biological characterization to study interfacial phenomena, including (but not limited to) molecular adsorption, fluid flow dynamics, determination of surface species and morphology, and (bio) molecular binding kinetics.

physics.ins-det↗
arXiv2018

Fast compressive Raman bio-imaging via matrix completion

Raman microscopy is a powerful method combining non-invasiveness with no special sample preparation. Because of this remarkable simplicity, it has been widely exploited in many fields, ranging from life and materials sciences, to engineering. Notoriously, due to the required imaging speeds for bio-imaging, it has remained a challenge how to use this technique for dynamic and large-scale imaging. Recently, compressive Raman has been put forward, allowing for fast imaging, therefore solving the issue of speed. Yet, due to the need of strong a priori information of the species forming the hyperspectrum, it has remained elusive how to apply this technique for microspectroscopy of (dynamic) biological tissues. Combining an original spectral under-sampling measurement technique with matrix completion framework for reconstruction, we demonstrate fast and inexpensive label-free molecular imaging of biological specimens (brain tissues and single cells). Therefore, our results open interesting perspectives for clinical and cell biology applications using the much faster compressive Raman framework.

physics.med-ph↗
arXiv2018

High-sensitivity high-speed compressive spectrometer for Raman imaging

Compressive Raman is a recent framework that allows for large data compression of microspectroscopy during its measurement. Because of its inherent multiplexing architecture, it has shown imaging speeds considerably higher than conventional Raman microspectroscopy. Nevertheless, the low signal-to-noise (SNR) of Raman scattering still poses challenges for high-sensitivity bio-imaging exploiting compressive Raman: (i) the idle solvent acts as a background noise upon imaging small biological organelles, (ii) current compressive spectrometers are lossy precluding high-sensitivity imaging. We present inexpensive high-throughput spectrometer layouts for high-sensitivity compressive hyperspectroscopy. We exploit various modalities of compressive Raman allowing for up to 80X reduction of data storage and 2X microspectroscopy speed up at a 230-nm spatial resolution. Such achievements allowed us to chemically image sub-diffraction-limited biological specimens (lipid bilayers) in few seconds.

physics.optics↗
arXiv2018

Label-free imaging of cholesterol and lipid distributions in model membranes

Over recent decades, lipid membranes have become standard models for examining the biophysics and biochemistry of cell membranes. Interrogation of lipid domains within biomembranes is generally done with fluorescence microscopy via exogenous chemical probes. However, most fluorophores have limited partitioning tunability, with the majority segregating in the least biologically relevant domains (i.e., low-density liquid domains). Therefore, a molecular-level picture of the majority of non-labeled lipids forming the membrane is still elusive. Here, we present simple, label-free imaging of domain formation in lipid monolayers, with chemical selectivity in unraveling lipid and cholesterol composition in all domain types. Exploiting conventional vibrational contrast in spontaneous Raman imaging, combined with chemometrics analysis, allows for examination of ternary systems containing saturated lipids, unsaturated lipids, and cholesterol. We confirm features commonly observed by fluorescence microscopy, and provide an unprecedented analysis of cholesterol distribution at the single-membrane level.

physics.bio-ph↗