Generalized phase conjugation for 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 generalized phase conjugation method for 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

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

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 ({\mu}SFA) 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-{\mu}SFA allows exploration of molecular confinement between surfaces with chemical selectivity and correlation with interaction forces

Water Structure, Dynamics, and Sum-Frequency Generation Spectra at Electrified Graphene Interfaces

The properties of water at an electrified graphene electrode are studied via classical molecular dynamics simulations with a constant potential approach. We show that the value of the applied electrode potential has dramatic effects on the structure and dynamics of interfacial water molecules. While a positive potential slows down the reorientational and translational dynamics of water, an increasing negative potential first accelerates the interfacial water dynamics before a deceleration at very large magnitude potential values. Further, our spectroscopic calculations indicate that the water rearrangements induced by electrified interfaces can be probed experimentally. In particular, the calculated water vibrational sum-frequency generation (SFG) spectra show that SFG specifically reports on the first two water layers at 0 V but that at larger magnitude applied potentials the resulting static field induces long-range contributions to the spectrum. Electrified graphene interfaces provide promising paradigm systems for comprehending both short- and long-range neighboring aqueous system impacts

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

Compressive Raman microspectroscopy parallelized by single-photon avalanche diode arrays

We demonstrate an efficient and scalable compressive Raman parallelization scheme based on single-photon avalanche diode (SPAD) arrays to reach pixel dwell times of 23 $\mu$s, representing over 10$\times$ speed-up using the otherwise weak spontaneous Raman effect

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

Interrogating the Light-Induced Charging Mechanism in Li-Ion Batteries Using <i>Operando</i> Optical Microscopy

Photobatteries, batteries with a light-sensitive electrode, have recently been proposed as a way of simultaneously capturing and storing solar energy in a single device. Despite reports of photocharging with multiple different electrode materials, the overall mechanism of operation remains poorly understood. Here, we use operando optical reflection microscopy to investigate light-induced charging in LixV2O5 electrodes. We image the electrode, at the single-particle level, under three conditions: (a) with a closed circuit and light but no electronic power source (photocharging), (b) during galvanostatic cycling with light (photoenhanced), and (c) with heat but no light (thermal). We demonstrate that light can indeed drive lithiation changes in LixV2O5 while maintaining charge neutrality, possibly via a combination of faradaic and nonfaradaic effects taking place in individual particles. Our results provide an addition to the photobattery mechanistic model highlighting that both intercalation-based charging and lithium concentration polarization effects contribute to the increased photocharging capacity

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

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