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Two-photon excited fluorescence (2PEF) microscopy is the most popular non-linear imaging method of biomedical samples. State-of-the art 2PEF microscopes use multiple detectors and spectral filter sets to discriminate different fluorophores based on their distinct emission behavior (emission discrimination). One drawback of 2PEF is that fluorescence photons outside the filter transmission range are inherently lost, thereby reducing the imaging efficiency and speed. Furthermore, emission discrimination of different fluorophores may fail if their emission profiles are too similar. Here, we present an alternative 2PEF method that discriminates fluorophores based on their excitation spectra (excitation discrimination). For excitation we use two lasers of different wavelengths (ω 1 , ω 2 ) resulting in excitation energies at 2ω 1 , 2ω 2 , and the mixing energy ω 1 +ω 2 . Both lasers are frequency encoded (FE) by an intensity modulation at distinct frequencies while all 2PEF emission is collected on a single detector. The signal is fed into a lock-in-amplifier and demodulated at various frequencies simultaneously. A customized nonnegative matrix factorization (NNMF) then generates fluorescence images that are free of cross talk. Combining FE-2PEF with multiple detectors has the potential to enable the simultaneous imaging of an unprecedented number of fluorophores.

A stimulated Raman microscope is conventionally performed by modulating either the pump or Stokes beam and demodulating the other. Here, we propose a double modulation scheme that modulates both beams at f m and 2f m . Exploiting aliasing and reduction of the repetition rate, we show that the proposed double modulation scheme amplifies the signal amplitude by a factor of 1.5, 2, and 4 for different modulation frequencies and experimental realizations for the same average power at the sample. By deriving the noise power for different sources, we show that the double modulation scheme can perform stimulated Raman scattering (SRS) imaging with an up to 16-fold speed improvement as compared with single beam modulation.

Impulsive stimulated Raman scattering (ISRS) is a robust technique for studying low frequency (<300 cm -1 ) Raman vibrational modes, but ISRS has faced difficulty in translation to an imaging modality. A primary challenge is the separation of the pump and probe pulses. Here we introduce and demonstrate a simple strategy for ISRS spectroscopy and hyperspectral imaging that uses complementary steep edge spectral filters to separate the probe beam detection from the pump and enables simple ISRS microscopy with a single-color ultrafast laser source. ISRS spectra are obtained that span from the fingerprint region down to <50 cm -1 vibrational modes. Hyperspectral imaging and polarization-dependent Raman spectra are also demonstrated.

We report on the use of a thin diffuser placed in the close vicinity of a camera sensor as a simple and effective way to superlocalize plasmonic nanoparticles in 3D. This method is based on holographic reconstruction via quantitative phase and intensity measurements of a light field after its interaction with nanoparticles. We experimentally demonstrate that this thin diffuser can be used as a simple add-on to a standard bright-field microscope to allow the localization of 100 nm gold nanoparticles at video rate with nanometer precision (1.3 nm laterally and 6.3 nm longitudinally). We exemplify the approach by revealing the dynamic Brownian trajectory of a gold nanoparticle trapped in various pockets within an agarose gel. The proposed method provides a simple but highly performant way to track nanoparticles in 3D.

In this Letter, we report a high-efficiency, miniaturized, ultra-fast coherent beam, combined with 3D-printed micro-optics directly on the tip of a multicore fiber bundle. The highly compact device footprint (180 µm in diameter) facilitates its incorporation into a minimally invasive ultra-thin nonlinear endoscope to perform two-photon imaging.

We report a line-scanning imaging modality of compressive Raman technology with a single-pixel detector. The spatial information along the illumination line is encoded onto one axis of a digital micromirror device, while spectral coding masks are applied along the orthogonal direction. We demonstrate imaging and classification of three different chemical species.

Real-time vibrational microscopy has been recently demonstrated by various techniques, most of them utilizing the well-known schemes of coherent anti-stokes Raman scattering and stimulated Raman scattering. These techniques readily provide valuable chemical information mostly in the higher vibrational frequency regime (>400  cm -1 ). Addressing the low vibrational frequency regime (<200  cm -1 ) is challenging due to the usage of spectral filters that are required to isolate the signal from the Rayleigh scattered excitation field. In this Letter, we report on rapid, high-resolution, low-frequency (<130  cm -1 ) vibrational microscopy using impulsive coherent Raman excitation. By combining impulsive excitation with a fast acousto-optic delay line, we detect the Raman-induced optical Kerr lensing and spectral shift effects with a 25 μs pixel dwell time to produce shot-noise limited, low-frequency hyper-spectral images of various samples.

We report a line scanning imaging modality of compressive Raman technology with spatial frequency modulated illumination using a single pixel detector. We demonstrate the imaging and classification of three different chemical species at line scan rates of 40 Hz.

High-speed imaging is of the utmost importance for video-rate live cell investigations or to study extended sample areas at sufficient spatial resolution within reasonable time scales. Improving the speed of single-focus stimulated Raman scattering (SRS) microscopy is ultimately restricted by the sample's damage threshold and the shot noise of the demodulated laser source. To overcome this limitation, we present a dual-focus SRS approach modulating the pump laser for each focus at a distinct frequency. The corresponding probe beams are detected each by a photodiode and demodulated individually by two separate lock-in units to avoid inter-focal cross-talk. Two laterally or axially displaced images as well as hyperspectral SRS images can be obtained simultaneously within the field of view of the objective lens. The modular implementation presented here can be extended to multiple foci by using multi-channel acousto-optics modulators in combination with multi-channel lock-in amplifiers.

A simple technique for far-field single-shot noninterferometric determination of the phase transmission matrix of a multicore fiber with over 100 cores is presented. This phase retrieval technique relies on the aperiodic arrangement of the cores.

We report two-photon lensless imaging through a novel Fermat's golden spiral multicore fiber. This unique layout optimizes the sidelobe levels, field of view, crosstalk, group delay, and mode density to achieve a sidelobe contrast of at least 10.9 dB. We demonstrate experimentally the ability to generate and scan a focal point with femtosecond pulses and perform two-photon imaging.

To increase the information per pixel in stimulated Raman scattering (SRS) microscopy as well as to correct from artifacts, it is valuable to acquire images at two different Raman shifts. We present a three-color SRS approach acquiring two perfectly registered SRS images where both pump beams are modulated at distinct frequencies while demodulating the Stokes beam. Our implementation uses two optical parametric oscillators that can be tuned to an almost arbitrary energy difference of Raman shifts, allowing investigation of fingerprint resonances simultaneously to CH-stretch vibrations.

We propose and implement a broadband, compact, and low-cost wavefront sensing scheme by simply placing a thin diffuser in the close vicinity of a camera. The local wavefront gradient is determined from the local translation of the speckle pattern. The translation vector map is computed thanks to a fast diffeomorphic image registration algorithm and integrated to reconstruct the wavefront profile. The simple translation of speckle grains under local wavefront tip/tilt is ensured by the so-called "memory effect" of the diffuser. Quantitative wavefront measurements are experimentally demonstrated, both for the few first Zernike polynomials and for phase-imaging applications requiring high resolution. We finally provided a theoretical description of the resolution limit that is supported experimentally.

Hollow core fibers are considered as promising candidates to deliver intense temporally overlapping picosecond pulses in applications such as stimulated Raman scattering (SRS) microscopy and endoscopy because of their inherent low nonlinearity compared to solid-core silica fibers. Here we demonstrate that, contrary to prior assumptions, parasitic signals are generated in Kagomé lattice hollow core fibers. We identify the origin of the parasitic signals as an interplay between the Kerr nonlinearity of air and frequency-dependent fiber losses. Importantly, we identify the special cases of experimental parameters that are free from parasitic signals, making hollow core fibers ideal candidates for noise-free SRS microscopy and endoscopy.

We report a simple add-on for broadband stimulated Raman scattering (SRS) microscopes to enable fast and programmable spectroscopy acquisition. It comprises a conventional dispersive spectrometer layout incorporating a fast digital micromirror device (DMD). The approach is validated by acquiring SRS spectra of standard chemicals. We demonstrate a DMD's advantage in broadband SRS by showing higher signal-to-noise ratio using a multiplexed Hadamard spectral basis and compressive sensing detection. Our results apply to a variety of frequency-domain pump-probe spectroscopy.

Multicore fiber bundles are widely used in endoscopy due to their miniature size and their direct imaging capabilities. They have recently been used, in combination with spatial light modulators, in various realizations of endoscopy with little or no optics at the distal end. These schemes require characterization of the relative phase offsets between the different cores, typically done using off-axis holography, thus requiring both an interferometric setup and, typically, access to the distal tip. Here we explore the possibility of employing phase retrieval to extract the necessary phase information. We show that in the noise-free case, disordered fiber bundles are superior for phase retrieval over their periodic counterparts, and demonstrate experimentally accurate retrieval of phase information for up to 10 simultaneously illuminated cores. Thus, phase retrieval is presented as a viable alternative for real-time monitoring of phase distortions in multicore fiber bundles.

We demonstrate femtosecond pump-probe transient absorption spectroscopy using a programmable dispersive filter as an ultra-fast delay line. Combined with fast synchronous detection, this delay line allows for recording of 6 ps decay traces at 34 kHz. With such acquisition speed, we perform single point pump-probe spectroscopy on bulk samples in 80 μs and hyperspectral pump-probe imaging over a field of view of 100 μm in less than a second. The usability of the method is illustrated in a showcase experiment to image and discriminate between two pigments in a mixture.

We demonstrate pixelation-free real-time widefield endoscopic imaging through an aperiodic multicore fiber (MCF) without any distal opto-mechanical elements or proximal scanners. Exploiting the memory effect in MCFs, the images in our system are directly obtained without any post-processing using a static wavefront correction obtained from a single calibration procedure. Our approach allows for video-rate 3D widefield imaging of incoherently illuminated objects with imaging speed not limited by the wavefront-shaping device refresh rate.

We investigate lensless endoscopy using coherent beam combining and aperiodic multicore fibers (MCF). We show that diffracted orders, inherent to MCF with periodically arranged cores, dramatically reduce the field-of-view (FoV), and that randomness in MCF core positions can increase the FoV up to the diffraction limit set by a single fiber core, while maintaining a MCF experimental feasibility. We demonstrate experimentally pixelation-free lensless endoscopy imaging over a 120 μm FoV with an aperiodic MCF designed with widely spaced cores. We show that this system is suitable to perform beam scanning imaging by simply applying a tilt to the proximal wavefront.

We report an experimental test of single-shot polarimetry applied to the problem of real-time monitoring of the output polarization states in each core within a multicore fiber bundle. The technique uses a stress-engineered optical element, together with an analyzer, and provides a point spread function whose shape unambiguously reveals the polarization state of a point source. We implement this technique to monitor, simultaneously and in real time, the output polarization states of up to 180 single-mode fiber cores in both conventional and polarization-maintaining fiber bundles. We demonstrate also that the technique can be used to fully characterize the polarization properties of each individual fiber core, including eigen-polarization states, phase delay, and diattenuation.

We show femtosecond time-resolved nonlinear pump-probe spectroscopy using a fiber soliton as the probe pulse. Furthermore, we exploit soliton dynamics to record an entire transient trace with a power-encoded delay sweep. The power-encoded delay line takes advantage of the dependency of the soliton trajectory in the (λ,z) space upon input power; the difference in accumulated group delay between trajectories converts a fast power sweep into a fast delay sweep. We demonstrate the concept by performing transient absorption spectroscopy in a test sample and validate it against a conventional pump-probe setup.

We present a method that allows one to measure the real and imaginary parts of the third-order susceptibility in a wide-field coherent anti-Stokes Raman scattering setup using a quadriwave lateral shearing interferometer. This permits the retrieval of the undistorted Raman spectrum and the removal of a nonresonant signal from the surrounding solvent, which otherwise may overwhelm weak resonances.

We report a step toward scanning endomicroscopy without distal optics. The focusing of the beam at the distal end of a fiber bundle is achieved by imposing a parabolic phase profile across the exit face with the aid of a spatial light modulator. We achieve video-rate images by galvanometric scanning of the phase tilt at the proximal end. The approach is made possible by the bundle, designed to have very low coupling between cores.

We demonstrate the use of a large-pitch Kagome-lattice hollow-core photonic crystal fiber probe for Raman spectroscopy. The large transmission bandwidth of the fiber enables both the excitation and Raman beams to be transmitted through the same fiber. As the excitation beam is mainly transmitted through air inside the hollow core, the silica luminescence background is reduced by over 2 orders of magnitude as compared to standard silica fiber probes, removing the need for fiber background subtraction.

A wavefront sensor is used as a direct observation tool to image the Gouy phase shift in photonic nanojets created by micrometer-sized dielectric spheres. The amplitude and phase distributions of light are found in good agreement with a rigorous electromagnetic computation. Interestingly the observed phase shift when travelling through the photonic jet is a combination of the awaited π Gouy shift and a phase shift induced by the bead refraction. Such direct spatial phase shift observation using wavefront sensors would find applications in microscopy, diffractive optics, optical trapping, and point spread function engineering.

Conventional fluorescence detection is sensitive to an intricate product of the number of fluorescent emitters times the local excitation intensity. Here, we describe a method to locally quantify the excitation intensity and the number of emitters separately, enabling a clear distinction between the phenomena responsible for a given fluorescence signal. Our technique is based on harmonic excitation modulation and higher-order fluorescence demodulation. It is compatible with a wide range of observations, opening new characterization routes for fluorescence detection or imaging on complex systems, such as plasmonic substrates or scattering media.

We demonstrate stimulated Raman microscopy with broadband pump and Stokes pulses, using spectral focusing to attain spectral resolution and to rapidly acquire spectra within a spectral window determined by the bandwidth of the pulses. As the Stokes pulse, we use the redshifted soliton generated in a photonic crystal fiber, which allows for simple shifting of the accessible spectral window.

Spectral compression by self-phase modulation of amplitude- and phase-shaped pulses is demonstrated as superior compared to pulses that have only been phase shaped. We synthesize linearly negatively chirped parabolic pulses, which we send through a nonlinear photonic crystal fiber, in which self-phase modulation compresses the spectrum of the pulses to within 20% of the Fourier transform limit.

We demonstrate the ability of single-subwavelength-size nanoapertures fabricated in a gold metal thin film to enhance second-harmonic generation (SHG) as compared to a bare metal film. Nonlinear microscopy imaging with polarization resolution is used to quantify the SHG enhancement in circular and triangular nanoaperture shapes. The dependence of the measured SHG enhancement on circular aperture diameters is seen to originate from both phase retardation effects and field enhancements at the nanoaperture edge. Triangular nanoapertures exhibit superior SHG enhancement compared with circular ones, as expected from their noncentrosymmetric shape.

We study tight focus coherent anti-Stokes Raman scattering (CARS) emission in a microcavity where the active medium is squeezed between two independent planar mirrors. We show strong modifications in the CARS forward and backward far-field radiation patterns. For low-order cavities, we demonstrate that most of the emitted power can be concentrated into a direction perpendicular to the mirrors.