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Coherent anti-Stokes Raman scattering (CARS) has found wide applications in biomedical research. Compared with alternatives, single-beam CARS is especially attractive at low frequencies. Yet, currently existing schemes necessitate a relatively complicated setup to perform high-resolution spectroscopy. Here we show that the spectral sharp edge formed by an ultra-steep long-pass filter is sufficient for performing CARS spectroscopy, simplifying the system significantly. We compare the sensitivity of the presented methodology with available counterparts both theoretically and experimentally. Importantly, we show that this method, to the best of our knowledge, is the simplest and most suitable for vibrational imaging and spectroscopy in the very low-frequency regime (<200  cm -1 ).

We demonstrate focusing and imaging through a scattering medium without access to the fluorescent object by using wavefront shaping. Our concept is based on utilizing the spatial fluorescence contrast which naturally exists in the hidden target object. By scanning the angle of incidence of the illuminating laser beam and maximizing the variation of the detected fluorescence signal from the object, as measured by a bucket detector at the front of the scattering medium, we are able to generate a tightly focused excitation spot. Thereafter, an image is obtained by scanning the focus over the object within the memory effect range. The requirements for applicability of the method and the comparison with speckle-correlation based focusing methods are discussed.

In recent years, wavefront shaping has been utilized to control and correct distorted light for enhancing a bright spot, generation of a Bessel beam or darkening a complete area at the output of a scattering system. All these outcomes can be thought of as enhancing a particular mode of the output field. In this letter, we study the relation between the attainable enhancement factor, corresponding to the efficiency of mode conversion, and the field distribution of the target mode. Working in the limit of a thin diffuser enables not only a comparison between experimental and simulated results, but also allows for derivation of an analytic formula. These results shed light on the ability to use a scattering medium as a mode converter and on the relationship between the desired shape and the efficiency.

Stimulated Raman scattering (SRS) has recently become useful for chemically selective bioimaging. It is usually measured via modulation transfer from the pump beam to the Stokes beam. Impulsive stimulated Raman spectroscopy, on the other hand, relies on the spectral shift of ultrashort pulses as they propagate in a Raman active sample. This method was considered impractical with low energy pulses since the observed shifts are very small compared to the excitation pulse bandwidth, spanning many terahertz. Here we present a new apparatus, using tools borrowed from the field of precision measurement, for the detection of low-frequency Raman lines via stimulated-Raman-scattering-induced spectral shifts. This method does not require any spectral filtration and is therefore an excellent candidate to resolve low-lying Raman lines (<200  cm -1 ), which are commonly masked by the strong Rayleigh scattering peak. Having the advantage of the high repetition rate of the ultrafast oscillator, we reduce the noise level by implementing a lock-in detection scheme with a wavelength shift sensitivity well below 100 fm. This is demonstrated by the measurement of low-frequency Raman lines of various liquid samples.

Harmonic generation by tightly-focused Gaussian beams is finding important applications, primarily in nonlinear microscopy. It is often naively assumed that the nonlinear signal is generated predominantly in the focal region. However, the intensity of Gaussian-excited electromagnetic harmonic waves is sensitive to the excitation geometry and to the phase matching condition, and may depend on quite an extended region of the material away from the focal plane. Here we solve analytically the amplitude integral for second harmonic and third harmonic waves and study the generated harmonic intensities vs. focal-plane position within the material. We find that maximum intensity for positive wave-vector mismatch values, for both second harmonic and third harmonic waves, is achieved when the fundamental Gaussian is focused few Rayleigh lengths beyond the front surface. Harmonic-generation theory predicts strong intensity oscillations with thickness if the material is very thin. We reproduced these intensity oscillations in glass slabs pumped at 1550nm. From the oscillations of the 517nm third-harmonic waves with slab thickness we estimate the wave-vector mismatch in a Soda-lime glass as Δk(H)= -0.249μm(-1).

Noninvasive label-free imaging of biological systems raises demand not only for high-speed three-dimensional prescreening of morphology over a wide-field of view but also it seeks to extract the microscopic functional and molecular details within. Capitalizing on the unique advantages brought out by different nonlinear optical effects, a multimodal nonlinear optical microscope can be a powerful tool for bioimaging. Bringing together the intensity-dependent contrast mechanisms via second harmonic generation, third harmonic generation and four-wave mixing for structural-sensitive imaging, and single-beam/single-pulse coherent anti-Stokes Raman scattering technique for chemical sensitive imaging in the finger-print region, we have developed a simple and nearly alignment-free multimodal nonlinear optical microscope that is based on a single wide-band Ti:Sapphire femtosecond pulse laser source. Successful imaging tests have been realized on two exemplary biological samples, a canine femur bone and collagen fibrils harvested from a rat tail. Since the ultra-broad band-width femtosecond laser is a suitable source for performing high-resolution optical coherence tomography, a wide-field optical coherence tomography arm can be easily incorporated into the presented multimodal microscope making it a versatile optical imaging tool for noninvasive label-free bioimaging.

We present a scheme for recovering the complex input field launched into a waveguide array, from partial measurements of its output intensity, given advance knowledge that the input is sparse. In spite of the fact that in general the inversion problem is ill-conditioned, we demonstrate experimentally and in simulations that the prior knowledge of sparsity helps overcome the loss of information. Our method is based on GESPAR, a recently proposed efficient phase retrieval algorithm. Possible applications include optical interconnects and quantum state tomography, and the ideas are extendable to other multiple input and multiple output (MIMO) communication schemes.

We show that the polarization state of coherent light propagating through an optically thick multiple scattering medium can be controlled by wavefront shaping, that is, by controlling only the spatial phase of the incoming field with a spatial light modulator. Any polarization state of light at any spatial position behind the scattering medium can be attained with this technique. Thus, transforming the random medium to an arbitrary optical polarization component becomes possible.

We analyze the spatiotemporal distortions of an ultrashort pulse focused through a thin scattering surface. We show and experimentally verify that in such a scenario temporal distortions are proportional to the distance from the optical axis and are present only outside the focal point, as result of geometrical path length differences. We use wavefront shaping to correct for the spatiotemporal distortions and to temporally compress chirped input pulses through the scattering medium.

We study the case of two simultaneous three-wave-mixing processes, where one frequency is converted to another through an intermediate frequency. The common assumption is that these processes can occur only when the material is transparent at all participating frequencies. Here we show experimentally that, under appropriate conditions, the intermediate frequency remains dark throughout the interaction. This means that even if the material is opaque at the intermediate frequency, the conversion will remain efficient. New possibilities of frequency conversion are therefore available, e.g. through absorptive bands in the ultraviolet or mid-infrared. Moreover, though it was hitherto assumed that the phase mismatch value is governed only by dispersion, we show here that phase matching also depends on light intensity. These findings promise novel all optical switching techniques.

We demonstrate the acquisition of stimulated Raman scattering spectra with the use of a single femtosecond pulse. High-resolution vibrational spectra are obtained by shifting the phase of a narrow band of frequencies within the input pulse spectrum, using spectral shaping. The vibrational lines are resolved via amplitude features formed in the spectrum after interaction with the sample. Using this technique, low-frequency Raman lines (<100 cm⁻¹) are observed on both the Stokes and anti-Stokes sides.

We present a simple and easily implementable scheme for multiplexed Coherent Anti-Stokes Raman Scattering (CARS) spectroscopy and microscopy using a single femtosecond pulse, shaped with a narrow spectral notch. We show that a tunable spectral notch, shaped by a resonant photonic crystal slab, can serve as a narrowband, optimally time-delayed probe, resolving a broad vibrational spectrum with high spectral resolution in a single-shot measurement. Our single-source, single-beam scheme allows the simple transformation of any multiphoton microscope with adequate bandwidth into a nearly alignment-free CARS microscope.

We introduce an illumination configuration which is a spatiotemporal analog of a non-diffracting X-wave. By interfering multiple ultrashort converging plane waves, we generate a tight central spot at which a transform limited ultrashort pulse is formed. Outside this tight focus a spatiotemporal speckle field with longer duration and reduced peak power is created. We investigate this spatiotemporal X-wave configuration analytically, numerically, and experimentally demonstrate the effect using two photon excitation fluorescence.