We demonstrate a scheme for efficient coherent anti-Stokes Raman scattering (CARS) microscopy free of nonresonant background. Our method is based on a compact Er:fiber laser source. Impulsive excitation of molecular resonances is achieved by an 11 fs pulse at 1210 nm. Broadband excitation gives access to molecular resonances from 0 cm(-1) up to 4000 cm(-1). Time-delayed narrowband probing at 775 nm enables sensitive and high-speed spectral detection of the CARS signal free of nonresonant background with a resolution of 10 cm(-1).

We present a compact coherent anti-Stokes Raman scattering microscope based on a widely tunable picosecond Er:fiber laser. Intense and bandwidth-limited 1 ps pump pulses at a center wavelength of 775 nm are generated via frequency mixing within the broadband fundamental at 1.55 microm. Narrowband Stokes pulses are obtained by frequency shifting of solitons in a highly nonlinear bulk fiber and subsequent second-harmonic generation. The tuning range from 850 nm to 1100 nm gives access to vibrational resonances between 1150 cm(-1) and 3800 cm(-1). A first imaging application in the spectral region of CH stretch vibrations is demonstrated.

A simple scheme for video-rate wide-field coherent anti-Stokes Raman scattering (CARS) microscopy is presented. The method is based on collinear nonphase-matching illumination. The mechanisms leading to CARS signal generation are investigated. We find that refraction-mediated phase-matching is the main effect. Video-rate wide-field CARS microscopy of polystyrene beads and CARS wide-field images of C. elegans embryos are shown, and the capabilities and the limitations of the scheme are discussed.

We demonstrate a compact pulse compression scheme that offers flexible chirp control for improved conversion efficiencies in high resolution nonlinear optical microscopy. An Er:fiber laser combined with a highly nonlinear optical fiber yields pulses centered at 1100 nm with a bandwidth of 500 nm. The compressed pulses with a duration of 7.6 fs enable simultaneous second-harmonic generation, third-harmonic generation, and four-wave mixing microscopy. The spectrum is tailored for an ideal compromise between conversion efficiency and spectral discrimination between the three types of broadband nonlinear signals. Distinct differences in structural contrast obtained from the simultaneous read-out of the three nonlinear signals are demonstrated in a biological sample.

We demonstrate a method for broadband laser pulse characterization based on a spectrally resolved cross-correlation with a narrowband flat-top gate pulse. Excellent phase-matching by collinear excitation in a microscope focus is exploited by degenerate four-wave mixing in a microscope slide. Direct group delay extraction of an octave spanning spectrum which is generated in a highly nonlinear fiber allows for spectral phase retrieval. The validity of the technique is supported by the comparison with an independent second-harmonic fringe-resolved autocorrelation measurement for an 11 fs laser pulse.