Ultra-low timing jitter, Ti:Al2O3 synchronization for stimulated Raman scattering and pump-probe microscopy.

SIGNIFICANCE: Stimulated Raman scattering (SRS) and pump-probe microscopy are implementations of multiphoton microscopy that acquire high-resolution, label-free images of live samples encoded with molecular contrast. Most commercial multiphoton microscopes cannot access these techniques since they require sample illumination by two temporally synchronized ultrafast pulse trains. We present a compact and robust way of synchronizing an additional Ti:sapphire laser with a conventional single-beam multiphoton microscope to realize an instrument that can acquire images with enhanced molecular specificity. AIM: A passive optical synchronization scheme for a pair of commercially available, unmodified modelocked Ti:sapphire lasers was developed. The suitability of this synchronization scheme for advanced biomedical microscopy was investigated. APPROACH: A pair of modelocked Ti:sapphire lasers were aligned in master-slave configuration. Five percent of the master laser output was used to seed the modelocking in the slave laser cavity. The timing jitter of the master and slave pulse trains was characterized using an optical autocorrelator. The synchronized output of both lasers was coupled into a laser scanning microscope and used to acquire spectral focusing SRS and pump-probe microscopy images from biological and nonbiological samples. RESULTS: A timing jitter between the modelocked pulse trains of 0.74 fs was recorded. Spectral focusing SRS allowed spectral discrimination of polystyrene and polymethyl methacrylate beads. Pump-probe microscopy was used to record excited state lifetime curves from hemoglobin in intact red blood cells. CONCLUSION: Our work demonstrates a simple and robust method of upgrading single-beam multiphoton microscopes with an additional ultrafast laser. The resulting dual-beam instrument can be used to acquire label-free images of sample structure and composition with high biochemical specificity.

Nonlinear femtosecond pump-probe spectroscopy using a power-encoded soliton delay line.

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.

Fiber-based ultrashort pulse delivery for nonlinear imaging using high-energy solitons.

We present an approach for fiber delivery of femtosecond pulses relying on pulse breakup and soliton self-frequency shift in a custom-made solid-core photonic bandgap fiber. In this scheme, the fiber properties themselves ensure that a powerful Fourier-transform-limited pulse is emitted at the fiber output, hence doing away with the need for complex precompensation and enabling tunability of the excitation. We report high-energy soliton excitation for two-photon fluorescence microspectroscopy over a 100-nm range and multimodal nonlinear imaging on biological samples.