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Coherent anti-Stokes Raman scattering (CARS) can be used to excite vibrational bonds with chemical selectivity, high spatial and spectral resolution, and high sensitivity, which has many applications in biomedical research. The common way to realize CARS imaging is illuminating sample with two synchronized ultra-short pulses. Recent development of various fiber laser schemes based on nonlinear optical effect provides compact laser source for CARS imaging. However, the nonlinear conversion in optical fiber may inevitably introduce temporal or spectral noise to the newly generated pulses. In this paper, we have proposed a polarization-maintaining (PM) passive-synchronized picosecond fiber laser system that generates dual-color picosecond pulses for CARS. An Er-doped fiber laser and a Yb-doped fiber laser were passively synchronized by cross phase modulation based on master-slave injection scheme. In the experiment, the wavelength of one branch was fixed at 791 nm, which was generated by second harmonic generation of Er-doped fiber laser. The wavelength of the other branch can be continuously tuned from 1017-1047 nm, which was obtained by adding an active spectral broadening module and an optical bandpass filter after Yb-doped fiber laser. As a result, the laser source allows to probe vibrational bonds with frequencies difference between 2809 cm-1 and 3091 cm-1 . Finally, the achieved tunable synchronized pulses enabled us to microscopically image mouse ear samples. The compact optical fiber laser proposed with PM fiber design, stable synchronization and large wavelength tunability would become a promising laser source for CARS imaging in clinical use.

Photochromic probes with reversible fluorescence have revolutionized the fields of single molecule spectroscopy and super-resolution microscopy, but lack sufficient chemical specificity. In contrast, Raman probes with stimulated Raman scattering (SRS) microscopy provides superb chemical resolution for super-multiplexed imaging, but are relatively inert. Here we report vibrational photochromism by engineering alkyne tagged diarylethene to realize photo-switchable SRS imaging. The narrow Raman peak of the alkyne group shifts reversibly upon photoisomerization of the conjugated diarylethene when irradiated by ultraviolet (UV) or visible light, yielding “on” or “off” SRS images taken at the photoactive Raman frequency. We demonstrated photo-rewritable patterning and encryption on thin films, painting/erasing of cells with labelled alkyne-diarylethene, as well as pulse-chase experiments of mitochondria diffusion in living cells. The design principle provides potentials for super-resolution microscopy, optical memories and switches with vibrational specificity., Probes with reversible fluorescence are useful in super-resolution microscopy, but lack sufficient chemical specificity. Here, the authors engineer alkyne tagged diarylethene to realize photo-switchable stimulated Raman scattering probes with high chemical resolution, for applications in living cells.

We have proposed and implemented a polarization-maintaining passively synchronized fiber laser system, which could deliver tunable dual-color picosecond pulses by including a frequency-doubling module and a spectral broadening module. Specifically, the output from the involved Er-doped fiber laser were used to generate second-harmonic pulses at 790 nm with a quadratic nonlinear crystal. In parallel, the amplified pulses from the synchronized Yb-doped fiber laser were launched into a 150-m single mode fiber, which resulted in not only substantial spectral bandwidth broadening from 0.1 to 20.1 nm, but also a significant Raman-induced signal around 1080 nm. Consequently, narrow spectra from 1018-1051 nm and 1070-1095 nm could be continuously tuned via a tunable bandpass filter, corresponding to Raman bonds from 2835-3143 cm−1 and 3312-3525 cm−1. Finally, the achieved tunable synchronized pulses enabled us to microscopically examine mouse ear samples based on coherent anti-Stokes Raman and second harmonic generation imaging. Therefore, our tunable passively-synchronized fiber laser system would be promising to provide a simple and compact laser source for subsequent coherent Raman microscopy.

Polarization-maintaining passively synchronized ytterbium and erbium fiber lasers were demonstrated to deliver tunable pulses of 1016-1048 nm and frequency doubled pulses at 790 nm, which were used in coherent anti-Stokes Raman imaging.

We have demonstrated a compact fiber laser with broad and fast wavelength tunability for coherent anti-Stokes Raman scattering (CARS) microscopy. Originated from an Er-doped fiber laser, the Stokes pulses can be tuned from 1015 to 1060 nm within 300 μs from supercontinuum of a tapered high nonlinear fiber, while pump pulses at 790 nm were obtained by second harmonic generation. The two beams were then sent to microscopes for CARS detection of oil, ethanol and mouse ear samples. This fast and broadly tunable fiber laser in the all-polarization-maintaining architecture would be promising to implement rapid label-free histology in clinical translation.