A 0D discrete molecule [Co(3,5-pdc)(H2O)5].2H2O (1) was obtained in quantitative yield from the reaction of CoCl2.6H2O and pyridine-3,5-dicarboxylate (3,5-pdc) in pure water solvent at ambient temperature. While a 1D zigzag chain species, [{Co(3,5-pdc)(H2O)4}.H2O]n (2), was produced in a water-rich environment, a 2D layer compound, [Co(3,5-pdc)(H2O)2]n (3), with a 6(3) topology was generated under a water-reduced condition and a 2D sheet structure, [{Cu(3,5-pdc)(py)2}.H2O.EtOH]n (4), was formed under a water-poor condition. Compounds 1, 2, and 4 were characterized by single-crystal X-ray diffraction analysis. The 1D zigzag chain 2 shows a recoverable collapsing property. Compound 4 adopts a 2D sheet structure with a 4.8(2) topology, observed for the first time for the 3,5-pdc-related metal-organic frameworks. Water content was found to be an important factor in determining the topologies of the products in the self-assembly of divalent metal ions (Co2+, Cu2+) and pyridine-3,5-dicarboxylate under mild conditions.

Simultaneous backward and forward second harmonic generations from isolated type-I collagen matrix are observed. Optical interference behaviors of these nonlinear optical signals are studied with accurately determined fibril thickness by an atomic force microscope. The nonlinear emission directions are strongly dependent on the coherent interaction within and between collagen fibrils. A linear relationship is obtained to estimate collagen fibril thickness with nanometer precision noninvasively by evaluating the forward/backward second harmonic generation ratio.

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We reported a record high power (>250 mW) and compact near-infrared fiber-optic femtosecond Cherenkov radiation source and its new application on nonlinear light microscopy for the first time (to our best knowledge). The high power femtosecond Cherenkov radiation was generated by 1.03 μm femtosecond pulses from a portable diode-pumped laser and a photonic crystal fiber as a compact, flexible, and highly efficient wavelength convertor. Sectioned nonlinear light microscopy images from mouse brain blood vessel network and rat tail tendon were then performed by the demonstrated light source. Due to the advantages of its high average output power (>250 mW), high pulse energy (>4 nJ), excellent wavelength conversion efficiency (>40%), compactness, simplicity in configuration, and turn-key operation, the demonstrated femtosecond Cherenkov radiation source could thus be widely applicable as an alternative excitation source to mode-locked Ti:Sapphire lasers for future clinical nonlinear microscopy or other applications requiring synchronized multi-wavelength light sources.

With a micro-electro-mechanical system (MEMS) mirror, we successfully developed a miniaturized epi-third-harmonic-generation (epi-THG) fiber-microscope with a video frame rate (31 Hz), which was designed for in vivo optical biopsy of human skin. With a large-mode-area (LMA) photonic crystal fiber (PCF) and a regular microscopic objective, the nonlinear distortion of the ultrafast pulses delivery could be much reduced while still achieving a 0.4 microm lateral resolution for epi-THG signals. In vivo real time virtual biopsy of the Asian skin with a video rate (31 Hz) and a sub-micron resolution was obtained. The result indicates that this miniaturized system was compact enough for the least invasive hand-held clinical use.

Self-phase-modulation and group velocity dispersion of near IR femtosecond pulses in fibers restrict their use in two-photon fluorescence microscopy (TPFM). Here we demonstrate a hollow-core photonic crystal fiber based two-photon fluorescence microscope with low nonlinearity and dispersion effects. We use this fiber-based TPFM system to take two-photon fluorescence (chlorophyll) images of mesophyll tissue in the leaf of Rhaphidophora aurea. With less than 2mW average power exposure on the leaf at 755nm, the near zero-dispersion wavelength, chloroplasts distribution inside the mesophyll cells can be identified with a sub-micron spatial resolution. The acquired image quality is comparable to that acquired by the conventional fiber-free TPFM system, due to the negligible temporal pulse broadening effect.

Since the first demonstration in 1990, two-photon fluorescence microscopy (TPFM) has made a great impact on biomedical researches. With its high penetration ability, low out-of-focus photodamage, and intrinsic three-dimensional (3D) sectioning capability, TPFM has been widely applied to various medical diagnosis and genome researches. Recently, single-mode optical fibers were introduced into the TPFM systems for remote optical pulse delivery. Fiberbased TPFM has advantages including isolating the vibration from laser and electronic devices, flexible system design, and low cross-talks. It is also the first step toward an all-fiber based two-photon endoscope. However, due to serious temporal broadening when conventional Ti:sapphire based femtosecond pulses propagate through the fiber, the twophoton excitation efficiency of the fiber-optic TPFM is much lower than the conventional one. The temporal broadening effect mainly comes from group velocity dispersion (GVD) and self-phase modulation (SPM), which also leads to significant spectral broadening. To reduce the temporal broadening effect, here we present a hollow-core photonic-bandgap fiber based TPFM. By replacing the conventional single-mode fiber with the hollow core photonic bandgap fiber, the GVD and SPM effects can be greatly reduced for high intensity, ultra-short pulse delivery. Femtosecond Ti:sapphire pulses passing through the fiber with negligible GVD and SPM effects is demonstrated in this paper. Much improvement of two-photon fluorescence excitation efficiency is thus achieved with the hollow-core photonic-bandgap fiber based TPFM.

We demonstrate a compact and self-starting fiber-delivered femtosecond Cr:forsterite laser for nonlinear light microscopy. A semiconductor saturable absorber mirror provides the self-starting mechanism and maintains long-term stability in the laser cavity. Four double-chirped mirrors are employed to reduce the size of the cavity and to compensate for group velocity dispersion. Delivered by a large-mode-area photonic crystal fiber, the generated laser pulses can be compressed down to be with a nearly transform-limited pulse width with 2.2-nJ fiber-output pulse energy. Based on this fiber-delivered Cr:forsterite laser source, a compact and reliable two-photon fluorescence microscopy system can thus be realized.