We demonstrate a modular and versatile experimental setup that enables straightforward compression (and then shaping)
of ultrashort laser pulses at the imaging plane of a two-photon microscope. A commercially available pulse shaper is
used in conjunction with a commercially available broadband Ti:Sapphire oscillator to produce sub-8fs pulses at the
focus of a high-numerical-aperture objective. Automated adaptive pulse compression, based on multiphoton intrapulse
interference phase scan (MIIPS), is verified in situ by shaper assisted interferometric autocorrelation. Two-photon
excited fluorescence image of a mouse kidney slide is obtained to confirm microscopic sectioning capabilities.
The fundamental difficulty of achieving a coherently enhanced sensing method at standoff distances greater than 10
meters has been solved by single-beam coherent anti-Stokes Raman scattering and by actively measuring and
eliminating chromatic dispersion experienced by the broad-bandwidth (100 nm) laser pulses. Characteristic Raman
spectra for several chemicals in gas, liquid, and solid states, are successfully obtained from a 12 meter standoff distance.
The results obtained indicate this is a promising approach to standoff detection of chemicals, hazardous contaminations,
The molecular first hyperpolarizability β of di-2-ANEPEQ and di-8-ANEPPS have been measured using hyper-Rayleigh scattering. Because of the strong fluorescence produced by the ANEP dyes, time correlated single photon counting Hyper-Rayleigh scattering measurements and spectral decomposition have been used to obtain accurate β values that correct for the competing fluorescent signal. The molecular hyperpolarizability β is measured for various wavelengths and compared with a two level model. Solvent effects have also been measured; the experimental results are consistent with a two valence bond state model.