We present the first detailed demonstrations of octave-spanning SC generation in all-normal dispersion photonic crystal fibers (ANDi PCF) in the visible and near-infrared spectral regions. The resulting spectral profiles are extremely flat without significant fine structure and with excellent stability and coherence properties. The key benefit of SC generation in ANDi PCF is the conservation of a single ultrashort pulse in the time domain with smooth and recompressible phase distribution. For the first time we confirm the exceptional temporal properties of the generated SC pulses experimentally and demonstrate their applicability in ultrafast transient absorption spectroscopy. The experimental results are in excellent agreement with numerical simulations, which are used to illustrate the SC generation dynamics by self-phase modulation and optical wave breaking. To our knowledge, we present the broadest spectra generated in the normal dispersion regime of an optical fiber.

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A noncollinearly phase-matched optical parametric amplifier pumped by a commercial 2 MHz fiber laser is presented and discussed. The pump system allows the direct generation of a seed continuum from a sapphire plate. Clean pulses with up to 860 nJ energy and down to 14 fs pulse length can be obtained over a fundamental tuning range from 620 to 970 nm. Conversion by second- and third-harmonic generation as well as sum frequency mixing results in an extended tuning range down to well below 300 nm.

The initial photochromic reaction of dithizonatophenylmercury(II) in solution was investigated by femtosecond transient absorption spectroscopy. Ultrafast excitation within less than 100 fs caused a radiationless photoreaction with a time constant of 1.5 ps, which is interpreted as C=N isomerization through a conical intersection. The orthogonally twisted intermediate state was observed through its excited-state absorption. Bifurcation along pathways towards the ground states of the orange cis and blue trans configurations occurs below the funnel of the conical intersection. The photochromism of the title compound in a very polar solvent such as methanol is observed for the first time.

An interferometric technique has been used to determine the thermooptic coefficient (dn/dT) of polycrystalline ZnSe and ZnS at 0.6328 microm, 1.15 microm, 3.39 microm, and 10.6 microm; polycrystalline CdTe and TI-20 glass at 1.15 microm, 3.39 microm, and 10.6 microm; polycrystalline CaF(2) and BaF(2) at 0.6328 microm, 1.15 microm, and 3.39 microm, and pure and europium-doped single crystal KCl at 0.6328 microm, 1.15microm, 3.39 microm, and 10.6 microm. The values were obtained over the temperature range of 25-65 degrees C and were calculated using the observed change in optical path of the samples as they were heated. Some difficulties in thermometry were encountered in the standard configuration of sample and thermocouple probe, so measurements were made in an oil bath at the shortest wavelength at which the sample was transparent to provide temperature correction factors for each sample. An empirical dispersion relation for dn/dT has also been found for the semiconductor materials. This dispersion relation is of the form dn/dT = aR(b), where R is defined as lambda(2)/(lambda(2) - lambda(g)(2)), lambda(g) is the short wavelength cutoff associated with the energy gap, and a and b are constants which are different for each material.

The ultrafast fluorescence quenching of 2,6-sulfanyl-core-substituted naphthalenediimides was investigated by transient spectroscopy. We find a strong dependence of the relaxation on the chemical structure of the substituent. Direct linking of an aryl rest to the sulfur atom leads to a strong red shift of the fluorescence in 1 ps and the disappearance of the emission in 5-7 ps depending on the polarity and viscosity of the solvent. This complex behavior is interpreted with the help of quantum chemical calculations. The calculations suggest that the initial relaxation corresponds to a planarization of the substituents and an associated partial electron transfer. This is followed by a twisting of the phenylsulfanyl substituents out of the molecular plane that allows a complete localization of the electron-donating orbital on the aryl group. Finally the back transfer happens in another 5-7 ps. For an additional methylene spacer group between the sulfur and the aryl, this sequence of relaxation steps is not possible and a simple exponential decay, slower by about 1 order of magnitude, is found.

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