Efficient Pd-catalyzed Heck coupling methodology was employed to provide two new fluorene derivatives with phosphonate (2) and nitro (3) electron-withdrawing functionalities. Both derivatives exhibit two-photon absorption (2PA), as determined by nonlinear absorption measurements using a femtosecond pump/white light continuum probe “NLO spectrometer”. Both fluorene derivatives have high 2PA cross sections (650 and 1300 × 10-50 cm4 s photon-1 molecule-1 for compounds 2 and 3, respectively).

We present an experimental technique along with the method of data analysis to give nondegenerate two-photon absorption (2PA) spectra. We use a femtosecond pump pulse and a white-light continuum (WLC) probe to rapidly generate the 2PA spectra of a variety of materials. In order to analyze data taken with this method, the spectral and temporal characteristics of the WLC must be known, along with the linear dispersion of the sample. This allows determination of the temporal walk-off of the pump and probe pulses as a function of frequency caused by group-velocity mismatch. Data correction can then be performed to obtain the nonlinear losses. We derive an analytical formula for the normalized nonlinear transmittance that is valid under quite general experimental parameters. We verify this on ZnS and use it for the determination of 2PA spectra of some organic compounds in solution. We also compare some of the data on organics with two-photon fluorescence data and find good agreement.

Laser-induced damage at near operational laser excitation conditions can limit the performance of potassium dihydrogen phosphate (KH(2)PO(4), or KDP) and its deuterated analog (DKDP) which are currently the only nonlinear optical materials suitable for use in large-aperture laser systems. This process has been attributed to pre-existing damage precursors that were incorporated or formed during growth that have not yet been identified. In this work, we present a novel experimental approach to probe the electronic structure of the damage precursors. The results are modeled assuming a multi-level electronic structure that includes a bottleneck for 532 nm excitation. This model reproduces our experimental observations as well as other well-documented behaviors of laser damage in KDP crystals. Comparison of the electronic structure of known defects in KDP with this model allows for identification of a specific class that we postulate may be the constituent defects in the damage precursors. The experimental results also provide evidence regarding the physical parameters affecting the ability of individual damage precursors to initiate damage, such as their size and defect density; these parameters were found to vary significantly between KDP materials that exhibit different damage performance characteristics.

We report the two-photon-induced photoisomerization of 3-[1-(1,2-dimethyl-1H-indol-3-yl)-ethylidene]-4-isopropylidene-dihydrofuran-2,5-dione (1), a photochromic compound with λ max ) 385 nm, using 775-nm femtosecond pulsed laser irradiation. The resulting photoisomer had λ max ) 582 nm. The kinetic rate constant for the two-photon-induced electrocyclic isomerization reaction was measured at two different intensities (two different powers), showing a quadratic dependence with respect to the pump intensity. Results of pump-probe solution phase experiments and guest/host polymer thin film interferometric imaging studies are reported. A two-photon absorption molecular cross section σ2 ) 10.3 × 10 -48 cm 4 ‚s/photon was measured using Z-scan, further supporting a two-photon-induced isomerization process. Two-photon-induced interferometric recording in a fulgide-containing polymer film was demonstrated.

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The growth behavior of laser-induced damage sites is affected by a large number of laser parameters as well as site morphology. Here we investigate the effects of pulse duration on the growth rate of damage sites located on the exit surface of fused silica optics. Results demonstrate a significant dependence of the growth parameters on laser pulse duration at 351 nm from 1 ns to 15 ns, including the observation of a dominant exponential versus linear, multiple-shot growth behavior for long and short pulses, respectively. These salient behaviors are tied to the damage morphology and suggest a shift in the fundamental growth mechanisms for pulses in the 1-5 ns range.

The material response following nanosecond, UV laser induced breakdown inside of the exit surface of fused silica is investigated using multimodal time resolved microscopy. The study spans up to about 75 ns delay from the onset of material modification during the laser pulse through the observation of material ejection. A number of distinct processes were identified, including: a) the onset of optical absorption in the material arising from the buildup of an electronic excitation, b) the expansion of the hot modified region (plasma) along the surface and inside the bulk, c) the formation of radial and circumferential cracks, d) the swelling of the affected region on the surface and, e) the onset of ejection of material clusters at about 30 ns delay and its progression to a well‐defined jet by about 75 ns delay. Limited theoretical modeling is used to aid the interpretation of the data.

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