Numerical investigation of enhanced femtosecond supercontinuum via a weak seed in noble gases.

Numerical simulations are employed to elucidate the physics underlying the enhanced femtosecond supercontinuum generation previously observed during optical filamentation in noble gases and in the presence of a weak seed pulse. Simulations based on the metastable electronic state approach are shown not only to capture the qualitative features of the experiment, but also reveal the relation of the observed enhancement to recent developments in the area of sub-cycle engineering of filaments.

Antitumor polycyclic acridines. 7. Synthesis and biological properties of DNA affinic tetra- and pentacyclic acridines.

New synthetic routes to a series of tetra- and pentacyclic acridines related in structure to marine natural products are reported. The novel water-soluble agent dihydroindolizino[7,6,5-kl]acridinium chloride 14 has inhibitory activity in a panel of non-small-cell lung and breast tumor cell lines exceeding that of m-AMSA. The salt inhibited the release of minicircle products of kDNA confirming that disorganization of topoisomerase II partly underlies the activity of the compound. COMPARE analysis of the NCI mean graph profile of compound 14 at the GI(50) level corroborates this conclusion with Pearson correlation coefficients (>0.6) to clinical agents of the topoisomerase II class: however, this correlation was not seen at the LC(50) level. The inhibitory action of 14 on Saccharomyces cerevisiae transfected with human topoisomerase II isoforms showed a 3-fold selectivity against the IIalpha isoform over the IIbeta isoform. Unlike m-AMSA, 14 is not susceptible to P-glycoprotein-mediated drug efflux and retains activity in lung cells with derived resistance to the topoisomerase II inhibitor etoposide.

High-dynamic-range cascaded-focus optical limiter.

We report experimental results of using an f/5 , cascaded-focus optical geometry for a high-dynamic-range optical limiter. The device consists of a 2-cm-thick CS(2) cell at the first focus and a reverse saturable-absorber dye in a thin cell (0.1 mm) at the second focus. The strong self-focusing in the CS(2) that is due to the ac Kerr effect and electrostriction keeps the energy at the second cell below its damage threshold. Using lead phthalocyanine in chloroform as the reverse saturable-absorption material, we clamped the maximum output energy below 1muJ for input energies up to 14.5 mJ without damage. We used a frequency-doubled, Q -switched 5-ns (FWHM) Nd:YAG laser operating at a 10-Hz repetition rate. The measured dynamic range of the device is at least 7500.

Investigation of an optical limiting mechanism in multiwalled carbon nanotubes.

We report our investigation of the mechanism that is responsible for the optical limiting behavior in multiwalled carbon nanotubes. We conducted energy-dependent transmission measurements, picosecond time-resolved pump-probe experiment, and nonlinear scattering experiments at 532-nm wavelength on multiwalled carbon nanotube suspension. For comparison, C(60)-toluene solutions and carbon black suspensions were also studied in the same experiments. The similarities that we observed between the multiwalled carbon nanotubes and carbon black suspension suggest that nonlinear scattering, which is known to be responsible for the limiting action in carbon black suspension, should play an important role in the limiting effect in multiwalled carbon nanotubes.

Nonlinear optical beam propagation for optical limiting.

We implement numerical modeling of high-energy laser-pulse propagation through bulk nonlinear optical materials using focused beams. An executable program with a graphical user interface is made available to researchers for modeling the propagation of beams through materials much thicker than the diffraction length (up to 10(3) times longer). Ultrafast nonlinearities of the bound-electronic Kerr effect and two-photon absorption as well as time-dependent excited-state and thermal nonlinearities are taken into account. The hydrodynamic equations describing the rarefaction of the medium that is due to heating are solved to determine thermal index changes for nanosecond laser pulses. We also show how this effect can be simplified in some cases by an approximation that assumes instantaneous expansion (so-called thermal lensing approximation). Comparisons of numerical results with several Z-scan, optical limiting and beam distortion experiments are presented. Possible application to optimization of a passive optical limiter design is discussed.

Optimization of optical limiting devices based on excited-state absorption.

Limiting devices protect sensitive optical elements from laser-induced damage (LID). Passive devices use focusing optics to concentrate the light through a nonlinear optical (NLO) element (or elements) to reduce the limiting threshold. Unfortunately, these NLO elements may themselves undergo LID for high inputs, restricting the useful dynamic range (DR). Recently, efforts at optimizing this DR have focused on distributing the NLO material along the propagation path z of a focused beam, resulting in different portions of the device (in z) exhibiting NLO response at different inputs. For example, nonlinear absorbers closer to the lens, i.e., upstream, protect device elements downstream near the focal plane. This results in an undesirable increase in the threshold, although the lowest threshold is always obtained with the final element at focus. Thus there is a compromise between DR and threshold. This compromise is determined by the material. We concentrate on reverse saturable absorber (RSA) materials (molecules exhibiting larger excited-state than ground-state absorption). We look at both tandem devices and devices in which the concentration of the NLO material is allowed to spatially vary in z. These latter devices require solid-state hosts. The damage threshold of currently available solid-state hosts is too low to allow known RSA materials to reach their maximum absorption, which occurs when all molecules are in their excited state. This is demonstrated by approximate analytical methods as well as by a full numerical solution of the nonlinear wave propagation equation over extremely large distances in z (up to 10(3)Z(0), where Z(0) is the Rayleigh range of the focused beam). The numerical calculations, based on a one-dimensional fast Fourier transform, indicate that proper inclusion of diffraction reduces the effectiveness of reverse saturable absorption for limiting, sometimes by more than a factor of 10. Liquid-based devices have higher damage thresholds (damage occurs to the cuvette wall) and, thus, larger nonlinear absorption. However, RSA material in liquid hosts may suffer from larger thermal lensing.

Measurement of the optical damage threshold in fused quartz.

The damage thresholds of five different types of quartz glass used for the production of spectroscopic cuvettes for liquids were determined with single temporal and spatial mode nanosecond pulses at 532 nm. One of the glasses had a damage threshold of ≃420 J/cm(2), which was more than twice that of the other glasses.

Eclipsing Z-scan measurement of lambda/10(4) wave-front distortion.

We introduce a simple modification to the Z-scan technique that results in a sensitivity enhancement that permits measurement of nonlinearly induced wave-front distortion of =lambda/10(4). This sensitivity was achieved with 10-Hz repetition-rate pulsed laser sources. Sensitivity to nonlinear absorption is also enhanced by a factor of =3. This method permits characterization of nonlinear thin films without the need for waveguiding.

Phase-controlled transistor action by cascading of second-order nonlinearities in KTP.

We demonstrate a 4.6-to-1 modulation depth imposed on the fluence of an intense 1.06-microm picosecond pulse by varying the relative phase of a weak second-harmonic control pulse under near phase-matched conditions. This transistorlike action is based on quadratic nonlinearities in KTP.

Self-focusing and self-defocusing by cascaded second-order effects in KTP.

We monitor the induced phase change produced by a cascaded chi((2)):chi((2)) process in KTP near the phase-matching angle on a picosecond 1.06-microm-wavelength beam using the Z-scan technique. This nonlinear refraction is observed to change sign as the crystal is rotated through the phase-match angle in accordance with theory. This theory predicts the maximum small-signal effective nonlinear refractive index of n(eff)(2) congruent with +/-2 x 10(-14) cm(2)/W (+/-1 x 10(-11) esu) for an angle detuning of +/-5 degrees from phase match for this 1-mm-thick crystal with a measured d(eff) of 3.1 pm/V. For a fixed phase mismatch, this n(eff)(2) scales linearly with length and as d(eff)(2) however, for the maximum n(eff)(2) the nonlinear phase distortion becomes sublinear with irradiance for phase shifts near pi/4.

Measurement of nondegenerate nonlinearities using a two-color Z scan.

A simple dual-wavelength (two-color) Z-scan geometry is demonstrated for measuring nonlinearities at frequency omega(p) owing to the presence of light at omega(e). This technique gives the nondegenerate two-photon absorption (2PA) coefficient beta(omega(p); omega(e)) and the nondegenerate nonlinear refractive index n(2)(omega(p); omega(e)), i.e., cross-phase modulation. We demonstrate this technique on CS(2) for n(2) and on ZnSe where 2PA and n(2) are present simultaneously.

Self-protecting semiconductor optical limiters.

We present a detailed characterization of passive, picosecond optical-power-limiting devices using tightly focused beams in thick semiconductor samples. This study of limiting in ZnSe with 30-psec, 532-nm pulses shows that the resulting internal self-action (two-photon absorption plus free-carrier self-defocusing) protects the bulk material from optical damage. Simple scaling relations were determined from our results that link the limiting energy and the dynamic range to the focusing geometry and sample dimensions. These relations were used to design a monolithic optical limiter, optimized to have maximum dynamic range and minimum limiting energy. This device limits at an input energy of 10 nJ (300 W) and has a dynamic range greater than 10(4).

Diffusive transverse coupling between adjacent InSb transphasor channels.

The proportionality of a transphasor signal to the photoexcited carrier density has been utilized to measure the transfer of the signal between adjacent optical channels and to estimate practical transphasor packing densities (~10(3) cm(-2)) for a pure, bulk étalon of InSb, 280 microm thick. By using the transphasor as a probe of the carrier population distribution produced by an adjacent beam, the ambipolar diffusion length was measured as 74 microm.

Carrier diffusion measurements in InSb by the angular dependence of degenerate four-wave mixing.

Studies of the angular dependence of cw degenerate four-wave mixing in n-type InSb have yielded a value for the diffusion length, l(D), of 60 +/- 2 microm. From this, the dependence of l(D) on photoexcited carrier concentration is calculated. A simple model has been developed to estimate the corresponding parallel-processing capabilities of semi-conductor-based, all-optical, parallel-processing digital computing systems.