L Botha

Laser induced and controlled chemical reaction of carbon monoxide and hydrogen

Bimolecular chemical reaction control of gaseous CO and H(2) at room temperature and atmospheric pressure, without any catalyst, using shaped femtosecond laser pulses is presented. High intensity laser radiation applied to a reaction cell facilitates non-resonant bond breakage and the formation of a range of ions, which can then react to form new products. Stable reaction products are measured after irradiation of a reaction cell, using time of flight mass spectroscopy. Bond formation of C-O, C-C, and C-H bonds is demonstrated as CO(2)(+), C(2)H(2)(+), CH(+), and CH(3)(+) were observed in the time of flight mass spectrum of the product gas, analyzed after irradiation. The formation of CO(2) is shown to be dependent on laser intensity, irradiation time, and on the presence of H(2) in the reaction cell. Using negatively chirped laser pulses more C-O bond formation takes place as compared to more C-C bond formation for unchirped pulses.

Comparative Study of the Dissociative Ionization of 1,1,1-Trichloroethane Using Nanosecond and Femtosecond Laser Pulses

Changes in the laser induced molecular dissociation of 1,1,1-trichloroethane (TCE) were studied using a range of intensities and standard laser wavelengths with nanosecond and femtosecond pulse durations. TCE contains C-H, C-C and C-Cl bonds and selective bond breakage of one or more of these bonds is of scientific interest. Using laser ionization time of flight mass spectrometry, it was found that considerable variation of fragment ion peak heights as well as changes in relative peak ratios is possible by varying the laser intensity (by attenuation), wavelength and pulse duration using standard laser sources. The nanosecond laser dissociation seems to occur via C-Cl bond breakage, with significant fragmentation and only a few large mass ion peaks observed. In contrast, femtosecond laser dissociative ionization results in many large mass ion peaks. Evidence is found for various competing dissociation and ionization pathways. Variation of the nanosecond laser intensity does not change the fragmentation pattern, while at high femtosecond intensities large changes are observed in relative ion peak sizes. The total ionization yield and fragmentation ratios are presented for a range of wavelengths and intensities, and compared to the changes observed due to a linear chirp variation.

Optimal Control of the Population Dynamics of the Ground Vibrational State of a Polyatomic Molecule

Simulating coherent control with femtosecond pulses on a polyatomic molecule with anharmonic splitting was demonstrated. The simulation mimicked pulse shaping of a Spatial Light Modulator (SLM) and the interaction was described with the Von Neumann equation. A transform limited pulse with a fluence of 600 J/m2 produced 18% of the population in an arbitrarily chosen upper vibrational state, n =2. Phase only and amplitude only shaped pulse produced optimum values of 60% and 40% respectively, of the population in the vibrational state, n=2, after interaction with the ultra short pulse. The combination of phase and amplitude shaping produced the best results, 80% of the population was in the targeted vibrational state, n=2, after interaction. These simulations were carried out with all the population initially in the ground vibrational level. It was found that even at room temperatures (300 Kelvin) that the population in the selected level is comparable with the case where all population is initially in the ground vibrational state. With a 10% noise added to the amplitude and phase masks, selective excitation of the targeted vibrational state is still possible.

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Modeling of injection seeding of a pulsed high-pressure CO2 laser

A computer model for injection seeding of a high pressure CO2 laser is presented. A rate equation model is used to predict single longitudinal mode (SLM) operation through injection of a cw seed into the resonator cavity. The coupled non-linear differential equations are solved using a Runge-Kutta method. Predictions for the minimum injection power required to produce SLM pulses are made. Detuning off resonance and the effect of the output coupler reflectivity and small signal gain on SLM operation is also considered. Conditions for stable SLM operation through injection of a cw seed are suggested. Single mode operation, even in the detuned case, can be attained due to the homogeneous broadening of the gain, and the rapid growth of the pulse under high gain conditions.