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Register a new userIonization of molecular hydrogen and deuterium by a frequency-doubled Ti:sapphire laser pulses
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A theoretical study of the intense-field single ionization of molecular hydrogen or deuterium oriented either parallel or perpendicular to a linear polarized laser pulse (400 nm) is performed for different internuclear separations and pulse lengths in an intensity range of $(2-13)times10^{13} $W cm$^{-2}$. The investigation is based on a non-perturbative treatment that solves the full time-dependent Schrodinger equation of both correlated electrons within the fixed-nuclei and the dipole approximation. The results for various internuclear separations are used to obtain the ionization yields of molecular hydrogen and deuterium in their ground vibrational states. An atomic model is used to identify the influence of the intrinsic diatomic two-center character of the problem.
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We present experimental results for the ionization of aniline and benzene molecules subjected to intense ultrashort laser pulses. Measured parent molecular ions yields were obtained using a recently developed technique capable of three-dimensional imaging of ion distributions within the focus of a laser beam. By selecting ions originating from the central region of the focus, where the spatial intensity distribution is nearly uniform, volumetric-free intensity-dependent ionization yields were obtained. The measured data revealed a previously unseen resonant-like multiphoton ionization process. Comparison of benzene, aniline and Xe ion yields demonstrate that the observed intensity dependent structures are not due to geometric artifacts in the focus. Finally we attribute the ionization of aniline to a stepwise process going through the pi-sigma^star state which sits 3 photons above the ground state and 2 photons below the continuum.
A quasi-classical model (QCM) of molecular dynamics in intense femtosecond laser fields has been developed, and applied to a study of the effect of an ultrashort `control pulse on the vibrational motion of a deuterium molecular ion in its ground electronic state. A nonadiabatic treatment accounts for the initial ionization-induced vibrational population caused by an ultrashort `pump pulse. In the QCM, the nuclei move classically on the molecular potential as it is distorted by the laser-induced Stark shift and transition dipole. The nuclei then adjust to the modified potential, non-destructively shifting the vibrational population and relative phase. This shift has been studied as a function of control pulse parameters. Excellent agreement is observed with predictions of time-dependent quantum simulations, lending confidence to the validity of the model and permitting new observations to be made. The applicability of the QCM to more complex multi-potential energy surface molecules (where a quantum treatment is at best difficult) is discussed.
The alignment dependence of the ionization behavior of H$_2$ exposed to intense ultrashort laser pulses is investigated on the basis of solutions of the full time-dependent Schrodinger equation within the fixed-nuclei and dipole approximation. The total ionization yields as well as the energy-resolved electron spectra have been calculated for a parallel and a perpendicular orientation of the molecular axis with respect to the polarization axis of linear polarized laser pulses. For most, but not all considered laser peak intensities the parallel aligned molecules are easier to ionize. Furthermore, it is shown that the velocity formulation of the strong-field approximation predicts a simple interference pattern for the ratio of the energy-resolved electron spectra obtained for the two orientations, but this is not confirmed by the full ab initio results.
We investigate molecular dynamics of multiple ionization in N2 through multiple core-level photoabsorption and subsequent Auger decay processes induced by intense, short X-ray free electron laser pulses. The timing dynamics of the photoabsorption and dissociation processes is mapped onto the kinetic energy of the fragments. Measurements of the latter allow us to map out the average internuclear separation for every molecular photoionization sequence step and obtain the average time interval between the photoabsorption events. Using multiphoton ionization as a tool of multiple-pulse pump-probe scheme, we demonstrate the modification of the ionization dynamics as we vary the x-ray laser pulse duration.
We have constructed a pulsed laser system for the manipulation of cold Rb atoms. The system combines optical telecommunications components and frequency doubling to generate light at 780 nm. Using a fast, fibre-coupled intensity modulator, output from a continuous laser diode is sliced into pulses with a length between 1.3 and 6.1 ns and a repetition frequency of 5 MHz. These pulses are amplified using an erbium-doped fibre amplifier, and frequency-doubled in a periodically poled lithium niobate crystal, yielding a peak power up to 12 W. Using the resulting light at 780 nm, we demonstrate Rabi oscillations on the F = 2 <-> F=3-transition of a single 87Rb atom.
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