Low-frequency above-threshold ionization of a model two-electron atom.

We calculate the energy spectrum of electrons ejected from a model two-electron atom exposed to an intense laser pulse and follow the spectrum's evolution in time. For the case of 13-photon double ionization, we see the appearance of above-threshold ionization peaks soon after the laser pulse reaches maximum intensity.

Comparing classical and quantum simulations of strong-field double-ionization.

We compare quantum mechanical and fully classical treatments of electron dynamics accompanying strong field double ionization. The major features seen in quantum mechanical simulations, including the double-ionization jets, are reproduced when using a classical ensemble of two-particle trajectories.

Potential surfaces and dynamics of the O(3P)+H2O(X1A1)-->OH(X2pi)+OH(X2pi) reaction.

We present global potential energy surfaces for the three lowest triplet states in O(3P)+H2O(X1A1) collisions and present results of classical dynamics calculations on the O(3P)+H2O(X1A1)-->OH(X2pi)+OH(X2pi) reaction using these surfaces. The surfaces are spline-based fits of approximately 20,000 fixed geometry ab initio calculations at the complete-active-space self-consistent field+second-order perturbation theory (CASSCF+MP2) level with a O(4s3p2d1f)/H(3s2p) one electron basis set. Computed rate constants compare well to measurements in the 1000-2500 K range using these surfaces. We also compute the total, rovibrationally resolved, and differential angular cross sections at fixed collision velocities from near threshold at approximately 4 km s(-1) (16.9 kcal mol(-1) collision energy) to 11 km s(-1) (122.5 kcal mol(-1) collision energy), and we compare these computed cross sections to available space-based and laboratory data. A major finding of the present work is that above approximately 40 kcal mol(-1) collision energy rovibrationally excited OH(X2pi) products are a significant and perhaps dominant contributor to the observed 1-5 micro spectral emission from O(3P)+H2O(X1A1) collisions. Another important result is that OH(X2pi) products are formed in two distinct rovibrational distributions. The "active" OH products are formed with the reagent O atom, and their rovibrational distributions are extremely hot. The remaining "spectator" OH is relatively rovibrationally cold. For the active OH, rotational energy is dominant at all collision velocities, but the opposite holds for the spectator OH. Summed over both OH products, below approximately 50 kcal mol(-1) collision energy, vibration dominates the OH internal energy, and above approximately 50 kcal mol(-1) rotation is greater than vibrational energy. As the collision energy increases, energy is diverted from vibration to mostly translational energy. We note that the present fitted surfaces can also be used to investigate direct collisional excitation of H2O(X1A1) by O(3P) and also OH(X2pi)+OH(X2pi) collisions.

Nonsequential double ionization as a completely classical photoelectric effect.

We introduce a unified and simplified theory of atomic double ionization. Our results show that at high laser intensities (I>/=10(14) W/cm(2)) purely classical correlation is strong enough to account for all of the main features observed in experiments to date.

Slow-down collisions and nonsequential double ionization in classical simulations.

We use classical simulations to analyze the dynamics of nonsequential double-electron short-pulse photoionization. We utilize a microcanonical ensemble of 10(5) two-electron "trajectories," a number large enough to provide large subensembles and even sub-subensembles associated with double ionization. We focus on key events in the final doubly ionized subensemble and back-analyze the subensemble's history, revealing a classical slow-down scenario for nonsequential double ionization. We analyze the dynamics of these slow-down collisions and find that a good phase match between the motions of the electrons can lead to very effective energy transfer, followed by escape over a suppressed barrier.