With the recently introduced concept of dominant interaction Hamiltonians, we construct numerically as well as analytically the spectrum of high harmonics (HH) generated in electron-ion scattering under an intense laser field. This is achieved by switching the interaction along classical electron trajectories between the integrable cases of the dipole coupled laser field or the ionic potential, depending on which potential is stronger. As a side effect, the intrinsically chaotic character of the dynamics is mapped onto the potential switching sequence while the trajectories become regular. As a consequence, only a few per cent of the trajectories needed in full semiclassical calculations are sufficient to construct the HH spectrum.
Applying the recently developed semiclassical hybrid dynamics [Grossmann, J. Chem. Phys. 125, 014111 (2006)], we study the decay of interference patterns in the reduced density as well as of the purity in a Morse oscillator test system due to the interaction with a finite harmonic bath at zero temperature. In the case that the bath mimics a continuous Ohmic spectral density, in addition to the quantum classical transition induced by the interaction with the environment, we corroborate the existence of a blueshift due to the bath coupling, predicted by Pollak [Phys. Rev. A 33, 4244 (1986)]. Furthermore, the decoherence dynamics of cat states is confirmed to be faster than that of single coherent states and we show that for a resonant bath the dissipation leads to an increase in the decoherence rate as compared to the low frequency bath.
We study the vibrational decoherence dynamics of an iodine molecule in a finite krypton cluster comprising the first solvation shell. A normal mode analysis allows us to successively increase the complexity of the description. For the ground state dynamics, comparison with experimental matrix results shows that already four degrees of freedom are sufficient to capture the main decoherence mechanism. For electronically excited iodine, we model the vibrational dynamics of initial Schrödinger cat-like states by the semiclassical hybrid dynamics [Grossmann, F. J. Chem. Phys. 2006, 125, 014111] and full quantum calculations, where available. Good agreement of the results is found for a reduced model with three degrees of freedom. We find non-Gaussian distortions of the bath density matrix, which is a necessary condition, if Schrödinger catlike states in the bath are to be identified. However, in contrast to the experiment [Segale, D.; et al. J. Chem. Phys. 2005, 122, 111104], we observe only incoherent superpositions of bath vibrational states.
Quantized systems whose underlying classical dynamics possess an elaborate mixture of regular and chaotic motion can exhibit rather subtle long-time quantum transport phenomena. In a short wavelength regime where semiclassical theories are most relevant, such transport phenomena, being quintessentially interference based, are difficult to understand with the system's specific long-time classical dynamics. Fortunately, semiclassical methods applied to wave packet propagation can provide a natural approach to understanding the connections, even though they are known to break down progressively as time increases. This is due to the fact that some long-time transport properties can be deduced from intermediate-time behavior. Thus, these methods need only retain validity and be carried out on much shorter time scales than the transport phenomena themselves in order to be valuable. The initial value representation of the semiclassical propagator of Herman and Kluk [Chem. Phys. 91, 27 (1984)] is heavily used in a number of molecular and atomic physics contexts, and is of interest here. It is known to be increasingly challenging to implement as the underlying classical chaos strengthens, and we ask whether it is possible to implement it well enough to extract the kind of intermediate-time information that reflects wave packet localization at long times. Using a system of two coupled quartic oscillators, we focus on the localizing effects of transport barriers formed by stable and unstable manifolds in the chaotic sea and show that these effects can be captured with the Herman-Kluk propagator.
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