Pseudo-time Schroedinger equation with absorbing potential for quantum scattering calculations

The Schroedinger equation with an energy-dependent complex absorbing potential, associated with a scattering system, can be reduced for a special choice of the energy-dependence to a harmonic inversion problem of a discrete pseudo-time correlation function. An efficient formula for Green's function matrix elements is also derived. Since the exact propagation up to time 2t can be done with only t real matrix-vector products, this gives an unprecedently efficient scheme for accurate calculations of quantum spectra for possibly very large systems.Comment: 9 page

Coherent Control of Isotope Separation in HD+ Photodissociation by Strong Fields

The photodissociation of the HD+ molecular ion in intense short- pulsed linearly polarized laser fields is studied using a time- dependent wave-packet approach where molecular rotation is fully included. We show that applying a coherent superposition of the fundamental radiation with its second harmonic can lead to asymmetries in the fragment angular distributions, with significant differences between the hydrogen and deuterium distributions in the long wavelength domain where the permanent dipole is most efficient. This effect is used to induce an appreciable isotope separation.Comment: Physical Review Letters, 1995 (in press). 4 pages in revtex format, 3 uuencoded figures. Full postcript version available at: http://chemphys.weizmann.ac.il/~charron/prl.ps or ftp://scipion.ppm.u-psud.fr/coherent.control/prl.p

The dynamical Green's function and an exact optical potential for electron-molecule scattering including nuclear dynamics

We derive a rigorous optical potential for electron-molecule scattering including the effects of nuclear dynamics by extending the common many-body Green's function approach to optical potentials beyond the fixed-nuclei limit for molecular targets. Our formalism treats the projectile electron and the nuclear motion of the target molecule on the same footing whereby the dynamical optical potential rigorously accounts for the complex many-body nature of the scattering target. One central result of the present work is that the common fixed-nuclei optical potential is a valid adiabatic approximation to the dynamical optical potential even when projectile and nuclear motion are (nonadiabatically) coupled as long as the scattering energy is well below the electronic excitation thresholds of the target. For extremely low projectile velocities, however, when the cross sections are most sensitive to the scattering potential, we expect the influences of the nuclear dynamics on the optical potential to become relevant. For these cases, a systematic way to improve the adiabatic approximation to the dynamical optical potential is presented that yields non-local operators with respect to the nuclear coordinates.Comment: 22 pages, no figures, accepted for publ., Phys. Rev.

The role of the geometric phases in adiabatic population tracking for non-Hermitian Hamiltonians

International audienceThe definition of instantaneous eigenstate populations for a dynamical non-self-adjoint system is not obvious. The naive direct extension of the definition used for the self-adjoint case leads to inconsistencies; the resulting artifacts can induce a false inversion of population or a false adiabaticity. We show that the inconsistency can be avoided by introducing geometric phases in another possible definition of populations. An example is given which demonstrates both the anomalous effects and their removal by our approach

Discussion of the adiabatic hypothesis in control schemes using exceptional points

International audienceWe present calculations for the action of laser pulses on vibrational transfer within the H-2(+) and Na-2 molecules in the presence of dissipation due to photodissociation of the molecule. The laser fields perform closed loops surrounding exceptional points in the laser parameter plane of intensity and wavelength. In principle the process should produce controlled vibrational transfers due to an adiabatic flip of the dressed eigenstates. We directly solve the Schrodinger equation with the complete time-dependent field instead of using the adiabatic Floquet formalism which initially suggested the design of the laser pulses. Results given by wavepacket propagations disagree with predictions obtained using the adiabatic hypothesis. Thus we show that there are large non-adiabatic exchanges and that the dissipative character of the dynamics renders the adiabatic flip very difficult to obtain. Using much longer durations than expected from previous studies, the adiabatic flip is only obtained for the Na-2 molecule and with strong dissociation