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We report on the selective ionization of oriented nonpolar molecules with asymmetric structure by using phase-controlled two-color omega + 2omega laser pulses with an intensity of 1.0 x 10(13) W/cm(2) (tunneling ionization regime) and a pulse duration of 130 fs. The orientation of 1-bromo-2-chloroethane was monitored by the directional asymmetries of the forward-backward emission in dissociative ionization. The observed direction of orientation clearly confirms that molecular orientation is induced not by dynamic orientation but by selective ionization of oriented molecules, which reflects the structure of the highest occupied molecular orbital. This method can be applied for the vast majority of molecules.

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The mechanisms of anisotropic near-IR tunnel ionization and high-order harmonic generation (HHG) in a CO molecule are theoretically investigated by using the multiconfiguration timedependent Hartree-Fock (MCTDHF) method developed for the simulation of multielectron dynamics of molecules. The multielectron dynamics obtained by numerically solving the equations of motion (EOMs) in the MCTDHF method is converted to a single orbital picture in the natural orbital representation where the first-order reduced density matrix is diagonalized. The ionization through each natural orbital is examined and the process of HHG is classified into different optical paths designated by a combinations of initial, intermediate and final natural orbitals. The EOMs for natural spin-orbitals are also derived within the framework of the MCTDHF, which maintains the first-order reduced density matrix to be a diagonal one throughout the time propagation of a many-electron wave function. The orbital dependent, timedependent effective potentials that govern the dynamics of respective time-dependent natural orbitals are deduced from the derived EOMs, of which the temporal variation can be used to interpret the motion of the electron density associated with each natural spin-orbital. The roles of the orbital shape, multiorbital ionization, linear Stark effect and multielectron interaction in the ionization and HHG of a CO molecule are revealed by the effective potentials obtained. When the laser electric field points to the nucleus O from C, tunnel ionization from the C atom side is enhanced; a hump structure originating from multielectron interaction is then formed on the top of the field-induced distorted barrier of the HOMO effective potential. This hump formation, responsible for the directional anisotropy of tunnel ionization, restrains the influence of the linear Stark effect on the energy shifts of bound states.

We have investigated coherent control of the dissociative ionization of IBr using phase-controlled two-color omega+2omega laser pulses with an intensity of 1.0 x 10(12) W/cm and a pulse duration of 130 fs. The directional asymmetries of the photofragment angular distributions showed oscillation behavior dependent on the relative phase difference between the omega and 2omega pulses. The phase dependencies of the directional asymmetries observed for iodine ions and bromine ions were out of phase with each other. This result shows that a phase-controlled omega+2omega optical field can produce molecular orientation in which the optical field discriminates between parallel and antiparallel configuration of molecules that have a permanent dipole.

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