Field-free orientation of CO molecules by femtosecond two-color laser fields

We report the first experimental observation of non-adiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion angular distributions after Coulomb explosion with an 800 nm pulse. The orientation of the molecules is controlled by the relative phase of the two-color field. The results are compared to quantum mechanical rigid rotor calculations. The demonstrated method can be applied to study molecular frame dynamics under field-free conditions in conjunction with a variety of spectroscopy methods, such as high-harmonic generation, electron diffraction and molecular frame photoemission

Following dynamic nuclear wave packets in N2,O2, and CO with few-cycle infrared pulses

We study the evolution of nuclear wave packets launched in molecular nitrogen, oxygen, and carbon monoxide by intense 8-fs infrared pulses. We use velocity map imaging to measure the momentum of the ion fragments when these wave packets are interrogated by a second such pulse after a variable time delay. Both quasibound and dissociative wave packets are observed. For the former, measurements of bound-state oscillations are used to identify the participating states and, in some cases, extract properties of the relevant potential-energy surfaces. Vibrational structure is resolved in both energy and oscillation frequencies for the cations of oxygen and carbon monoxide, displaying the same quantum wave-packet motion in both energy and time domains. In addition, vibrational structure is seen in the dication of carbon monoxide in a situation where the energy resolution by itself is inadequate to resolve the structure