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Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train - a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.
Ultrafast processes in matter can be captured and even controlled by using sequences of few-cycle optical pulses, which need to be well characterized, both in amplitude and phase. The same degree of control has not yet been achieved for few-cycle ext
A density matrix approach is developped for the control of a mixed-state quantum system using a time-dependent external field such as a train of pulses. This leads to the definition of a target density matrix constructed in a reduced Hilbert space as
We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detecti
We present a systematic approach based on Bloch vectors treatment and the Magnus quantum electrodynamical formalism to study qubit manipulation by a train of pulses. These investigations include one of the basic processes involved in quantum computat
A quasi-classical model (QCM) of molecular dynamics in intense femtosecond laser fields has been developed, and applied to a study of the effect of an ultrashort `control pulse on the vibrational motion of a deuterium molecular ion in its ground elec