Several schemes for coherent quantum control of atomic and molecular processes have been proposed and investigated by using the techniques of adiabatic passage and ultrashort pulses, respectively. Some interesting results have been found.
Efficient excitation of an ensemble of atoms and molecules to a desired state is of fundamental importance not only for spectroscopy but also for quantum control of molecular dynamics in chemical and biological processes. The latter usually occurs on a much shorter time scale (in the femtosecond range) giving rise to steadily advanced problem how to excite one of the nearby levels, even when they are well within the broad fs pulse spectrum. We propose a new effective method for selective excitation of atoms based on the atomic coherence and discuss a sensitive method to verify experimentally the proposed mechanism using the technique of quantum beating in pump-probe experiments.
Recent advances in the ultrashort laser technology have spawned a series of new directions of research in atomic and molecular physics. This work compounds two studies on the control and probing of atomic matter by ultrafast laser pulses. The first study is concerned with the control of quantum wavepackets focusing by chirped, ultrashort laser pulses. The ability to control wavepacket focusing is important for the achievement of specific excitation pathways, for controlling chemical reactivity or even molecular synthesis. In this work, we present a general method for wavepacket control in the weak field limit. Numerical simulations involving the ICN molecule confirm our theoretical framework. The second study refers to the ionization of sodium Rydberg states via half-cycle pulses (HCPs). For this process, our full quantum-mechanical calculations demonstrate an asymmetry in both ionization rates and ionization spectrum between the downhill (Stark red-shifted) and uphill (Stark blue- shifted) states. The asymmetry is explained by appealing to a semi-classical model of the interfering ionization pathways.
We show that the technique of Stark-chirped rapid adiabatic passage (SCRAP), can be implemented in tripod quantum systems. We propose a scheme for coherent superposition among two ground states via Stark-shiftchirped rapid adiabatic passage technique in a tripod system. Tripod-SCRAP uses four laser pulses: an intense far-off-resonance Stark laser pulse modifies the transition frequency between the states by Stark shifting their energies and three nearly resonant pump, Stokes, and control laser pulses that fractionally transfer the population between the ground states via adiabatic passage. In our scheme, the pulse duration of the pump pulse must be larger than the pulse duration of the Stokes and control pulses, although with a smaller amplitude, and the atom encounters with the pump, Stokes, control, and Stark laser pulses with counterintuitive order (Stokes pulse arrives before the rest of the pulses). This technique can be applied to one-photon as well as multiphoton transitions and it is not necessary to vanish the pulses (pump and Stokes) simultaneously and it is a powerful alternative tool for f-STIRAP and tripod-STIRAP techniques at least when inhomogeneous broadenings are included. inhomogeneous broadening. This technique is robust against moderate variations in the intensities of the laser pulses,in detunings, and in delays between the pulses.