Coherent control of population transfer in Rydberg atoms via chirped microwave pulses.

We present a comprehensive and ab initio nonperturbative investigation of the coherent population transfer among the 3D high-lying Rydberg hydrogen and alkali atomic states via linearly polarized chirped microwave pulses. The time-dependent Schrödinger equation for the dynamical evolution of Rydberg atoms is accurately and efficiently solved by means of the time-dependent generalized pseudospectral method. For atomic H, the population transfer from n = 35 to 30 with nearly 100% efficiency is achieved by means of the sequential two-photon Deltan = -1 transitions. The calculation fully utilizes all of the available orbital angular momentum l states for a given n, and the interference pattern and population evolution dynamics of individual l states are analyzed in detail. It is shown that the coherent control of the population transfer from the high n to the low n states can be accomplished by the optimization of the chirping parameters and microwave field strength. Similar analysis is performed for the Na atom, where the alkali atomic structure is described by an accurate model potential. We found that while the global population transfer pattern is qualitatively similar, there are significant differences in the dynamical response of atomic H and Na to the chirped microwave fields. Due to the degeneracy of the l states (for a given n) in unperturbed atomic H, the population transfer involves significant coupling and interference among a number of low-lying l states. For the case of Na atoms, however, the population transfer from the n to (n - 1) state is dominated by a single channel, namely, from the |n,l = 0> to the |n - 1,l = 0> state.