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The Journal of Physical Chemistry A

Coherent Control of Population Transfer in Rydberg Atoms via Chirped Microwave Pulses

Juan J. Carrera, Shih‐I Chu

Published Aug 28, 2007• 3 citations

Abstract

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.

DOI: 10.1021/jp073283r

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We demonstrate theoretically that Li atoms can be transferred to states of a lower principal quantum number by exposing them to a frequency chirped microwave pulse. The population transfer of Li atoms from the n = 75 state to n = 70 with more than 90% efficiency is achieved by means of the sequential single-photon Δn = –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. Using the time-dependent multilevel approach, we describe the process reasonably well as a sequence of adiabatic rapid passages.

The time-dependent multilevel approach (TDMA) and B-spline expansion technique are used to study the coherent population transfer between the quantum states of a potassium atom by a single frequency-chirped microwave pulse. The Rydberg potassium atom energy levels of n = 6–15, l = 0–5 states in zero field are calculated and the results are in good agreement with other theoretical values. The time evolutions of the population transfer of the six states from n = 70 to n = 75 in different microwave fields are obtained. The results show that the coherent control of the population transfer from the lower states to the higher ones can be accomplished by optimizing the microwave pulse parameters.

Using the time-dependent multilevel approach and the B-spline technique, populations of Rydberg lithium atoms in chirped microwave pulses are demonstrated. Firstly the populations of two energy levels are controlled by the microwave pulse parameters. Secondly the atoms experience the consequence 70s-71p-72s-73p-74s in a microwave field using optimized microwave field parameters. It is shown that the coherent control of the population transfer in the microwave field from the initial to the target states can be accomplished by optimizing the microwave field parameters.

Using the time-dependent multilevel approach (TDML), this paper studies the dynamics of coherent control of Rydberg lithium atoms and demonstrates that Rydberg lithium atoms can be transferred to states of higher principal quantum number by exposing them to specially designed frequency-chirped laser pulses. The population transfer from n = 70 to n = 75 states of lithium atoms with efficiency of more than 90% is achieved by means of the sequential adiabatic rapid passages. The results agree well with the experimental ones and show that the coherent control of the population transfer from the lower n to the higher n states can be accomplished by the optimization of the chirping parameters and the intensity of laser field.

The time-dependent multilevel approach (TDMA) and the B-spline expansion technique are used to study the properties of Rydberg lithium atom. The energy level structures of high excited states n = 7075, l = 05 and population transfer of lithium atom in a microwave field are studied by numerical calculation. The results show that the coherent control of the population transfer in microwave field from the initial to the target states can be accomplished by optimizing the microwave field parameters. and that each state plays a crucial role in the transition process.

Using a time-dependent multilevel approach, we demonstrate that lithium atoms can be transferred to states of lower principle quantum number by exposing them to a frequency chirped microwave pulse. The population transfer from n = 79 to n = 70 states of lithium atoms with more than 80% efficiency is achieved by means of the sequential two-photon Δn = −1 transitions. It is shown that the coherent control of the population transfer can be accomplished by the optimization of the chirping parameters and microwave field strength. The calculation results agree well with the experimental ones and novel explanations have been given to understand the experimental results.