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Physical Review A

Coherent population transfer among Rydberg states by subpicosecond, half-cycle pulses

N. E. Tielking, R. R. Jones

Published Aug 1, 1995• 53 citations
Publisher

Abstract

Ultrashort, unipolar electric-field pulses have been used to coherently redistribute population between Rydberg states in sodium. The population in several Rydberg states is recorded simultaneously as a function of peak field. In addition, two temporally separated pulses have been used to interferometrically characterize the redistribution process. In the lowest fields, the experimental results are in agreement with the predictions of lowest-order perturbation theory. At slightly higher fields, still well below the ionization threshold, the redistribution process becomes nonperturbative, and a numerical integration of the time-dependent Schr\"odinger equation must be used to achieve partial agreement between theory and experiment.

DOI
10.1103/physreva.52.1371

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Ultrashort, unipolar electric-field pulses have been used to coherently redistribute population between Rydberg states in sodium. The population in several Rydberg states is recorded simultaneously as a function of peak field. In addition, two temporally separated pulses have been used to interferometrically characterize the redistribution process. In the lowest fields, the experimental results are in agreement with the predictions of lowest-order perturbation theory. At slightly higher fields, still well below the ionization threshold, the redistribution process becomes nonperturbative, and a numerical integration of the time-dependent Schr"odinger equation must be used to achieve partial agreement between theory and experiment.
In this paper, ultrashort, unipolar electric-field (terahertz) pulses have been used to coherently control population transfer between Rydberg states in lithium atom. Our numerical results show that populations of lithium atoms can be driven to lower or higher n levels with a train of half-cycle pulses, and the the transition rate is sensitive to the static-electric-field strength, the main laser frequency, the optical pulse profile, and the chirp of the laser pulse. If the paramerters of the half-cycle pulses is optimized appropriately, the population can be transferred to the target state completely.
Ultrashort, nearly unipolar electric field pulses are used to produce novel dynamic states in Rydberg atoms. A single 500 fsec field pulse redistributes essentially all of the population from a single stationary Rydberg state to hundreds of different final states. The dynamic evolution of the nonstationary wave packet is monitored using a second, time-delayed pulse. The time-dependent momentum-space probability distribution of the wave packet can be retrieved experimentally using a classical impulse approximation.
Expanding the wave function in terms of eigenstates, we calculated the population redistribution of high-Rydberg hydrogen atoms under the interactions of external time-dependent electromagnetic fields. Our numerical results show that populations of Rydberg atoms can be driven down to lower nnn levels with a train of half-cycle pulses. Oscillations of the Rydberg population through both nnn levels and lll levels are observed during these interactions. The approach may have applications in providing an effective mechanism for producing near ground-state atoms from the initially high-Rydberg distributions found in recombining ultracold plasmas such as encountered in the antihydrogen trapping experiments at CERN.
We present the technique and results of our study of the redistribution of Rydberg states in barium by a half cycle pulse (HCP). A survey of previous research concerning the interaction of half cycle pulses with Rydberg atoms reveals a lack of experimental data in the area of state redistribution. This is primarily due to an inability to identify the redistributed states accurately using the currently available tool: selective field ionization (SFI). We present the limitations of SFI as a state identification tool. We then present a survey of isolated core excitation as a state identification tool, along with its limitations in dealing with a mixture of states. Combining SFI and ICE overcomes these limitations and allows for the accurate characterization of a mixture of Rydberg states, as found in HCP redistribution. We present our results for the HCP redistribution of a series of ns and nd initial states, for n from 30 to 40, at various HCP intensities. These results primarily involved single photon transitions, confining us to the linear regime. Analyzing the results of these redistributions with respect to the energy difference between initial and final states yielded information about the frequency structure, after transmission to the interaction region, of the HCP. This led us to postulate on the effects of diffraction on the HCP. We conclude with several suggestions for the improvement of the experimental system, as well as a direction for future research.
We have ionized Rydberg atoms using subpicosecond half-cycle electromagnetic pulses. The threshold electric field required to ionize a Rydberg state with effective quantum number n∗{\mathit{n}}^{\mathrm{*}}n∗ is found to scale as ${\mathit{n}}^{\mathrm{*}\mathrm{\ensuremath{-}}2}$ for states with n∗{\mathit{n}}^{\mathrm{*}}n∗>13 in contradistinction to the ${\mathit{n}}^{\mathrm{*}\mathrm{\ensuremath{-}}4}$ threshold scaling for static field ionization and high order multiphoton ionization. This novel result is explained using a classical model.