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Bulletin of the American Physical Society

Population of Rydberg states in short intense laser pulses

Joel Venzke, Brynn Reiff, Zetong Xue, Erez Shani, Agnieszka Jaroń-Becker, Andreas Becker

Published Oct 21, 2017• 0 citations
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When exposed to intense light of \ensuremath{\sim}580 nm, the ground state of K shifts up in energy, passing through two-photon resonances with Rydberg states and finally crossing the two-photon ionization limit. Using laser pulses of 0.5 to 13 ps duration, we have shown experimentally that ionization occurs for short pulses, but for long pulses the population is diverted into the Rydberg states where some population survives the peak intensity of the pulse, in excellent agreement with a dynamic Floquet model.
We conduct a systematic investigation of the oscillations of the Rydberg-state populations as a function of intensity arising from strong-field multiphoton excitation of Rydberg atoms. By numerically solving the time-dependent Schrödinger equation and by constructing a quantum model based on Freeman resonances, we elucidate the underlying physical mechanisms governing the intensity-dependent oscillatory behavior of the Rydberg-state population dynamics. Our analysis shows that these oscillations originate from the synergistic interplay of three distinct quantum-interference mechanisms: (1) interference between excitation pathways at the rising and falling edges of the laser pulse (long-time interference), (2) interference between different optical cycles within the same side of the laser pulse (short-time interference), and (3) interference within individual optical cycles (intracycle interference). Additionally, we find that ground-state depletion has varying degrees of influence on the oscillation patterns formed by the three interference mechanisms under different laser-intensity conditions.
Our recent approximate analytical results on the evolution of the initial state and the excitation from this state of a band of high Rydberg states by an optical pulse [Phys. Rev. A 55, 2144 (1997)] are compared with more exact numerical results. The difference between the two approaches is that the approximations of representative atom-field couplings and equidistant spacing of high Rydberg states, applied in the analytical model, are removed in the numerical model. We find that the approximate analytical model is not able to reproduce all the results of the more exact numerical model, if the laser pulse is very short (i.e., much shorter that the Kepler period of the resonantly excited high Rydberg state) or very intense (i.e., when the Rabi period for the resonant transition is substantially shorter than the above Kepler period). This mainly concerns the redistribution of the population over different Rydberg states. The analytical model predicts a symmetric distribution centered around the resonantly excited Rydberg state, irrespective of the pulse duration and intensity, while the numerical model allows an asymmetric distribution with its maximum shifted towards lower Rydberg states. Despite the above-stated difference, the analytical model is able to give preliminary results for the total population of all the excited Rydberg states and the evolution of the initial state, imitating at least qualitatively the results of the numerical model in certain time and intensity scales.