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Physical Review Letters

Creating and Detecting Shaped Rydberg Wave Packets

Jeffrey L. Krause, Kenneth J. Schäfer, M. Ben-Nun, Kent R. Wilson

Published Dec 22, 1997• 50 citations
Publisher

Abstract

Inherently quantum mechanical, transient nanostructures with dynamics on a picosecond time scale can be produced by controlling the quantum dynamics of Rydberg electrons. Ultrashort, tailored light pulses are used to build structures in position and/or momentum space from the wave function of an electron. The optimal laser pulses required to make these structures can be computed and synthesized in the laboratory. As an example, we present a structure consisting of five peaks which acts as a time-dependent grating and can be detected via ultrafast extreme ultraviolet diffraction.

DOI
10.1103/physrevlett.79.4978

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Inherently quantum mechanical, transient nanostructures with dynamics on a picosecond time scale can be produced by controlling the quantum dynamics of Rydberg electrons. Ultrashort, tailored light pulses are used to build structures in position and/or momentum space from the wave function of an electron. The optimal laser pulses required to make these structures can be computed and synthesized in the laboratory. As an example, we present a structure consisting of five peaks which acts as a time-dependent grating and can be detected via ultrafast extreme ultraviolet diffraction.
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.
Quantum excitation is usually regarded as a transient process occurring instantaneously, leaving the underlying physics shrouded in mystery. Recent research shows that Rydberg-state excitation with ultrashort laser pulses can be investigated and manipulated with state-of-the-art few-cycle pulses. We theoretically find that the efficiency of Rydberg state excitation can be enhanced with a short laser pulse and modulated by varying the laser intensities. We also uncover new facets of the excitation dynamics, including the launching of an electron wave packet through strong-field ionization, the re-entry of the electron into the atomic potential and the crucial step where the electron makes a U-turn, resulting in twin captures into Rydberg orbitals. By tuning the laser intensity, we show that the excitation of the Rydberg state can be coherently controlled on a sub-optical-cycle timescale. Our work paves the way toward ultrafast control and coherent manipulation of Rydberg states, thus benefiting Rydberg-state-based quantum technology.
Summary form only given. Many realized or potential applications of optically driven ultrafast quantum dynamics require specially shaped quantum states, with the ability to detect these shapes and modify them using active feedback. We have developed methods to sculpt wave packets using shaped ultrafast optical pulses. We can also view these wave packets using quantum interference methods that have been adapted from holographic techniques used to characterize classical light. These quantum state holograms have been used as feedback to sculpt specific target shapes.
Using techniques of ultrafast coherent control, we propose a method to produce high-purity high-l\mathcal{l}l (angular momentum) states in Rydberg Stark wave packets. Two time-delayed phase-locked laser pulses excite the atom from a low-lying ``launch state'' into a low-l\mathcal{l}l Rydberg wave packet, in the presence of a static electric field. By choosing the time delays between the pulses, and the static electric field, we find that a high-l\mathcal{l}l state with high purity can be created at the target time.
High angular momentum Rydberg wave packets are studied. Application of carefully tailored electric fields to low angular momentum, high- n ( n ∼ 300) Rydberg atoms creates coherent superpositions of Stark states with near extreme values of angular momentum, [cursive l]. Wave packet components orbit the parent nucleus at rates that depend on their energy, leading to periods of localization and delocalization as the components come into and go out of phase with each other. Monitoring survival probability signals in the presence of position dependent probing leads to observation of characteristic oscillations based on the composition of the wave packet. The discrete nature of electron energy levels is observed through the measurement of quantum revivals in the wave packet localization signal. Time-domain spectroscopy of these signals allows determination of both the population and phase of individual superposition components. Precise manipulation of wave packets is achieved through further application of pulsed electric fields. Decoherence effects due to background gas collisions and electrical noise are also detailed. Quantized classical trajectory Monte-Carlo simulations are introduced and agree remarkably well with experimental results.