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Physical Review Letters

Creating and Probing Electronic Wave Packets Using Half-Cycle Pulses

R. R. Jones

Published May 20, 1996• 121 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.76.3927

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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.
Summary form only given. Unipolar half-cycle pulses (HCPs) can be used to alter the momentum distribution of atomic electrons over subpicosecond timescales. Previously, momentum kicks from HCPs were used to produce electronic wave packets from highly excited Rydberg eigenstates. In addition, these pulses have been used to kick bound electrons into the continuum, making it possible to monitor the time-dependent momentum distribution of electronic wave packets. Conversely, our most recent experiments have shown that HCPs can extract momentum from free electrons, facilitating their capture by positive ions. In the experiments, calcium atoms in the singlet 4s4p level are photoionized into the continuum using a 1.5ps, 390-nm laser pulse.
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.
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.
Localized wavepackets are created in high- n ( n ~ 300) Rydberg atoms which travel in near-circular orbits around the nucleus. Application of carefully tailored electric fields to quasi-1D Rydberg atoms creates coherent superpositions of Stark states with near extreme values of one of the components of the angular momentum. Half-cycle electric field pulses (HCPs) probe the dynamics of the circular states producing signature oscillations in survival probability that correspond to the expected wavepacket evolution. Although these wavepackets slowly dephase and lose their localization, their motion can be followed for several orbits and provides an analog of the original Bohr model, i.e., an electron in circular classical orbit around the nucleus. Measurements of the asymmetry in survival probability with increasing probe strength at different phases of the orbit confirm orbital motion of the wavepacket. Classical trajectory Monte-Carlo simulations (CTMC) agree with experimental results, and provide promising leads for future studies.
Recent advances in the study of Rydberg atoms have focused on the control, manipulation and detection of Rydberg wave packets using novel external fields such as half-cycle pulses. The radial degree of freedom has been controlled and used to process information encoded in Rydberg states. However, these previous experiments make use of only a single degree of freedom, restricting the potential of other degrees of freedom for quantum computing in Rydberg atoms. In this dissertation, we explore the control and detection of other degrees of freedom in an electron wave packet, such as the angular momentum quantum number ℓ, the magnetic quantum number m and the electron spin; so that the full range of quantum numbers can participate in information processing. We first propose an interferometric control of the population of angular momentum states using two time-delayed phase-locked ultrafast laser pulses. The population of arbitrary angular momentum states can be greatly enhanced by optimizing the time delay and the relative phases between two laser pulses. We then qualitatively measure the evolution of angular momentum components in Stark wave packets by a weak half-cycle pulse (HCP). This measurement utilizes a time-delayed HCP and is proved to be effective for detecting various aspects of wave packet dynamics, particularly, the evolution of non-stationary states. The technique relies on the fact that the HCP redistributes the eigenstate populations and induced the population variation which reflects the evolution of eigenstate phases. Finally, we find that the dynamics of m-states could be highly correlated with the internal degree of freedom of the electron, the spin. We study the effect of spin-orbit coupling on the wave packet dynamics and observe the angular precession of a Rydberg wave packet. The population redistribution from p to s states is highly sensitive to the polarization of the HCP and changes with the precession of the electron orbit. We obtain the selection rules and give an intuitive classical interpretation of angular momentum redistribution by an HCP. In short, new dynamics involving multiple degrees of freedom of an electron wave packet are discovered, observed and understood.
Summary form only given. Optical pulse shaping and wave-packet holography have been used to store information in the phase of an atomic Rydberg wave-packet. We present a new method of retrieving this phase information by using a terahertz domain half-cycle pulse (HCP) to coherently redistribute the Rydberg population. We use programmed optical pulses to create radial wave-packets in a beam of atomic Cs centered at n = 26p with one state phase-reversed from the others. An impulse model for this atom-HCP interaction is employed to qualitatively explain this flipped-state amplification.