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Exploring multiple degrees of freedom in Rydberg wave packets.

Haidan Wen

Published Jan 1, 2006• 0 citations
OpenAlex

Abstract

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.

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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.
The creation and detection of specific angular momentum states in Rydberg atoms is a significant advance in quantum-information processing. Detection of high angular momentum states in alkali-metal atoms is difficult because they are nearly-degenerate in energy. We present theoretical results on the detection of such states using terahertz-frequency half-cycle pulses (HCPs). Calculations are done for n=15,=0,...,14 states in hydrogen and cesium using a grid-based pseudopotential method. Our results indicate that HCP redistribution is a reliable method of distinguishing angular momentum Rydberg states.
The creation and detection of specific angular momentum states in Rydberg atoms is a significant advance in quantum-information processing. Detection of high angular momentum states in alkali-metal atoms is difficult because they are nearly-degenerate in energy. We present theoretical results on the detection of such states using terahertz-frequency half-cycle pulses (HCPs). Calculations are done for $n=15,\ensuremath{\ell}=0,\dots{},14$ states in hydrogen and cesium using a grid-based pseudopotential method. Our results indicate that HCP redistribution is a reliable method of distinguishing angular momentum Rydberg states.
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.
The field of coherent control has today been seeing significant progress, in a wide array of physical systems. One such system is the Rydberg atom. The long lifetime, strong dipole interactions, multiple degrees of freedom, and simple atomic structure make Rydberg atoms particularly appealing for experiments involving coherent control. The same properties have led to the exploration of Rydberg atoms as candidates for quantum information storage, processing and retrieval. Quantum information processing is a particular application of coherent control. Rather than being disparate subjects of study, coherent control of Rydberg atoms and processing of information stored as phase in different Rydberg levels are two sides of the same coin. In this dissertation, we experimentally characterize the effect of a half-cycle pulse on the phases of the states of a Rydberg wave packet and their mutual coherence. This has bearing both on our ability to control the states of the atom and on our ability to measure the information stored as quantum phase. We observe delay dependent phase shifts and losses of coherence. Despite a loss of information due to transfer of quantum amplitude to states outside the data register, we demonstrate partial retrieval of that information by the application of a second half cycle pulse. We also present an essential states model of the interaction, and we compare results from the model to experimental features observed. Although the particulars may vary, the concepts involved are quite general and may be applied to multilevel systems other than Rydberg atoms.
An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.
We study the dynamics of highly excited (Rydberg) atoms in laboratory-scale magnetic fields via their ionization by THz half-cycle pulses (HCPs). A half-cycle pulse is a unipolar electromagnetic pulse that can probe an atomic electron at all points along its orbit around the atomic core. The dynamical evolution of diamagnetic Zeeman states subjected to an ultrashort (picosecond) HCP is calculated for both hydrogen and sodium atoms. Diamagnetic Zeeman states are localized parallel and perpendicular to the magnetic field. We use a grid-based pseudo-potential method to determine these eigenstates of the combined Coulomb-diamagnetic potential. We study states with principal quantum number n between 15--30 in the ℓ-mixing regime at magnetic fields of 1--6T. These initial states are subjected to the electric field of an HCP and their subsequent time evolution is calculated by solving the time-dependent Schrodinger equation. The HCP width is varied between the short pulse (impulsive) and the long pulse limit, keeping the total momentum transferred a constant. We calculate the total ionized fraction, and also the spectrum of the ionized photoelectrons. We find that, in the impulsive limit, where the width of the pulse is much smaller than typical time scales in the system, the calculated amount of ionization and the photoelectron spectra are different depending on the localization of the initial state. These differences are shown to be due to the different initial momentum distributions of the parallel and perpendicular states. As the duration of the HCP is made longer, we find that ionization is suppressed as compared with the impulsive limit. The states localized perpendicular to the magnetic field are found to be much more sensitive to the HCP width than the parallel states, reflecting the fact that the two classes of states interact with different parts of the Coulomb-diamagnetic potential during the HCP. The ionization characteristics are shown to scale classically with the principal quantum number. The results are presented in such a manner that they can be verified by experiment.