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High Angular Momentum Rydberg Wave Packets

B. Wyker

Published Dec 1, 2011• 0 citations
OpenAlex

Abstract

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.

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•Jan 1, 2006•0 citations
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.
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.
Quantum revivals in very-high-n (n ~ 300) high-l Rydberg wave packets generated from parent np states are used to examine decoherence induced by the application of 'coloured' noise from a random pulse generator and by collisions. In the absence of external perturbations, the high-l wave packets maintain their coherence for periods ~ 1 µs, i.e. for many hundreds of orbits. This coherence can be destroyed on sub-microsecond timescales by the application of even very small amounts of electrical noise at a rate that depends markedly on the spectral characteristics of the noise. In contrast, measurements over similar timescales with CO2 target gas densities of ~ 1011 cm−3 provided no evidence of collisional dephasing. The mechanisms responsible for decoherence are discussed with the aid of classical and quantum simulations. The results of these simulations are in good accord with the experimental data.
In this paper, a coherent superposition of angular-momentum states created by absorption of polarized light by molecules is analyzed. Attention is paid to the time evolution of wave packets representing the spatial orientation of the internuclear axis of a diatomic molecule. Two examples are considered in detail. Molecules absorbing light in a permanent magnetic field experiencing the Zeeman effect and molecules absorbing light in a permanent electric field experiencing the quadratic Stark effect. In a magnetic field, we have a wave packet that evolves in time exactly as a classical dipole oscillator in a permanent magnetic field (classical-physics picture of the Zeeman effect). In the second case, we have a wave packet that goes through periodical changes of shape of the packet with revivals of the initial shape. This is pure quantum behavior. The classical motion of angular momentum in an electric field in the case of a quadratic Stark effect is known to be a periodic. Solutions obtained for wave packet evolution are briefly compared with Rydberg-state coherent wave packets and harmonic-oscillator wave packets. Zeeman and Stark effects in small molecules continuously attract the attention of researchers, theoreticians, as well as experimentalists. These investigations allow us to obtain a deeper understanding of the interaction of molecules with stationary external fields and also can be used as a practical tool to measure different molecular characteristics, such as permanent electric or magnetic dipole moments, intramolecular perturbations, etc. It is worthwhile analyzing these effects as an evolution of wave packets. All this motivates a comparison of the quantum and classical picture of Zeeman and Stark effects in molecules.PACS No.: 33.55.Be
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.
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.