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Physical Review A

Creating high-purity angular-momentum-state Rydberg atoms by a pair of unipolar laser pulses

Peipei Xin, Hong Cheng, Shanshan Zhang, Han-Mu Wang, Zi-Shan Xu, Hongping Liu

Published Apr 23, 2018• 1 citation

Abstract

We propose a method of producing high-purity angular-momentum-state Rydberg atoms by a pair of unipolar laser pulses. The first positive-polarity optical half-cycle pulse is used to prepare an excited-state wave packet while the second one is less intense, but with opposite polarity and time delayed, and is employed to drag back the escaping free electron and clip the shape of the bound Rydberg wave packet, selectively increasing or decreasing a fraction of the angular-momentum components. An intelligent choice of laser parameters such as phase and amplitude helps us to control the orbital-angular-momentum composition of an electron wave packet with more facility; thus, a specified angular-momentum state with high purity can be achieved. This scheme of producing high-purity angular-momentum-state Rydberg atoms has significant application in quantum-information processing.

DOI: 10.1103/physreva.97.043425

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We propose a method of producing high-purity angular-momentum-state Rydberg atoms by a pair of unipolar laser pulses. The first positive-polarity optical half-cycle pulse is used to prepare an excited-state wave packet while the second one is less intense, but with opposite polarity and time delayed, and is employed to drag back the escaping free electron and clip the shape of the bound Rydberg wave packet, selectively increasing or decreasing a fraction of the angular-momentum components. An intelligent choice of laser parameters such as phase and amplitude helps us to control the orbital-angular-momentum composition of an electron wave packet with more facility; thus, a specified angular-momentum state with high purity can be achieved. This scheme of producing high-purity angular-momentum-state Rydberg atoms has significant application in quantum-information processing.

Using techniques of ultrafast coherent control, we propose a method to produce high-purity high-

\mathcal{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-

\mathcal{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-

\mathcal{l}

state with high purity can be created at the target time.

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.

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.

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.

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 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.