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Physical Review A

Decay of oriented Rydberg wave packets excited with far-infrared radiation

G. M. Lankhuijzen, Marcel Drabbels, F. Robicheaux, Lambertus D. Noordam

Published Jan 1, 1998• 10 citations
Publisher

Abstract

Transitions from bound atomic Rydberg Stark states in a static electric field to autoionizing Rydberg states above the electric-field-induced ionization threshold are studied using a broadband, tunable free-electron laser (photon energy 160--1400 ${\mathrm{cm}}^{\ensuremath{-}1}$, pulse duration $\ensuremath{\sim}1$ ps) and compared with multichannel quantum defect theory calculations. An atomic streak camera is used to record the time-resolved electron emission transients of the autoionizing atoms. For Stark states located on the downfield side of the potential, the far-infrared ionization spectrum is found to be smooth and the electron emission prompt $(<2$ ps), whereas for Stark states located on the upfield side, the far-infrared spectrum has sharp resonances, and the lifetime of the quasicontinuum states is considerably longer. The electron-emission transients from optical ionization of ground-state atoms are compared to transients from far-infrared ionization of Rydberg atoms, showing that the angular motion of the wave packet is responsible for the ionization dynamics for both cases, but different coherent superpositions of angular momentum states are excited depending on the initial state. Finally, we discuss the feasability of using Rydberg atoms as an ultrafast far-infrared detector, starting from a downfield state, or as a wavelength-selective detector, starting from an upfield state.

DOI
10.1103/physreva.57.440

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Physical Review A•Apr 13, 2015•18 citations
Transitions from bound atomic Rydberg Stark states in a static electric field to autoionizing Rydberg states above the electric-field-induced ionization threshold are studied using a broadband, tunable free-electron laser (photon energy 160--1400 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1, pulse duration \ensuremath∼1\ensuremath{\sim}1\ensuremath∼1 ps) and compared with multichannel quantum defect theory calculations. An atomic streak camera is used to record the time-resolved electron emission transients of the autoionizing atoms. For Stark states located on the downfield side of the potential, the far-infrared ionization spectrum is found to be smooth and the electron emission prompt (<2(<2(<2 ps), whereas for Stark states located on the upfield side, the far-infrared spectrum has sharp resonances, and the lifetime of the quasicontinuum states is considerably longer. The electron-emission transients from optical ionization of ground-state atoms are compared to transients from far-infrared ionization of Rydberg atoms, showing that the angular motion of the wave packet is responsible for the ionization dynamics for both cases, but different coherent superpositions of angular momentum states are excited depending on the initial state. Finally, we discuss the feasability of using Rydberg atoms as an ultrafast far-infrared detector, starting from a downfield state, or as a wavelength-selective detector, starting from an upfield state.
The short-pulse dynamics of excitation and stimulated emission between highly excited states (15<n<60)(15<n<60)(15<n<60) is studied with picosecond far-infrared pulses (40--60 $\ensuremath{\mu}\mathrm{m}$) originating from a free electron laser. We measured the excitation of a Rydberg wave packet in rubidium around n=40n=40n=40 excited from a deeper bound $(n\ensuremath{\approx}20)$ Rydberg state by a picosecond far-infrared laser pulse. Moreover, starting from a stationary n=40n=40n=40 state we found that upon irradiating with a short far-infrared laser pulse, adjacent Rydberg states are populated by resonant Raman transfer via a deeper (n=20)(n=20)(n=20) bound state. Finally, we discuss the dynamics of wave-packet excitation at a Cooper minimum in lithium, where sign change of the excitation matrix elements causes excitation at large distances from the atomic core. Possible measurement methods for this effect are discussed and found to yield different information.
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.
Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.
The Stark spectra of autoionizing Rydberg states of Xe converging to the second ionization limit 5p5{p}^{5}p5 2P1/2^{2}P_{1/2}2P1/2​ have been investigated as a function of applied electric field over the range 26--2362 V/cm. Single-photon excitation from the Xe ground state was achieved using coherent radiation near 92.5 nm, generated by frequency tripling the pulsed output of a frequency-doubled dye laser in a free jet of rare-gas atoms. For the lowest electric field only the ns' and nd' series were observed. As the electric field was increased the np' series appeared because of the mixing of wave functions with different l values. Further increase of the electric field caused the appearance of hydrogenlike Stark manifolds. The Stark spectrum was simulated in a two-step procedure with no adjustable parameters. Using a jl-coupling basis set the Hamiltonian matrix was diagonalized to determine the energy levels and corresponding eigenfunctions for a given electric field strength. The intensities and line shapes were then calculated using the formalism developed by Fano for a many-discrete-level--single-continuum configuration interaction. This treatment was sufficient to reproduce the positions, widths, and shapes of most observed features. At field strengths between 1000 and 2000 V/cm, however, an additional modulation structure with a spacing of about 2.7 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ appeared on top of the \ensuremath{\Vert}M\ensuremath{\Vert}=1 autoionizing resonances, which could not be explained by our simple theoretical model.
We have studied ionization and excitation of Rydberg atoms by intense sub‐picosecond electromagnetic field pulses of less than one cycle duration. The ionization threshold electric field scales as the binding energy (i.e., n*−2, rather than the n*−4 threshold scaling characteristic of static field ionization and high order multiphoton ionization. This altered behavior is due to the short duration and the subcycle nature of the field. We also find a wide distribution of final states produced by these pulses, which are effectively ‘‘in resonance’’ for dozens of transitions simultaneously.
We study the ionization of Rydberg atoms in a single-cycle-pulse electric field based on both classical and quantum calculations. The ionization-probability curve exhibits a ``ripple'' structure as a function of the pulse duration and the field amplitude. These ripple structures are found to be dependent on the angular distribution of the initial state. A large electron-emission asymmetry is observed, and the ionized electron is almost completely emitted to one side of the atom except when the pulse length is roughly one Rydberg period. In both the long-pulse and the short-pulse regimes, larger electron energy can be expected from the ionization of lower-lying Rydberg states, matching the observation in a recent experiment [S. Li and R. R. Jones, Phys. Rev. Lett. 112, 143006 (2014)]. This trend is closely related to the electron-emission asymmetry associated with the field-direction change in a single-cycle pulse. The possible implications of the different energy transfer in a single-cycle pulse from that in a multicycle pulse are also discussed briefly for the strong-field ionization of the ground atomic state.