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Journal of Physics B Atomic Molecular and Optical Physics

Steering neutral atoms in strong laser fields

Sebastian Eilzer, U. Eichmann

Published Oct 8, 2014• 28 citations
Publisher

Abstract

The seminal strong-field tunnelling theory introduced by L V Keldysh plays a pivotal role. It has shaped our understanding of atomic strong-field processes, where it represents the first step in complex ionisation dynamics and provides reliable tunnelling rates. Tunnelling rates, however, cannot be necessarily equated with ionisation rates. Taking into account the electron dynamics in the Coulomb potential following the tunnelling process, the process of frustrated tunnelling ionisation has been found to lead to excited Rydberg atoms. Here, we excite He atoms in the strong-field tunnelling regime into Rydberg states. A high percentage of these Rydberg atoms survive in high intensity laser fields. We exploit this fact together with their high polarisability to kinematically manipulate the Rydberg atoms with a second elliptically polarised focused strong laser field. By varying the spatial overlap of the two laser foci, we are able to selectively control the deflection of the Rydberg atoms. The results of semi-classical calculations, which are based on the frustrated tunnelling model and on the ponderomotive acceleration, are in accord with our experimental data.

DOI
10.1088/0953-4075/47/20/204014

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The seminal strong-field tunnelling theory introduced by L V Keldysh plays a pivotal role. It has shaped our understanding of atomic strong-field processes, where it represents the first step in complex ionisation dynamics and provides reliable tunnelling rates. Tunnelling rates, however, cannot be necessarily equated with ionisation rates. Taking into account the electron dynamics in the Coulomb potential following the tunnelling process, the process of frustrated tunnelling ionisation has been found to lead to excited Rydberg atoms. Here, we excite He atoms in the strong-field tunnelling regime into Rydberg states. A high percentage of these Rydberg atoms survive in high intensity laser fields. We exploit this fact together with their high polarisability to kinematically manipulate the Rydberg atoms with a second elliptically polarised focused strong laser field. By varying the spatial overlap of the two laser foci, we are able to selectively control the deflection of the Rydberg atoms. The results of semi-classical calculations, which are based on the frustrated tunnelling model and on the ponderomotive acceleration, are in accord with our experimental data.
Using field ionization combined with the direct detection of excited neutral atoms we measured the distribution of principal quantum number n of excited He Rydberg states after strong-field excitation at laser intensities well in the tunneling regime. Our results confirm theoretical predictions from semiclassical and quantum mechanical calculations and simultaneously underpin the validity of the semiclassical frustrated tunneling ionization model. Moreover, since our experimental detection scheme is spin sensitive in the case of He atoms, we show that strong-field excitation leads to strong population of triplet states. The origin of it lies in the fact that high angular momentum states are accessible in strong-field excitation. Thus, singlet-triplet transitions become possible due to the increased importance of spin-orbit interaction rather than due to direct laser induced spin-flip processes.
The authors have studied phenomena related to the ionisation of indium Rydberg atoms by an external electric field. The indium atoms are excited in an atomic beam apparatus by pulsed dye laser light. The high-lying states are populated in one step from the ground state by an ultraviolet, frequency-doubled dye laser or by stepwise excitation using two dye lasers in the visible region. Shortly after the excitation, an electric field is applied in the interaction region which causes ionisation of the highly excited atoms. The authors have investigated (i) the lowest adiabatic ionisation threshold over a wide range of n values and compared the results with model predictions, (ii) the structure in the adiabatic part of the ionisation spectrum, and (iii) the transition from adiabatic to diabatic ionisation as a function of the slew rate of the ionising field pulse and the quantum defect and quantum numbers of the atomic state concerned. The ionisation signal is demonstrated to shift considerably towards higher field strengths with increasing slew rate. A qualitative explanation is presented and consequences for the detection efficiency are mentioned. Differences in the field ionisation behaviour between nearly degenerate excited states are demonstrated and exploited to achieve selective detection of fine-structure and even hyperfine-structure states.
We study a hitherto unexplored regime of the Rydberg excitation blockade using highly Stark-shifted, yet long-living, states of Rb atoms subject to electric fields above the classical ionization limit. Such states allow tuning the dipole-dipole interaction strength while their ionization rate can be changed over 2 orders of magnitude by small variations of the electric field. We demonstrate laser excitation of the interacting Rydberg states followed by their detection using controlled ionization and magnified imaging with high spatial and temporal resolution. Our work reveals new possibilities to engineer the interaction strength and dynamically control the ionization and detection of Rydberg atoms, which can be useful for realizing and assessing quantum simulators that vary in space and time.
Rather than being freed to the continuum, the strong-field tunneled electrons can make a trajectory driven by the remaining laser fields and have certain probability to be captured by the high lying Rydberg states of the parent atoms or molecules. To explore the effect of molecular orbital on Rydberg state excitation, the ellipticity dependence of Rydberg state yields of N2 and O2 molecules are experimentally investigated using cold target recoil ion momentum spectroscopy and are compared with their counterpart atoms Ar and Xe with comparable ionization potentials. We found the generation probability of the neutral Rydberg fragment O2* was orders of magnitude higher than that of Xe* due to the butterfly-shaped highest occupied molecular orbital of O2. Meanwhile, our experimental and simulation results reveal that it is the initial momentum distribution (determined by the detailed characteristics of orbitals) that finally leads to the tendency that the Rydberg state yield of O2 (Ar) decreased slower than that obtained for Xe (N2) when the ellipticity of the excitation laser field is increased.
Rydberg-state excitation of atoms in strong infrared laser fields provides a new complementary aspect of the perspective of atom--strong field interactions. In this article, we perform an experimental and theoretical study on the corresponding process of diatomic molecules, N2{\mathrm{N}}_{2}N2​ and O2{\mathrm{O}}_{2}O2​. We show that neutral molecules can also survive strong 800-nm laser fields in high Rydberg states, while their behavior is remarkably different in comparison with their companion atoms, Ar and Xe. The Rydberg excitation of N2{\mathrm{N}}_{2}N2​ generally behaves similarly to Ar, while that of O2{\mathrm{O}}_{2}O2​ is more significantly suppressed than the ionization compared to Xe in a high intensity region, which can be understood in the frame of a semiclassical picture, together with their different structures of molecular orbitals. However, distinct quantum features in the Rydberg excitation processes that are apparently beyond the semiclassical picture have been identified, i.e., the less suppressed probability of O2{\mathrm{O}}_{2}O2​ at low intensity and the oscillation behavior of the ratio between N2{\mathrm{N}}_{2}N2​ and Ar, indicating that our understanding of the relevant physics is still far from complete.
Substantial neutral atoms can tunnel to excited states in an intense laser field and subsequently generate coherent emission through free induction decay. We experimentally observe an enhanced coherent emission in the harmonic slightly below the threshold, which is consistent with the free induction decay of Rydberg states produced by the frustrated tunnelling ionization (FTI) process. We further find that the intensity of the coherent emission significantly depends on the chirp of laser pulses. The simulations based on the strong field approximation model show that laser chirp affects the probability that the returned electrons recombine to the Rydberg states. Our result shows that coherent emission can be controlled by laser chirp, which facilitates understanding the dynamics of the Rydberg atom and coupling mechanism between the below-threshold harmonics and atomic energy level. In addition, the coherent below-threshold FTI emission we observed has small divergence which is good for EUV light source applications.