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Physical Review Letters

Linear Stark Effect for a Sulfur Atom in Strong High-Frequency Laser Fields

Pananghat Balanarayan, Nimrod Moiseyev

Published Jun 18, 2013• 8 citations
Publisher

Abstract

Current trends in laser technology have reached the regime of studying atoms stabilized against ionization, going beyond the perturbation theory. In this work, properties of a laser-dressed sulfur atom are examined in this stabilization regime. The electronic structure of a sulfur atom changes dramatically as it interacts with strong high-frequency laser fields. Degenerate molecularlike states are obtained for the ground state triplet of the laser-dressed sulfur atom for high-frequency and moderate intensity laser parameters. The degenerate ground state is obtained for a laser intensity which is smaller by more than one order of magnitude than the intensity required for hydrogen atoms due to many electron screening effects. An infinitesimally weak static field mixes these degenerate states to give rise to asymmetric states with large permanent dipole moments. Hence, a strong linear Stark effect rather than the usual quadratic one is obtained.

DOI
10.1103/physrevlett.110.253001

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Current trends in laser technology have reached the regime of studying atoms stabilized against ionization, going beyond the perturbation theory. In this work, properties of a laser-dressed sulfur atom are examined in this stabilization regime. The electronic structure of a sulfur atom changes dramatically as it interacts with strong high-frequency laser fields. Degenerate molecularlike states are obtained for the ground state triplet of the laser-dressed sulfur atom for high-frequency and moderate intensity laser parameters. The degenerate ground state is obtained for a laser intensity which is smaller by more than one order of magnitude than the intensity required for hydrogen atoms due to many electron screening effects. An infinitesimally weak static field mixes these degenerate states to give rise to asymmetric states with large permanent dipole moments. Hence, a strong linear Stark effect rather than the usual quadratic one is obtained.
Bound quantum states such as atoms can be torn apart by strong oscillating fields. A natural expectation is that stronger fields lead to more certain destruction. In contradiction to this intuition, some theories predict a striking reversal: that as the field intensity is raised above some threshold, bound state wavefunctions can spatially bifurcate and become increasingly stable with increasing field intensity. This ``strong field stabilization'' was predicted decades ago in the context of atoms in pulsed laser fields, but has resisted experimental observation due to extreme laser intensity requirements and theoretical controversy. We report the experimental observation of strong-field stabilization of a ground state, using trapped neutral atoms to emulate the dynamics of atomic electrons in an extremely strong laser field. We directly image the predicted wavepacket bifurcation, measure an ionization rate non-monotonic in field amplitude, and map out the regime of stabilization as a function of laser pulse parameters. We observe that stabilization persists down to surprisingly low drive frequencies, near and below the scale of the lowest-energy excitations of the bound state. These results confirm and extend a long-standing prediction of extreme quantum dynamics, and showcase a complementary tool for probing strong-field phenomena near and beyond the frontier of current laser technology.
The Electric Stark effect of a Kramers-Henneberger (KH) state of hydrogen atoms in both linearly and circularly polarized laser fields is studied. For the ground KH state of H atoms with a small quiver amplitude, the quadratic Stark effect is observed. For a large quiver amplitude, the Stark effect is quadratic only in a weak electric field and quickly changes to linear as the electric field increases. The atomic structure of the KH state is very sensitive to the electric field and can be easily polarized. The huge polarizability and induced dipole moment are comparable to those of Rydberg atoms.
Resonant photoionization in the intense high-frequency regime can exhibit extremely asymmetric Autler-Townes doublets whose origin remains debated. It has been attributed either to interference between perturbative ionization pathways or to a nonperturbative dressing of the continuum. Here, we show that these interpretations arise from a common effective Hamiltonian framework, in which dressed-state stabilization is governed by the coherent interplay of resonant and nonresonant pathways. We demonstrate that further simplification, using the strong-field approximation, obscures this mechanism. In contrast, our time-dependent essential-state model, where electrons are rigorously coupled to the continuum, achieves excellent agreement with simulations of the time-dependent Schrödinger equation for helium.
Abstract The spontaneous emission of a quantum system driven by a high-intensity, high-frequency classical laser field is analyzed. The study is based on the accurate consideration of the quantum system interacting with vacuum-quantized field modes in the first order of perturbation theory, while the intense laser field is considered classically beyond this theory. It is demonstrated that the spectrum of the spontaneous emission can be used for analyzing the strong-field dynamics and the structure of the energy spectrum of an atomic system. In particular, it is found that in high-frequency fields (where the energy of the laser quanta is greater than the ionization potential) atoms manifest the features of the Kramers–Henneberger atom. It is also found that in the stabilization regime, the atom emits both odd and even laser radiation harmonics.
A formulation of quantum electrodynamics is given that applies to atoms in a strong laser field by perturbation theory in a non-relativistic regime. Dipole approximation is assumed. The dual Dyson series, here discussed by referring it to the Birkhoff theorem for singularly perturbed linear differential equations, can be applied and a perturbation series obtained transforming the Hamiltonian by a Pauli-Fierz transformation. But, if just few photons are present high-order harmonics cannot be generated. So, it is proven that odd high-order harmonics only appear when the laser field is intense and one can substitute the creation and annihilation operators by the square root of the mean number of photons taken to be huge, the field retaining its coherency property as observed experimentally for harmonics. In this case, the Hamiltonian for perturbation theory comes to the Kramers-Henneberger form. The theory has a dipolar contribution when the free-electron quiver motion amplitude is larger than the atomic radius. For a Coulomb potential one has that the outer electron is periodically kicked, and so a prove is given that the same should happen to Rydberg atoms in intense microwave fields. The distribution representing the kicking has a Fourier series with just odd terms. Using a modified Rayleigh-Schrödinger perturbation theory, it is shown that under the same condition of validity of the quiver motion amplitude to atomic radius ratio, the atomic wave function is only slightly modified by the laser field due to the way the energy levels rearrange themselves. This gives a prove of stabilization in the limit of laser frequency going to infinity. Then, perturbation theory can be applied when the Keldysh parameter becomes smaller with respect to the shifted distance between the energy levels of the atom.