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.
Neutral Rydberg state excitation in strong UV laser fields of Xe atoms has been studied and compared with direct ionization. The yields of both strong-field excitation and ionization have been measured as a function of UV laser intensity and ellipticity. The underlying physical mechanism has been discussed based on the experimental results, indicating that the Rydberg states are populated via multi-photon resonance excitation in strong 400 nm laser fields. Finally, a comparative study of Xe and
O2 with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.
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 and
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 generally behaves similarly to Ar, while that of
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 at low intensity and the oscillation behavior of the ratio between
N2 and Ar, indicating that our understanding of the relevant physics is still far from complete.
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.
In this work, we have experimentally and theoretically investigated the high-lying Rydberg state excitation for noble gas atoms subject to an intense near-infrared laser field. To obtain the signal of these high-lying Rydberg atoms which are further ionized by a constant electric field
(Fc), coincident detection of the photoelectrons and photoions with well-chosen arrival times is performed. Based on a fitting to the time dependence of the coincidently measured photofragment yields with a semiempirical formula, we can extract a principal quantum number distribution (PQND) of the population of the excited states in a range closely related to the strength of
Fc. The extracted valid PQND is in qualitative agreement with a semiclassical model calculation. Our work thus provides a method to extract the PQND and study the ultrafast high-lying Rydberg state excitation.
Abstract We investigate the influence of singlet and triplet spin states on rescattered photoelectrons in strong-field ionization of excited helium. Choosing either a symmetric or antisymmetric spatial wave function as the initial state results in different scattering cross sections for the 1 s 2 s 1 S and 3 S states. These cross sections are used in the semi-classical model of strong-field ionization. Our investigations show that the photoelectron momentum distributions of rescattered electrons exhibit a significant dependence on the relative spin state of the projectile and the bound electron which should be observable in experiments. The proposed experimental approach can be understood as a testbed for probing the spin dynamics of electrons during strong-field ionization and the presented results as a baseline for their identification.