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Bulletin of the American Physical Society

Time evolution of Rydberg states as a function of the Rydberg-parent atom relative velocity

Enrique J. Galvez, John R. Lewis, F. DeZela

Published May 1, 1993• 0 citations
OpenAlex

Abstract

Using state-resolved field ionization we have studied the time evolution of sodium Rydberg states, in a thermal atomic beams initially excited to 28s. The velocities of the detected Rydberg atoms were selected using the time-of-flight technique. With this selection we were able to study the time evolution of atoms with average velocities v{sub r} different from v{sub b}, the average velocity of the ground state atoms of the beam. We observe that for v{sub r}{approximately}v{sub b} the time evolution is dominated by blackbody radiation induced transitions to neighboring levels. However, as v{sub r}>>v{sub b} collisional transfers become important. For v{sub r}>>v{sub b} the time evolution is dominated by collisional transfer. The data shows evidence of both n{sup -} and l{sup -} changing collisions. We will compare a modeled theory with the data.

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Journal of Physics B Atomic Molecular and Optical Physics•May 26, 2005•34 citations
Using state-resolved field ionization we have studied the time evolution of sodium Rydberg states, in a thermal atomic beams initially excited to 28s. The velocities of the detected Rydberg atoms were selected using the time-of-flight technique. With this selection we were able to study the time evolution of atoms with average velocities v{sub r} different from v{sub b}, the average velocity of the ground state atoms of the beam. We observe that for v{sub r}{approximately}v{sub b} the time evolution is dominated by blackbody radiation induced transitions to neighboring levels. However, as v{sub r}>>v{sub b} collisional transfers become important. For v{sub r}>>v{sub b} the time evolution is dominated by collisional transfer. The data shows evidence of both n{sup -} and l{sup -} changing collisions. We will compare a modeled theory with the data.
Collisional and thermal ionization of sodium n S and n D Rydberg atoms with n = 8–20 has been studied. The experiments were performed using a two-step pulsed laser excitation in an effusive atomic beam at atom density of about 2 × 10 10 cm −3 . Molecular and atomic ions from associative, Penning and thermal ionization processes were detected. It was found that the atomic ions were created mainly due to photoionization of Rydberg atoms by photons of blackbody radiation at the ambient temperature of 300 K. Blackbody ionization rates and effective lifetimes of Rydberg states of interest were determined. The molecular ions were found to be from associative ionization in Na( nL ) + Na(3S) collisions. Rate constants of associative ionization have been measured using an original method based on relative measurements of Na + 2 and Na + ion signals.
We have observed the evolution of cold Rydberg gases and ultracold plasmas in an environment that allows for the control of interactions of the blackbody radiation temperature from 4K to 300K. The work in this thesis describes the influence of initial densities, populations, excitation state, evolution time and thermal background temperature on the evolution of cold Rydberg gases as well as directly excited ultracold plasmas. With some initial ionization, cold-Rydberg-atom gases easily develop a positive space charge that traps electrons for times on the order of tens of mus. This acts as a catalyst for electron-Rydberg atom collisions, increasing the collision probabilities by orders of magnitude and profoundly altering the final state of the Rydberg gas. Using state-selective field ionization, we have provided direct proof that these collisions cause changes in l-states, and we have seen the first experimental evidence that they also lead to inelastic n-changing collisions, as predicted by theory. We have also found evidence for Rydberg-Rydberg collisions, enabled by the attractive electric-dipole forces between atoms in high-l states and possibly by van-der-Waal's interactions at very high-n . Thermal interactions are seen to influence the formation of a plasma from a cold Rydberg gas. Plasmas form more easily in the presence of a 300K radiation field than at 4K, due to the contribution of thermal ionization to the plasma formation. The background temperature also appears to affect the electron temperature in both the directly excited plasma and the plasma spontaneously formed from a cold Rydberg gas. In Rydberg atom gases that have undergone partial ionization, electron temperatures were estimated using the dependence of n-changing collisions on the electron temperature.
Thermal collisions between laser excited Xe(nf) Rydberg atoms and a variety of neutral atomic and molecular targets have been investigated. In Xe(nf)-HF collisions, n-changing, 4-changing and collisional ionization were observed. For n = 26 and 27, absolute collisional cross sections for these processes have been determined using time-resolved selective field ionization. In addition, the first evidence of molecular rotational excitation through the transfer of energy of electronic excitation from a Rydberg atom is presented. In Xe(nf) - Xe, Kr, Ar, CO2, CO and N2 collisions the dominant mechanism was observed to be 4-changing: no evidence of n-changing or collisional ionization was apparent. Absolute collisional cross sections have been determined for a range of n between 24 and 37. Comparison of these cross sections with those obtained using a theoretical model in which effects due to the Rydberg core are ignored appears to lead to satisfactory results only for Xe, Kr and CO2, whereas when core effects are included satisfactory agreement between experiment and theory is found in all cases.
A stochastic model of associative ionization in collisions of Rydberg atoms with ground-state atoms is presented. The conventional Duman–Shmatov–Mihajlov–Janev (DSMJ) model treats the ionization as excitation of Rydberg electron to the continuum by the electric-dipole field generated by exchange interaction within the quasi-molecular ion. The stochastic model essentially extends this treatment by taking into account redistribution of population over a range of Rydberg states prior to ionization, which is caused by non-adiabatic processes in overlapping multiple level crossings of quasi-molecular Rydberg states. The redistribution is modelled as diffusion of electrons in the Rydberg energy spectrum using a Fokker–Planck-type equation. The process of l -mixing of Rydberg states at large internuclear distances and twisting of the collision trajectories on attractive potentials are taken into account. The choice of the collision velocity distribution is also shown to be important. Associative ionization rates have been calculated for Na**( nl ) + Na collisions with n = 5–25 and l = 0, 1, 2, and compared with the available experimental data and the calculations performed using the nonlinear DSMJ model. At relatively low n the stochastic model yields a substantially better agreement with the experimental data than the DSMJ model, while the results of both models converge at large n .