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 .
Atoms and molecules in highly excited (Rydberg) states have a number of unique characteristics due to the strong dependence of their properties on the values of principal quantum numbers. The paper discusses the results of an investigation of collisional Rydberg complexes specific features, resulting in the development of dynamic chaos and the accompanying diffusion autoionization processes. It is shown (experiment and theory) that, in subthermal low energies, the global chaotic regime that evolved in quasimolecular systems leads to significant changes in the Rydberg gases radiation/ionization kinetics. The effect of Förster resonance on the width of the fluorescence spectra and stochastic ionization processes in Rydberg systems is also discussed.
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.
We report a systematic experimental and numerical study of the expansion of ultra-cold Rydberg plasmas. Specifically, we have measured the asymptotic expansion velocities,
v0, of ultra-cold neutral plasmas (UNPs) which evolve from cold, dense samples of Rydberg rubidium atoms using ion time-of-flight spectroscopy. From this, we have obtained values for the effective initial plasma electron temperature,
Te,0=mionv02/kB (where
mion is the Rb
+ ion mass), as a function of the original Rydberg atom density and binding energy,
Eb,i. We have also simulated numerically the interaction of UNPs with a large reservoir of Rydberg atoms to obtain data to compare with our experimental results. We find that for Rydberg atom densities in the range
107−109 cm
−3, for states with principal quantum number
n>40,
Te,0 is insensitive to the initial ionization mechanism which seeds the plasma. In addition, the quantity
kBTe,0 is strongly correlated with the fraction of atoms which ionize, and is in the range
0.6×∣Eb,i∣≲kBTe,0≲2.5×∣Eb,i∣. On the other hand, plasmas from Rydberg samples with
n≲40 evolve with no significant additional ionization of the remaining atoms once a threshold number of ions has been established. The dominant interaction between the plasma electrons and the Rydberg atoms is one in which the atoms are deexcited, a heating process for electrons that competes with adiabatic cooling to establish an equilibrium where
Te,0 is determined by their Coulomb coupling parameter,
Γe∼0.01.
ization of Rydberg atoms by a single-cycle pulse, and also its implications for the strong field ionization of ground state. The required threshold field amplitude (for 10% ionization probability) scales inversely with the binding energy of initial states and also the pulse-duration square when the pulse duration becomes much shorter than the classical Rydberg period. A simple model is introduced to understand this threshold behavior, where the nonzero displacement induced by a single-cycle pulse plays a critical role. By combining with the adiabatic-ionization threshold in the low-frequency limit, an ionization window is expected for the ionization of different states. The ionization-probability curve exhibits a “ripple” structure as a function of the pulse duration and the field amplitude, which is sensitive to the angular distribution of initial states. The observation of larger emitted-electron energy for the ionization of lower-lying Rydberg states in a recent experiment [S Li and R. R. Jones, Phys. Rev. Lett. 112, 143006 (2014)] is confirmed in our calculations for both sodium and hydrogen atoms. The differences between the ionization dynamics in a single-cycle pulse and that in a multi-cycle pulse are also discussed and presented.