Abstract. Collisional and thermal ionization of sodium nS and nD Rydberg atoms with n=8-20 has been studied. The experiments were performed using a twostep 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 has been found that the atomic ions were created mainly due to photoionization of Rydberg atoms by photons of blackbody radiation at the ambient temperature of 300K. 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 Collisional and thermal ionization of sodium Rydberg atoms I 2

Detailed analysis of spectral line broadening and variations in relative intensities of hyperfine spectral components due to optical pumping is presented. Hyperfine levels of sodium 3p 1/2 and 3p 3/2 levels are selectively excited in a supersonic beam at various laser intensities under the conditions when optical pumping time is shorter than transit time of atoms through the laser beam. The excitation spectra exhibit significant line broadening at laser intensities well below the saturation intensity, and redistribution of intensities of hyperfine spectral components is observed, which in some cases is contradicting with intuitive expectations. Theoretical analysis of the dynamics of optical pumping shows that spectral line broadening depends sensitively on branching coefficient of the laser-driven transition. Analytical expressions for branching ratio dependent critical Rabi frequency and critical laser intensity are derived, which give the threshold for onset of noticeable line broadening by optical pumping. The critical laser intensity has its smallest value for transitions with branching coefficient equal to 0.5, and it can be much smaller than the saturation intensity. Transitions with larger and smaller branching coefficients are relatively less affected. The theoretical excitation spectra were calculated numerically by solving density matrix equations of motion using the split propagation technique, and they well reproduce the observed effects of line broadening and peak intensity variations. The calculations also show that presence of dark (i.e., not laser-coupled) Zeeeman sublevels in the lower state results in effective branching coefficients which vary with laser intensity and differ from those implied by the sum rules, and this can lead to peculiar changes in peak ratios of hyperfine components of the spectra.

We consider Penning ionization of Rydberg atom pairs as an Auger-type process induced by the dipole-dipole interaction and employ semiclassical formulae for dipole transitions to calculate the autoionization width as a function of the principal quantum numbers, n d , n i , of both atoms. While for symmetric atom pairs with = = n n n d i 0 the well-known increase of the autoionization width with increasing n 0 is obtained, the result for asymmetric pairs is counterintuitive-for a fixed n i of the ionizing atom of the pair, the autoionization width strongly increases with decreasing n d of the de-excited atom. For H Rydberg atoms this increase reaches two orders of magnitude at the maximum of the n d dependence, and the same type of counterintuitive behavior is exhibited also by Na, Rb and Cs atoms. This is a purely quantummechanical effect, which points towards existence of optimal (we call them 'Tom' and 'Jerry' for 'big' and 'small') pairs of Rydberg atoms with respect to autoionization efficiency. Building on the model of population redistribution in cold Rydberg gases proposed in [1], we demonstrate that population evolution following the initial laser excitation of Rydberg atoms in state n 0 would eventually lead to the formation of such Tom-Jerry pairs with > > n n n i d 0 which feature autoionization widths that are enhanced by several orders of magnitude compared to that of two atoms in the initial laser-excited state n 0 . We also show that in the high-density regime of cold Rydberg gas experiments the ionization rate of Tom-Jerry pairs can be substantially larger than the blackbody radiation-induced photoionization rate.

This paper is devoted to clarifying the implications of hyperfine (HF) interaction in the formation of adiabatic (i.e., "laser-dressed") states and their expression in the Autler-Townes (AT) spectra. We first use the Morris-Shore model [J. R. Morris and B. W. Shore, Phys. Rev. A 27, 906 (1983)] to illustrate how bright and dark states are formed in a simple reference system where closely spaced energy levels are coupled to a single state with a strong laser field with the respective Rabi frequency S . We then expand the simulations to realistic hyperfine level systems in Na atoms for a more general case when non-negligible HF interaction can be treated as a perturbation in the total system Hamiltonian. A numerical analysis of the adiabatic states that are formed by coupling of the 3p 3/2 and 4d 5/2 states by the strong laser field and probed by a weak laser field on the 3s 1/2 − 3p 3/2 transition yielded two important conclusions. Firstly, the perturbation introduced by the HF interaction leads to the observation of what we term "chameleon" states-states that change their appearance in the AT spectrum, behaving as bright states at small to moderate S , and fading from the spectrum similarly to dark states when S is much larger than the HF splitting of the 3p 3/2 state. Secondly, excitation by the probe field from two different HF levels of the ground state allows one to address orthogonal sets of adiabatic states; this enables, with appropriate choice of S and the involved quantum states, a selective excitation of otherwise unresolved hyperfine levels in excited electronic states.

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 nonadiabatic 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.

A model potential method is used to investigate photoabsorption from the Na(3p3/2) state. Absorption cross sections into higher Rydberg states and photoionization cross sections are presented as an analytical function of photo electron energy. Einstein coefficients for spontaneous emissions 3p3/2 ← ns1/2, nd5/2, nd3/2 are tabulated for n up to 50. The Einstein coefficients and low-energy ionization cross sections are believed to be accurate to better than 2–3%, above 1 eV the error may increase to 4–6%.

The results of experimental and theoretical studies of collisional ionization of Na Rydberg atoms in nS and nD (n = 8-20) states are presented. Molecular and atomic ions from associative ionization and photoionization by blackbody radiation were detected after pulsed laser excitation of Rydberg states in crossed Na atomic beams. An original method of determination of associative ionization rate constants based on the measurement of ratios of molecular and atomic ion signals was used, which did not require the determination of absolute number density of Rydberg atoms. The measured rate constants of associative ionization of Rydberg atoms in collisions with ground-state Na atoms are compared with the results of our earlier single-beam experiment and theoretical calculations. It is shown that the stochastic ionization model, which describes the collisional ionization of Rydberg atoms in terms of chaotic migration of highly excited electron induced by the motion of the colliding nuclei, yields a significantly better agreement with the experimental results than the earlier Duman-Shmatov-Mihajlov-Janev model.

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