Transitions between Rydberg states of diatomic molecules in slow collisions with atoms

A close analytic representation has been found for the Green function of highly excited diatomic molecule in the framework of the multichannel quantum defect method. This expression has been used to describe the potential energy surfaces of the quasi-molecule X ₂ ^* +A. The specific behaviour of the terms of this system has been studied as a function of the angular orientation of the moleculeX ₂ and of the distanceR between the molecule and atomA. The terms have been found to have quasi-crossings responsible for the transitions when particles suffer collision. Some terms located near the continuous spectrum boundary, when the distance varies, cross the spectrum boundary and pass into auto-ionization state. Calculations have been made for the system H ₂ ^* +B, whereB is an inert gas atom. Cross-sections of the vibrational transitions occurring under slow atom-molecule collisions have been evaluated.     

Elementary processes involving Rydberg atoms and molecules in an intense laser radiation field

An analytical review of the theory of elementary atomic and molecular processes in the field of intense laser monochromatic radiation is presented. The discussion focuses on near-threshold processes involving Rydberg intermediate complexes, which play an important role in Earth’s upper atmosphere. The possibilities of the stationary method of radiative scattering matrix, based on the formalism of the renormalized Lippmann-Schwinger equations, are demonstrated. The approach is used to describe in a unified way a variety of near-threshold processes, the probability amplitudes of which are elements of the radiative scattering matrix for all possible reaction channels. They also include processes of restructuring of the particles (predissociation, associative ionization, exchange reactions, etc.), which in principle cannot be described using traditional nonstationary theories.     

Matter-wave interferometry with atoms in high Rydberg states

Matter-wave interferometry has been performed with helium atoms in high Rydberg states. In the experiments the atoms were prepared in coherent superpositions of Rydberg states with different electric dipole moments. Upon the application of an inhomogeneous electric field, the different forces on these internal state components resulted in the generation of coherent superpositions of momentum states. Using a sequence of microwave and electric field gradient pulses the internal Rydberg states were entangled with the momentum states associated with the external motion of these matter waves. Under these conditions matter-wave interference was observed by monitoring the populations of the Rydberg states as the magnitudes and durations of the pulsed electric field gradients were adjusted. The results of the experiments have been compared to, and are in excellent quantitative agreement with, matter-wave interference patterns calculated for the corresponding pulse sequences. For the Rydberg states used, the spatial extent of the Rydberg electron wavefunction was ～320?nm. Matter-wave interferometry with such giant atoms is of interest in the exploration of the boundary between quantum and classical mechanics. The results presented also open new possibilities for measurements of the acceleration of Rydberg positronium or antihydrogen atoms in the Earth's gravitational field.     

Plasma screening within Rydberg atoms in circular states

A Rydberg atom embedded in a plasma can experience penetration by slowly moving electrons within its volume. The original pure Coulomb potential must now be replaced by a screened Coulomb potential which contains either a screening length R_s or a screening factor A = R_s ^-1 . For any given discrete energy level, there is a Critical Screening Factor (CSF) A_c beyond which the energy level disappears (by merging into the continuum). Analytical results are obtained for the classical dependence of the energy on the screening factor, for the CSF, and for the critical radius of the electron orbit for Circular Rydberg States (CRS) in this screened Rydberg atom. The results are derived for any general form of the screened Coulomb potential and are applied to the particular case of the Debye potential. We also show that CRS can temporarily exist above the ionization threshold and are therefore the classical counterparts of quantal discrete states embedded into continuum. The results are significant not only to Rydberg plasmas, but also to fusion plasmas, where Rydberg states of multi-charged hydrogen-like ions result from charge exchange with hydrogen or deuterium atoms, as well as to dusty/complex plasmas.     

Dissipative preparation of multipartite Greenberger-Horne-Zeilinger states of Rydberg atoms

The multipartite Greenberger-Horne-Zeilinger(GHZ)states play an important role in large-scale quantum information processing.We utilize the polychromatic driving fields and the engineered spontaneous emissions of Rydberg states to dissipatively drive three-and four-partite neutral atom systems into the steady GHZ states,at the presence of the nextnearest neighbor interaction of excited Rydberg states.Furthermore,the introduction of quantum Lyapunov control can help us optimize the dissipative dynamics of the system so as to shorten the convergence time of the target state,improve the robustness against the spontaneous radiations of the excited Rydberg states,and release the limiting condition for the strengths of the polychromatic driving fields.Under the feasible experimental conditions,the fidelities of three-and four-partite GHZ states can be stabilized at 99.24%and 98.76%,respectively.     

Excitation of sodium atoms by 330-nm laser pulses

1/2 ) atoms in a dense sodium vapour irradiated by nanosecond laser pulses tuned near the 3S→4P transition was investigated. It was observed that the population of Na(4P) atoms remained high only within the laser pulse, in spite of the relatively long lifetime of the 4P level (110.ns)The 3P_1/2 level, which is populated as a result of cascade transitions from the higher levels, reached the highest population several nanoseconds after the laser shot. The fast population changes are explained by cascade-stimulated transitions between the excited atomic levels. Received: 16 July 1997/Revised version: 27 October 1997     

Electric dipole moments of lithium atoms in Rydberg states

Recently, the diverse properties of Rydberg atoms, which probably arise from its large electric dipole moment(EDM),have been explored. In this paper, we report electric dipole moments along with Stark energies and charge densities of lithium Rydberg states in the presence of electric fields, calculated by matrix diagonalization. Huge electric dipole moments are discovered. In order to check the validity of the EDMs, we also use these electric dipole moments to calculate the Stark energies by numerical integration. The results agree with those calculated by matrix diagonalization.     

High resolution laser spectroscopy of Ba Rydberg atoms

The purpose of the present paper is to illustrate some selected aspects of high resolution laser spectroscopy of Rydberg atoms, rather than giving an extensive review of the state of the art. The following topics will be discussed: (i) Excitation and detection of Ba Rydberg atoms with principal quantum numbers up ton≲300; (ii) Stark effect and atomic diamagnetism of high-n Ba Rydberg states in thel-mixing region, (iii) Resonance in singlet-triplet mixing of 6snp¹P₁ and 6snd¹D₂ Ba Rydberg states deduced from hyperfine structure measurements.     

Ratiometric comparison of intense field ionization of atoms and diatomic molecules

Intense-laser ionization rates for rare gas atoms and diatomic molecules have been precisely compared by making simultaneous measurements of ionization yield vs laser intensity for mixed atomic and molecular targets. At a given laser intensity, the N (2) and F (2) ionization yields are slightly greater than that of Ar. Conversely, comparison of O (2) and S (2) with Xe indicates significant ionization suppression in these molecules. Recent molecular ionization models that successfully describe ionization suppression in O (2) and its absence in N (2) fail to explain our observations in F (2) and S (2).     

Spin-orbit and spin-rotation coupling in doublet states of diatomic molecules

The spin-rotation interaction and the centrifugal correction to the spin-orbit coupling make indistinguishable contributions to the energy levels of a diatomic molecule in a multiplet state with Λ ≠ 0. A previous method of separating these two contributions, based on the use of the vibrational dependence of the spin-orbit coupling constant, is unreliable. It is suggested here that a better procedure is one based on the isotope dependences of the spin-rotation coupling constant γ and the centrifugal correction to the spin-orbit coupling constant A_D. Both γ_e and A_De are shown to be inversely proportional to μ, the reduced mass of the molecule, but their contributions to the energy have different isotope effects. The method is used to determine values of γ_e and A_De for the X²Π state of HCl⁺, and the form of the spin-orbit coupling function A(r) in the vicinity of the equilibrium bond length is derived. The implications for RKR calculations are considered briefly.     

Nonsequential double ionization of diatomic molecules by elliptically polarized laser pulses

Using the classical ensemble method, we investigate nonsequential double ionization （NSDI） of diatomic molecules by elliptically polarized laser pulses. The results show that the ellipticity of the laser field has a strong suppression effect on NSDI probabilities both in parallel and perpendicular alignments. The double ionization （DI） channel is commonly dominated by NSDI, and the NSDI channel changes with ellipticity. As ellipticity increases, more and more NSDIs occur through recollision excitation with subsequent field ionization （RESI）. Moreover, like the case of linear polarization, the two electrons involved in NSDI for perpendicularly aligned molecules are more likely to emit into the opposite hemispheres as compared to the case of parallel alignment. Additionally, this alignment effect increases as ellipticity increases.     

Excitation of the Rydberg states of lithium in a hollow-cathode discharge

Excited states of lithium are populated in a transverse hollow-cathode discharge (HCD) working in helium-lithium mixture. Excited state population is controlled through the HCD voltage by the high-energy electrons. This excitation is distributed among the different levels by collisions with neutral atoms and low-energy electrons. The measured excitation temperatures reflect these redistribution processes.     

Radiative lifetime and photoionization cross-section for Rydberg states in alkali-metal atoms

General properties were determined and asymptotic approximation formulas for probabilities of spontaneous decay and photoionization cross-sections were derived on the basis of numerically calculated amplitudes of bound-bound and bound-free radiation transitions from Rydberg nS-, nP- and nD-states of alkali atoms with high principal quantum numbers, up to n = 1000. The departure of data from the asymptotic formulas for states with principal quantum numbers in the range between n = 10 and n = 2000 from originally calculated data does not exceed 0.1–1%, and may be useful for estimations of natural radiation widths for arbitrary high Rydberg levels.