Resonance ionization spectroscopy, RIS, is a multistep photon absorption process in which the final state is the ionization continuum of an atom. The RIS process can be saturated with available pulsed lasers, so that one electron can be removed from each atom of the selected type. This method was first applied to the determination of the absolute number of Hes(2/sup 1/S) excited states produced when pulsed beams of protons interacted with helium gas. Laser schemes for RIS are classified into five basic types; with these, nearly all of the elements can be detected with commercially available lasers. A periodic table is included showing schemes applicable to all of the elements except He, Ne, F, and Ar. A compact theory of the RIS process is presented which delineates the conditions under which rate equations apply. Questions on the effects of collisional line broadening, laser coherence time, and nonresonant multiphoton ionization processes are discussed. The initial demonstration of one-atom detection of Cs is described. By using laser beams to saturate the RIS process and proportional counters as single-electron detectors, one-atom detection is made possible. With RIS, one-atom detection is highly selective, has the ultimate in sensitivity, and has excellent space and timemore » resolution. Furthermore, a modification of the technique in which single electrons (or single ions) are detected with a channel electron multiplier permits single-atom detection in a vacuum. The authors describe how RIS can be used for photophysics measurements such as far wing collisional line broadening, measurements of photoionization cross sections for excited states, and collisional redistribution among excited states.« less

Resonance ionization spectroscopy and one-atom detection

https://web.stanford.edu/group/Zarelab/publinks/145.pdf

Multiphoton ionization: a method for characterizing molecular beams and beam reaction products*

We report the first observation of perturbed and unperturbed Rydberg progressions of atomic uranium. Highlying levels within 1000 ${\mathrm{cm}}^{\ensuremath{-}1}$ of the ionization limit were accessed by time-resolved stepwise excitation using dye laser pulses tuned to resonant transitions. Atoms excited to these states were then photoionized by intense infrared radiation from a pulsed ${\mathrm{CO}}_{2}$ laser. The resultant photoion production was monitored. By delaying the infrared ionizing pulse, and thus discriminating against the shorter-lived valence states, we preferentially detected Rydberg levels with principal quantum numbers $n$ exceeding 60. Series convergence yields a value of the ionization limit of 6.1941 \ifmmode\pm\else\textpm\fi{} 0.0005 eV, in fair agreement with the value of 6.1912 \ifmmode\pm\else\textpm\fi{} 0.0025 eV obtained in photoionization studies. Ab initio calculations indicate that the unperturbed series belong to highly excited $5{f}^{3}7{s}^{2}\mathrm{np}$ and $\mathrm{nf}$ configurations.

Detection of Rydberg states in atomic uranium using time-resolved stepwise laser photoionization

: A revised and updated annotated bibliography on atomic transition probabilities covering the literature from 1914 through October 1977 is presented It contains approximately 2400 references and is divided into four main sections, with each article assigned a number The first section contains a listing, by number, of articles of general interest The second section lists by number all articles containing numerical data; it is arranged by element and stage of ionization and is further subdivided according to theoretical and experimental methods, comments, and compilations The third section contains a listing of all articles, including number, authors, title, and journal reference; it is arranged by year of publication and alphabetically by authors names within the year All foreign language papers are identified, and their titles are translated into English The final section contains a listing of all authors and the numbers of the papers they have authored or co-authored

Bibliography on Atomic Transition Probabilities: 1914 Through October 1977

Publisher Summary This chapter focuses on the general properties of Rydberg atoms, methods of production and detection, and spectroscopic techniques. The properties of the Rydberg atoms are very much hydrogen-like. Their energy is given by the Rydberg formula. Differences between Rydberg states of atoms and molecules arise from rotational vibrational excitations of the molecular ion. This leads to drastic effects when the frequency of the orbiting electron becomes comparable to the rotational vibrational frequencies. As a result, one finds a breakdown of the Born–Oppenheimer approximation and observes autoionization if part of the rotational vibrational energy is transferred to the Rydberg electron. For a certain class of molecules, even low-lying excited states show typical properties of Rydberg states. Because smooth changes are characteristic of classical systems, Rydberg atoms can be expected to show classical properties. In particular, according to Bohr's correspondence principle, the frequency of electromagnetic radiation emitted for transitions between neighboring states approaches the frequency at which the electron rotates around the ionic core.

Rydberg Atoms: High-Resolution Spectroscopy and Radiation Interaction—Rydberg Molecules

We report the observation of over 100 new high-lying odd levels in atomic uranium between 32 600 and 34 200 cm−1 using tunable laser techniques. These augment the 32 odd levels previously determined in this energy regime by conventional atomic spectroscopy. The method used in these studies, multistep photoionization under pulsed dye laser excitation, was also employed to make J assignments, measure radiative lifetimes, and to obtain absorption cross sections of transitions involving these levels.

Radiative lifetimes, absorption cross sections, and the observation of new high-lying odd levels of 238 U using multistep laser photoionization*

Determination of absolute atomic transition probabilities using time resolved optical pumping

D2 Observation and study of high lying rydberg and valence states in atomic uranium by multistep photoionization

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Detection of Rydberg states in atomic uranium using time-resolved stepwise laser photoionization

Radiative lifetimes, absorption cross sections, and the observation of new high-lying odd levels of 238 U using multistep laser photoionization*

Determination of absolute atomic transition probabilities using time resolved optical pumping

D2 Observation and study of high lying rydberg and valence states in atomic uranium by multistep photoionization