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Physics World

Rydberg states form molecular probes

Published Jul 1, 1998• 0 citations
Publisher

Abstract

Experiments have shown for the first time that Rydberg states can form in weakly bound molecular clusters. Rydberg states have been studied extensively in atoms, where one electron is excited into a large orbit around the nucleus. Equivalent states were observed in large molecules a few years ago, and the new results extend those findings to even larger molecular systems.

DOI
10.1088/2058-7058/11/7/4

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Experiments have shown for the first time that Rydberg states can form in weakly bound molecular clusters. Rydberg states have been studied extensively in atoms, where one electron is excited into a large orbit around the nucleus. Equivalent states were observed in large molecules a few years ago, and the new results extend those findings to even larger molecular systems.
Because of their unusual properties, Rydberg atoms, i.e., atoms with one electron occupying a highly excited orbit, have attracted the interest of many physicists. For example, due to their large size, such atoms are particularly sensitive to external fields. Fifty years ago, Segre and co-workers1 investigated the Stark effect and atomic diamagnetism of Rydberg states of alkalis with principal quantum numbers up to n = 30. During the last decade, Rydberg states have been studied extensively2 due to the availability of tunable laser radiation.
This talk will present several exciting nuggets from the last half-century of progress in our understanding of Rydberg electron physics in atoms and small molecules. Some key elements of this deepened understanding have emerged from experiments that were understood through the multichannel quantum defect theory developed by Seaton, Fano, Jungen and their collaborators. That powerful combination has enabled spectra of remarkable complexity and richness to be quantitatively understood and qualitatively interpreted using this framework. Another aspect of Rydberg physics connects with Enrico Fermi’s treatment of the interaction between a slow electron and a distant ground state atom, which has been predicted to generate a new chemical bonding mechanism that can bind an exotic long range diatomic or triatomic molecule whose internuclear distances can be as large as a small virus. The production of this class of exotic, weakly-bound Rydberg molecules has been demonstrated in a remarkable series of experiments in the last few years.
Introduction Series of atomic spectral lines had been studied by emission from excited vapors even before Balmer described the regularity of the visible lines of hydrogen in 1884. However, direct excitation had been restricted to the few lowest-lying levels, particularly those accessible by electric dipole transitions from the ground state using classical light sources. The advent of tunable lasers in the 1970s changed such spectroscopic limitations enormonsly, allowing excitation to a very much larger number of states. Atoms in highly excited states, typically with principal quantum numbers n ≥ 10, are called Rydberg atoms. They are oversize, fragile states of significant intrinsic interest. They are very rare in nature because of their size and fragility, but they are found in interstellar space (H I regions). One of the best sources for comprehensive descriptions of Rydberg atoms and references to the literature describing their exploration is Ref. [120]. It describes their characteristic properties and behavior both classically and quantum mechanically, and especially their strongly enhanced interactions with external fields. The first thing to note is that Rydberg atoms are usually characterized by a single, highly excited electron while all the other electrons remain in their original states. Thus their properties are very nearly classical, and the atoms are much closer to the ideal hydrogen-like model of Chap. 7, along with appropriate quantum defects (see Chap. 10). The spectroscopy of such states is especially interesting because the active electron is much less perturbed by the other electrons in the atom than when it is in lower states. Moreover, there are some special circumstances in which the energy of a Rydberg state is degenerate with an atomic state having two electrons excited to lower levels, and such configurations yield further new information. Second, Rydberg atoms do not usually decay back to the ground state by emission of characteristic radiation, so their study is mediated by other techniques that reveal new and interesting properties. Such properties arise because Rydberg atoms have a huge dipole moment and very low binding energy resulting from the large average distance between the excited electron and the nucleus-plus-core of the rest of the atom with net charge e . Third, transitions between Rydberg states are quite different from those connecting to the ground state for at least three reasons.
Abstract Ultracold molecules formed from association of a single Rydberg atom with surrounding atoms or molecules and those from double Rydberg excitations are discussed in this review. Ultralong-range Rydberg molecules possess a novel molecular bond resulting from scattering of the Rydberg electron from the perturber atoms or molecules. The strong interactions between Rydberg atoms in ultracold gases may lead to formation of macroscopic Rydberg macrodimers. The exquisite control over the properties of the Rydberg electron means that interesting and unusual few-body and quantum many-body features can be realized in such systems.
Rydberg atom is one with a highly excited electron, and this electron can interact with a second atom in its ground state to form a weakly bound Rydberg molecule.One example of such a bound state is a "trilobite Rydberg molecule," so-called because the electron's probability distribution resembles the long-extinct sea creature.Markus Exner at the Technical University of Kaiserslautern, Germany, and colleagues have now obtained high-resolution measurements of the vibrational spectra of trilobite Rydberg molecules formed from pairs of rubidium atoms [1].The results offer a rigorous test of theoretical models.