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Journal of Experimental and Theoretical Physics

Rydberg matter—A long-lived excited state of matter

Leif Holmlid, Edward A. Manykin

Published May 1, 1997• 13 citations
Publisher

Abstract

The theory of condensed excited matter, the so-called Rydberg matter (RM), is examined briefly. Explicit results are given for several physical quantities, notably, the work function and the resistivity, for which experimental results exist. The most important aspects of the experiments, which are fully described elsewhere, are discussed. Large densities of Rydberg species are formed in the experiments with cesium vapor in contact with carbon (graphite) surfaces. The resistivity of the RM formed is found to be 10 −2 –10 −3 Ω·m under varying conditions, while theory gives the order of 10 −3 Ω·m. The work function is experimentally found to be less than 0.7 eV, perhaps even less than 0.5 eV. Two different methods were used to extract this quantity from thermionic diode data. These work function values are much lower than reported for any known material, especially at the high temperatures, and they thus give strong support for the description of RM as a very dilute metal. Theory gives values ranging from 0.6 down to 0.2 eV, depending on the principal quantum number, which is estimated to be n =12–14 from the lifetime calculations and from the known pressure. Supporting evidence is found from spectroscopic studies of RM, from jellium calculations, and from recent confirming experiments. From the good agreement between theory and experiment we conclude that RM exists.

DOI
10.1134/1.558225

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Rydberg atom, with a large principal quantum number n, has big size, long lifetime, strong long-range interactions, and so on. These properties make Rydberg atoms potential candidate of quantum gate and single-photon source. Rydberg electron can interact with nearby ground-state atom, which is polarized by the Rydberg electron and is bound to the orbit of Rydberg electrons forming Rydberg molecule. As the kinetic energy of the Rydberg electron is very low, only the lowest partial waves will contribute to the molecular potential.#br#In this paper, the low electron-atom scattering with the semi-classical approximation is introduced, and the pseudopotential of interaction between Rydberg electron and ground-state atom is used to describe the long-range Rydberg molecular potential. Molecular potential curves for cesium (nS, n=30-60) are plotted according to the results of numerical computation, from which the outermost potential depth De and the equilibrium distance r0 of long-range cesium Rydberg molecule are deduced. Potential curves of cesium Rydberg molecules are consistent with the distribution curves in radial probability densities of cesium Rydberg electrons. Dependences of De and r0 on the principal quantum number n are investigated, this has an important role for the experimental measurements. The size of a Rydberg molecule depends on the equilibrium distance r0 and is proportional to the square of effective principal quantum number (n-δ )2. The calculated outermost potential depth De of Rydberg molecule becomes smaller with the increase of principal quantum number n. Rydberg molecule is very sensitive to the external field and can be used to measure and monitor weak signals.

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The radiative lifetimes τrad of the highly excited 4f7/2136s1/2(4)np3/2[11/2](n=21−31) Rydberg Tm states have been measured with the method of multistep laser excitation and electric field ionization. The lifetime values have been obtained with an accuracy of better than 15%. The influence of blackbody radiation on the states with n ≥ 27 has been observed. The experimental results are in good agreement with our previously calculated values obtained by relativistic perturbation theory with a zero-order model approximation. It has been shown that the τrad-versus-n* dependence (n* is the effective principal quantum number) is best described by the relation τrad = 0.0022.(n*)2.46 (μsec). This property may be attributed to the strongly expressed nonhydrogenlike behavior of the investigated states, which is caused by the essentially non-Coulombic core potential acting on the Rydberg electron.

Journal of the Optical Society of America B•Dec 1, 1989•8 citations
The theory of condensed excited matter, the so-called Rydberg matter (RM), is examined briefly. Explicit results are given for several physical quantities, notably, the work function and the resistivity, for which experimental results exist. The most important aspects of the experiments, which are fully described elsewhere, are discussed. Large densities of Rydberg species are formed in the experiments with cesium vapor in contact with carbon (graphite) surfaces. The resistivity of the RM formed is found to be 10 −2 –10 −3 Ω·m under varying conditions, while theory gives the order of 10 −3 Ω·m. The work function is experimentally found to be less than 0.7 eV, perhaps even less than 0.5 eV. Two different methods were used to extract this quantity from thermionic diode data. These work function values are much lower than reported for any known material, especially at the high temperatures, and they thus give strong support for the description of RM as a very dilute metal. Theory gives values ranging from 0.6 down to 0.2 eV, depending on the principal quantum number, which is estimated to be n =12–14 from the lifetime calculations and from the known pressure. Supporting evidence is found from spectroscopic studies of RM, from jellium calculations, and from recent confirming experiments. From the good agreement between theory and experiment we conclude that RM exists.
Abstract A condensed excited matter called Rydberg Matter (RM) have been studied experimentally for 30 years, but have not sparked widespread attention yet, unlike ordinary Rydberg atoms. RM formed by clusters of Rydberg atoms at a solid surface have a longer lifetime compared to Rydberg atoms, and is liquid-like. This review describes how the RM state is generated, and its potential applications. These include using RM for research into catalysis, space phenomena and sensor applications, or for producing environmentally friendly energy. A background on RM is presented, with its structure and special properties, and the working principle of RM generation. The experimental set-ups, materials, and detectors used are discussed, together with methods to improve the amount of RM produced. The materials used for the catalysts are of special interest, as this should have a large influence on the energy of the RM, and therefore also on the applications. Currently most of the catalysts used are potassium doped iron oxide designed for styrene production, which should give the possibility of improvements. And as there is little knowledge on the exact mechanisms for RM formation, suggestions are given as to where research should start.
Rydberg matter is a condensed excited state made of highly excited atoms. State of art of research in the field of Rydberg matter is briefly reviewed. Special attention is focused on the contribution of Russian and Swedish scientists' groups to the analysis of this problem. Most attention is concentrated on physical principles of pseudopotential method and density functional theory used to describe the Rydberg matter. The description of Rydberg matter as an excited state becomes viable after the formal replacement of excited atoms by ground state pseudoatoms. This procedure has been used to find parameters of Rydberg matter made of highly excited cesium atoms. Theoretical estimations conform to experimental data available.
Summary form only given. Laser-cooled atoms can be excited into Rydberg states to study Rydberg gases at high densities and low atomic velocities. Dense clouds of such atoms undergo virtually complete ionization when their density exceeds a critical value dependent on the principal quantum number n. We report a new regime in which the excited Rydberg population spontaneously evolves into long-lived high-l states, the lifetimes of which exceed the natural lifetimes of the initially excited Rydberg levels by two orders of magnitude. /sup 87/Rb atoms are collected and cooled to 50 /spl mu/K in a magneto optical trap (MOT), which is periodically turned off for 50 ms. 1 ms after the shutdown of the MOT the Rydberg atoms are created via a two-step excitation process using a 5 /spl mu/s long diode laser pulse.
Rydberg atom, with a large principal quantum number n, has big size, long lifetime, strong long-range interactions, and so on. These properties make Rydberg atoms potential candidate of quantum gate and single-photon source. Rydberg electron can interact with nearby ground-state atom, which is polarized by the Rydberg electron and is bound to the orbit of Rydberg electrons forming Rydberg molecule. As the kinetic energy of the Rydberg electron is very low, only the lowest partial waves will contribute to the molecular potential.#br#In this paper, the low electron-atom scattering with the semi-classical approximation is introduced, and the pseudopotential of interaction between Rydberg electron and ground-state atom is used to describe the long-range Rydberg molecular potential. Molecular potential curves for cesium (nS, n=30-60) are plotted according to the results of numerical computation, from which the outermost potential depth De and the equilibrium distance r0 of long-range cesium Rydberg molecule are deduced. Potential curves of cesium Rydberg molecules are consistent with the distribution curves in radial probability densities of cesium Rydberg electrons. Dependences of De and r0 on the principal quantum number n are investigated, this has an important role for the experimental measurements. The size of a Rydberg molecule depends on the equilibrium distance r0 and is proportional to the square of effective principal quantum number (n-δ )2. The calculated outermost potential depth De of Rydberg molecule becomes smaller with the increase of principal quantum number n. Rydberg molecule is very sensitive to the external field and can be used to measure and monitor weak signals.
In this work the existence of a novel type of molecule is shown whose binding is based solely on electron-atom scattering. These molecules are composed of a Rydberg atom and a ground state atom - here Rb(ns) and Rb(5s) - where the binding arises from scattering of the Rydberg electron from the ground state atom. The ground state atom is bound to the Rydberg wavefunction, which has radii on the order of 100nm, and thus these molecules are of long-range. Although the theoretical description of this interaction goes back to the famous work of Fermi in the year 1934 which was expanded in the following decades by Omont and Greene, the experimental proof of their existence was still missing. Up to now, experimental evidence for the ultralong-range Rydberg molecules was found only in spectral line broadenings. The present experiments have demonstrated the direct photoassociation of these ultralong-range Rydberg molecules for Rb(ns)-Rb(5s) triplet states from a cold and dense sample of rubidium 87 atoms for a range of principal quantum numbers, n, between 34 and 40. The high-resolution photoassociation spectra allowed for the observation of several vibrational states separated by only a few Megahertz. Based on the model by Greene the vibrational ground states v=0 are assigned and the dependence of their binding energy on the principal quantum number, n, is used to extract the triplet s-wave scattering length for electron-Rb(5s) collisions from the data. The remarkably good agreement between experiment and theory for the vibrational ground state v=0 over a range of principal quantum numbers attests to the accuracy of Fermi's original pseudopotential approach in describing interactions in excited multi-atom systems. Aside from this good agreement for the state v=0, the measurements also show that contributions from p-wave scattering cannot be neglected, as a number of excited vibrational states is observed in the experiment that are not predicted from the theory assuming only s-wave scattering. Calculations of Li, Pohl and coworkers have shown that a full solution of the electron-atom scattering is necessary for the assignment of all vibrational states. This work finds the molecular bound states to be very sensitive to both s-wave as well as p-wave electron-atom scattering and the Rydberg molecules turn out to be an accurate experimental platform to study electron-atom collisions in a previously inaccessible ultralow-energy regime. In general, the ultralong-range Rydberg molecules investigated here for rubidium are expected for all species with negative scattering length for electron-atom interaction, e. g. the other alkali atoms. Rydberg atom and ground state atom do not even have to be of the same chemical element, the only requirement is a negative scattering length of the ground state atom for electron scattering. Moreover, the binding force of the Rydberg electron is not restricted to a single ground state atom and molecules with more than one ground state atom can be created. The fact that these exotic molecules have huge bond lengths but nevertheless a vibrational spectrum with several states make a new type of ultracold Rydberg chemistry feasible. In the future, larger polymers or even heteronuclear molecules can be realized, where the number of atoms, the constituent atomic elements and the addressed Rydberg state allow to precisely select the properties of the long-range molecule.
The radiative lifetimes τrad of the highly excited 4f7/2136s1/2(4)np3/2[11/2](n=21−31) Rydberg Tm states have been measured with the method of multistep laser excitation and electric field ionization. The lifetime values have been obtained with an accuracy of better than 15%. The influence of blackbody radiation on the states with n ≥ 27 has been observed. The experimental results are in good agreement with our previously calculated values obtained by relativistic perturbation theory with a zero-order model approximation. It has been shown that the τrad-versus-n* dependence (n* is the effective principal quantum number) is best described by the relation τrad = 0.0022.(n*)2.46 (μsec). This property may be attributed to the strongly expressed nonhydrogenlike behavior of the investigated states, which is caused by the essentially non-Coulombic core potential acting on the Rydberg electron.