Abstract Many light-emitting objects, such as gases, have free charges or ions, and atoms are building blocks of those objects. Therefore, there are charge-atom interactions in those objects. A better understanding of charge-atom interactions will help to understand such objects. Among those objects, many atoms are in excited states, which causes light to be emitted. Highly excited states are called Rydberg states. In this article, we study the few-body charge-atom interactions of two-dimensional configurations, or planar Rydberg-atom/charge geometries. Specifically, we study one positive charge and two atoms, three atoms, four atoms, and five atoms lying on the same plane. In addition, we assume those atoms are in excited states, Rydberg states. Moreover, we investigate the principal quantum number dependence of such interactions. It has been shown that the maximum frequency shift of the n s n s n s + states is proportional to n 6 for an energy level in a certain principal quantum number range. Furthermore, we study the 1 R 2 dependent charge-atom interactions, where R is the distance between one atom and the positive charge.
Abstract Many light-emitting objects, such as gases, have free charges or ions, and atoms are building blocks of those objects. Therefore, there are charge-atom interactions in those objects. A better understanding of charge-atom interactions will help to understand such objects. Among those objects, many atoms are in excited states, which causes light to be emitted. Highly excited states are called Rydberg states. In this article, we study the few-body charge-atom interactions of two-dimensional configurations, or planar Rydberg-atom/charge geometries. Specifically, we study one positive charge and two atoms, three atoms, four atoms, and five atoms lying on the same plane. In addition, we assume those atoms are in excited states, Rydberg states. Moreover, we investigate the principal quantum number dependence of such interactions. It has been shown that the maximum frequency shift of the n s n s n s + states is proportional to n 6 for an energy level in a certain principal quantum number range. Furthermore, we study the 1 R 2 dependent charge-atom interactions, where R is the distance between one atom and the positive charge.
Charge-dipole interactions are very common interactions among atoms and molecules, especially materials that can emit light or contain free charges. The second-order charge-dipole interactions, proportional to 1 R 4 , are stronger than the second-order dipole-dipole interactions or van der Waals interactions, proportional to 1 R 6 , at longer distances. In reality, there is more than one atom or charge; therefore, we focus on few-body charge-dipole interactions, such as charge-dipole-dipole interactions. Laser cooling and trapping allow us to study such interactions with much higher precision. In this article, charge-dipole interactions will be investigated in cold gases. To increase the interaction strength, we excite the cold atoms to highly excited states, Rydberg states. Here, we treat one Rydberg atom as a dipole; the excited electron and the ion core are the two poles of an electric dipole. Specifically, we study charge-atom interactions in cold Rydberg gases. The laser-cooled lower level atoms were excited to highly excited states, and we scanned a microwave to look at the line shape of a particular transition between two Rydberg states. It has been shown that adding a charge can enhance atom-atom interactions under certain circumstances.
Charge-dipole interactions are very common interactions among atoms and molecules, especially materials that can emit light or contain free charges. The second-order charge-dipole interactions, proportional to R41, are stronger than the second-order dipole-dipole interactions or van der Waals interactions, proportional to R61, at longer distances. In reality, there is more than one atom or charge; therefore, we focus on few-body charge-dipole interactions, such as charge-dipole-dipole interactions. Laser cooling and trapping allow us to study such interactions with much higher precision. In this article, charge-dipole interactions will be investigated in ultracold gases. To increase the interaction strength, we excite the ultracold atoms to highly excited states, Rydberg states. Here, we treat one Rydberg atom as a dipole, the excited electron and the ion core are the two poles of an electric dipole. Specifically, we study charge-atom interactions in ultracold Rydberg gases.
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.
Systems of cold, interacting Rydberg atoms are of interest because they exhibit a wide range of collective quantum phenomena. This thesis describes experimental and theoretical work related to these systems with an emphasis on two phenomena: Rydberg excitation blockades and quantum-state-changing collisions. I begin by presenting a detailed calculation of the interaction energies of two Rydberg atoms for a variety of orientations, quantum states, and applied electric fields. The calculated energies are used to interpret the experimental results that follow. I then describe measurements showing that the widths of the distributions of Rydberg excitation number are related to the effectiveness of a Rydberg excitation blockade. These distributions are investigated as a function of principal quantum number, n, and applied electric field. In the presence of a Forster resonant field, sub-Poissonian distributions are measured. I next present a spectroscopic measurement of the energy level shift of a system of atoms which collectively shares two Rydberg excitations. The qualitative nature of the shift depends sensitively on the type of interactions between the atoms (van der Waals or dipole-dipole) and may be changed by changing the quantum state or applied electric field. This measurement provides the first spectroscopic proof that Rydberg excitation blockades are operative. Finally, I describe measurements of the probability for quantum state-changing and Penning-ionizing collisions to provide evidence for intrinsic, electric field-free-interaction resonances and complex many-body interactions in systems of cold Rydberg atoms.
Abstract The interactions between dipoles are called dipole–dipole interactions. One type of dipole–dipole interaction is van der Waals interaction. Similar to van der Waals interactions, the interactions between quadrupoles are called quadrupole–quadrupole interactions. Atoms can be treated not only as dipoles but also as quadrupoles. In this article, we study the quadrupole interactions between highly excited atoms or Rydberg atoms. In addition, unlike many other calculations, in which the primary focus was on the one-dimensional two-body quadrupole–quadrupole interactions, the primary aim of this article is to study the two-dimensional few-body quadrupole–quadrupole interactions. Specifically, the two-dimensional three-body interactions are investigated. This research has many applications, such as quadrupole-blockade for quantum computing, creating molecules based on quadrupole interactions, or quadrupole–quadrupole molecules.
This thesis is a theoretical study of the behavior of electrons in atoms and molecules subjected to external electromagnetic fields. Three electronic systems have been central in this work, the atomic and quasimolecular Rydberg states and the carbon allotrope graphene. The exaggerated properties of the highly excited Rydberg atoms, such as long lifetime, large spatial extension and low binding energy make them excellent candidates for both theoretical and experimental considerations. The analytical solutions of the hydrogen atom in quantum mechanics provide a good description for most Rydberg atoms. This is exploited in the work presented in this thesis and the accompanying papers, where we show results of numerical computations on interacting Rydberg atoms, with and without the presence of radiating fields, as well as dynamic Rydberg wave packets influenced by a train of femtosecond laser pulses. In the final part of the thesis the optical process of high-order harmonic generation in an extended molecular structure, represented by graphene, is considered. Rydberg atoms have a large dipole moment due to the large average electronic radius in the atom, which leads to a very strong dipole-dipole coupling between interacting particles in a gas of cold Rydberg atoms. This interaction, which is dependent on the internuclear separation between the atoms, induces a shift in the energy levels, which again prohibits the excitation of more than one atom in the gas, an effect commonly known as the Rydberg blockade. A correlated behavior is observed for the intrashell transitions in mutually excited Rydberg atoms. The microwave field driven dynamics is significantly supressed for internuclear distances below a given conditional radius which scales linearly with the principal quantum number n. Such an entangled electronic behavior may open for the realization of quantum gates applied in quantum informatics. The long-range interaction of Rydberg atoms is dominated by the dipole-dipole terms. Nevertheless, the investigation of two interacting Rydberg atoms, without the influence of electromagnetic radiation, has shown that the lower order multipolar terms play a vital role in the energy shifts as well as for the electronic probability distributions. We found that the energy curves, when including all multipole orders, correspond to both repulsive and attractive states with a stronger repulsion than attraction. We also propose a laser assisted approach for stabilization of Rydberg gases by controlled transitions between such attractive and repulsive energy states. Single-electron ionization of a dynamic Rydberg wave packet confined within a single energy level has been investigated. The ionization probability of an intrashell Rydberg wave packet depends strongly on the degree of polarization. For a wave packet driven repeatedly between the circular (least polarized) state and the linear (most polarized) state by a rotating microwave field and subjected to a train of femtosecond laser pulses, the ionization probability will depend crucially on the laser repetition rate and number of pulses. The angular-resolved ionization probability and energy distribution in the continuum are also influenced by these parameters. The last part of the thesis is devoted to the study of high-order harmonic generation (HHG) in graphene. In the simple man’s model HHG can be described by an electron that is ionized and driven in an external field, after which it returns to the parent atom and recombines, emitting a high-energy photon with frequency that is a multiple of the incident laser frequency. We show that the harmonic spectra obtained from the interaction with linearly as well as circularly polarized femtosecond lasers yield harmonics up the classical limit for extended molecules. In contrast to diatomic molecules, the stable grid structure of graphene ensures that the harmonic generation cutoff remains constant with increasing signal power as the graphene diameter extends beyond the classical limit. Additionally, for circularly polarized lasers harmonics exceeding the classical predictions have been observed.