Abstract The strong interaction between individual Rydberg atoms provides a powerful tool exploited in an ever-growing range of applications in quantum information science, quantum simulation and ultracold chemistry. One hallmark of the Rydberg interaction is that both its strength and angular dependence can be fine-tuned with great flexibility by choosing appropriate Rydberg states and applying external electric and magnetic fields. More and more experiments are probing this interaction at short atomic distances or with such high precision that perturbative calculations as well as restrictions to the leading dipole–dipole interaction term are no longer sufficient. In this tutorial, we review all relevant aspects of the full calculation of Rydberg interaction potentials. We discuss the derivation of the interaction Hamiltonian from the electrostatic multipole expansion, numerical and analytical methods for calculating the required electric multipole moments and the inclusion of electromagnetic fields with arbitrary direction. We focus specifically on symmetry arguments and selection rules, which greatly reduce the size of the Hamiltonian matrix, enabling the direct diagonalization of the Hamiltonian up to higher multipole orders on a desktop computer. Finally, we present example calculations showing the relevance of the full interaction calculation to current experiments. Our software for calculating Rydberg potentials including all features discussed in this tutorial is available as open source.
Abstract The strong interaction between individual Rydberg atoms provides a powerful tool exploited in an ever-growing range of applications in quantum information science, quantum simulation and ultracold chemistry. One hallmark of the Rydberg interaction is that both its strength and angular dependence can be fine-tuned with great flexibility by choosing appropriate Rydberg states and applying external electric and magnetic fields. More and more experiments are probing this interaction at short atomic distances or with such high precision that perturbative calculations as well as restrictions to the leading dipole–dipole interaction term are no longer sufficient. In this tutorial, we review all relevant aspects of the full calculation of Rydberg interaction potentials. We discuss the derivation of the interaction Hamiltonian from the electrostatic multipole expansion, numerical and analytical methods for calculating the required electric multipole moments and the inclusion of electromagnetic fields with arbitrary direction. We focus specifically on symmetry arguments and selection rules, which greatly reduce the size of the Hamiltonian matrix, enabling the direct diagonalization of the Hamiltonian up to higher multipole orders on a desktop computer. Finally, we present example calculations showing the relevance of the full interaction calculation to current experiments. Our software for calculating Rydberg potentials including all features discussed in this tutorial is available as open source.
We develop practical formulas for the calculation of the matrix elements of the interaction of the electromagnetic field with an atomic state, beyond the long-wavelength approximation. The atom-plus-field Hamiltonian is chosen to have the multipolar form, containing the electric, paramagnetic, and diamagnetic operators. The final workable expressions include the interactions to all orders and are derived by first expanding the fields in partial waves. The electric-field operator reaches a constant value as the radial variable becomes large, contrary to the result of the electric-dipole approximation (EDA) where the value of the corresponding operator increases indefinitely. Applications are given for Rydberg states of hydrogen up to n=50 and for free-free transitions in a Coulomb potential. Such matrix elements are relevant to a number of real and virtual processes occurring during laser-atom interactions. The computation is done numerically, using a combination of analytic with numerical techniques. By comparing the results of the EDA with those of the exact treatment, it is shown that the former is inadequate in such cases. This finding has repercussions on the theory and understanding of the physics of quantum systems in high-lying Rydberg levels and wave packets or in scattering states.
The work presented in this dissertation represents a comprehensive study on long-range interactions between alkali Rydberg atoms. As a consequence of their size, Rydberg atoms possess very large dipole moments, making them highly sensitive to external fields and to other Rydberg atoms. The strong dipole-dipole interaction between two Rydberg atoms results in a mixing of their angular momentum characters, which is the cornerstone of the work presented here. We describe the ℓ-mixing between various local molecular asymptotes through a residual Coulomb potential, assuming no electron cloud overlap. We then directly diagonalize an interaction Hamiltonian consisting of these Rydberg-Rydberg interactions and spin-orbit (fine structure) coupling in the Hund's case (c). In this manner, we calculate potential energy curves for various molecular symmetries and find that some of these curves exhibit deep potential wells, capable of supporting very extended bound molecular states ( macrodimers). We analyze the specific structure of the ℓ-mixing for these potential wells and derive convenient n-scaling relations for both their equilibrium separations Re and well depths De. We also explore various properties of the macrodimers, including their response to small electric fields and stability with respect to predissociation. We note throughout the dissertation that the detection of such extended dimers could help progress studies in a variety of areas such as exotic, ultracold chemistry and quantum information and computing. To facilitate detection, we propose a scheme to form and study the macrodimers via photoassociation (PA). We present calculated PA lineshapes from two different electronic ground states based on a harmonic trapping model. We find that both PA signals vary significantly with the laser detunings, indicating that different ℓ-characters could be probed at different equilibrium lengths. Finally, we extend the two-body formalism to the case of three interacting Rydberg atoms and present preliminary results for triply excited 58p rubidium atoms along a common axis. We provide a few examples of surface plots corresponding to different local asymptotes, each with a unique three-dimensional "landscape" and discuss the relevance of the physical features. The highlight of our analysis is the appearance of a potential well, which indicates the formation of a linear trimer. ^
In this thesis I present several theoretical methods to explore the excitation dynamics of Ultracold Rydberg systems in various regimes. For some applications the details of interactions between Rydberg atoms have to be carefully examined, while for others, the many-body aspect of Rydberg excitation may be crucial. In both cases, the basic prerequisite is to know the interactions sufficiently well. I will review the basic concepts how to evaluate molecular potentials in various Hund's cases and approximations. Long-range Rydberg-Rydberg interactions between Rydberg atoms induce ℓ-mixing which in certain situations gives rise to molecular resonances. For these resonances, we calculate long-range potentials in Hund's case (c) by diagonalization of an interaction matrix. The excitation dynamics of the resonances is always modeled as pair excitation. At high principal quantum number n, the interactions between Rydberg atoms can blockade the excitation of many surrounding atoms in the range of few μm. The atoms within this range are strongly correlated so that many-body treatments are, in general, needed. To describe this blockading effect and other manifestations of the collective behavior of Rydberg excitation, such as the many-body Rabi oscillations, spatial correlations between atoms and the fluctuations of the number of excited atoms, I have used three different approaches. In the mean-field approach the interactions between different atoms is modeled by a distribution of mean-field shifts for which a distribution of probabilities is calculated, A good agreement between the theoretical model and experimental measurements is found. To study the correlations between atoms the many-body wavefunction is numerically computed. The possibility of observing the many-body Rabi oscillations of Rydberg excitation and other aspects of many-body dynamics is analyzed. Although strong interactions cannot be treated perturbatively other expansions may be feasible. I will show that the expansion in powers of the single atom Rabi frequency can be evaluated in the interaction and Heisenberg picture. The expansion is expected to behave well for arbitrary strong interactions. ^
This paper is a short introduction to Rydberg physics and quantum nonlinear optics using Rydberg atoms. It has been prepared as a compliment to a series of lectures delivered during the Latin American School of Physics “Marcos Moshinsky” 2017. We provide a short introduction to the properties of individual Rydberg atoms and discuss in detail how the interaction potential between Rydberg atom pairs is calculated. We then discuss how this interaction gives rise to the Rydberg blockade mechanism. With the aid of hallmark experiments in the field applications of the blockade for creating correlated quantum systems are discussed. Our aim is to give an overview of this exciting and rapidly evolving field. The interested reader is referred to original work and more comprehensive reviews and tutorials for further details on these subjects.
Abstract Förster resonances provide a highly flexible tool to tune both the strength and the angular shape of interactions between two Rydberg atoms. We give a detailed explanation about how Förster resonances can be found by searching through a large range of possible quantum number combinations. We apply our search method to SS , SD and DD pair states of 87 Rb with principal quantum numbers from 30 to 100, taking into account the fine structure splitting of the Rydberg states. We find various strong resonances between atoms with a large difference in principal quantum numbers. We quantify the strength of these resonances by introducing a figure of merit C ˜ 3 which is independent of the magnetic quantum numbers and geometry to classify the resonances by interaction strength. We further predict to what extent excitation exchange is possible on different resonances and point out limitations of the coherent hopping process. Finally, we discuss the angular dependence of the dipole–dipole interaction and its tunability near resonances.
In this thesis I examine high-magnetic-field Rydberg spectra, with the goal of discerning the viability of using such states as an interaction mechanism for quantum computation processes. In the presence of a strong magnetic field of B0 = 2.6 T, high-lying states of E ~ -55 cm(-1) are non-degenerate and show a wide range of magnetic dipole moments. Near-degenerate pairs of states of the same mJ manifold but of different axial parity Pi_z will strongly interact in the presence of an applied weak parallel electric field F, generating a pair of highly polar states. I show experimental results that, in agreement with theoretical work presented here, illustrate the presence of strong permanent dipole moments p ~ 1500 ea0 under these conditions. Such Rydberg states can also be tuned into resonance through careful control of the magnetic field, and are suitable for developing quantum phase gates and performing Rydberg-Rydberg interaction experiments. In order to perform such high-field Rydberg excitation experiments, a stable, dense and well-controlled cold atom cloud is needed within a high-magnetic-field environment. Toward this end, I present a full characterization of the utilized high-field trapping apparatus, including measurements of the trapped atom sample size, shape, and temperature. Analysis of the loss rate from the high-magnetic-field atom trap, both as a function of the applied magnetic field B0 and transverse confinement are presented. Experimental results for the high-field confinement of 85Rb are presented, as well as the first demonstration of a high-field 87Rb trap. Current trap limitations and possible improvements to the trapping apparatus are discussed. Other applications of the high-magnetic-field trap, such as the investigation of ultracold two-component plasmas and three-body recombination experiments, are also presented.