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Dynamics of excited atoms and molecules interacting with external fields

Sigrid Ina Simonsen

Published Aug 30, 2013• 0 citations
OpenAlex

Abstract

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.

Related papers

Many-Body Effects in Rydberg Gases : Coherent Dynamics of Strongly Interacting Two-Level Atoms and Nonlinear Optical Response of a Rydberg Gas in EIT Configuration

Martin Gärttner

Subject of this thesis is the theoretical investigation of ensembles of atoms that are coherently laser-excited to a Rydberg state. Rydberg excited atoms interact with each other over large distances, which leads to strongly correlated many-body dynamics, demanding powerful numerical tools for their modeling. The first part of the thesis deals with effective two-level atoms consisting of a ground and a Rydberg state only. For resonant laser excitation a modified scaling behavior of the excitation number is observed, which is caused by effects of finite system size and coarse graining of the medium due to the finite atomic density. For off-resonant excitation, ordered structures arise out of an initially homogeneous gas, which are reflected in strongly peaked spatial correlations and modified excitation statistics. In the second part a fast decaying intermediate level is additionally taken into account. In this situation the phenomenon of electromagnetically induced transparency (EIT) is encountered. This effect is suppressed in the presence of strong interactions between the Rydberg atoms leading to an optical nonlinearity. A model predicting the properties of a cloud of Rydberg atoms in EIT configuration is developed. In both parts the models are validated by comparing their predictions to recent experimental observations.

•Jan 1, 2014•1 citation

Simulations of systems of cold Rydberg atoms

S. J. Thwaite

The past three decades have seen extraordinary progress in the manipulation of neutral atoms with laser light, to the point where it is now routine to trap and cool both individual atoms and entire atomic clouds to temperatures of only a few tens of nanoKelvin in a controlled and repeatable fashion. In this thesis we study several applications of Rydberg atoms – atoms with an electron in a highly excited state – within such ultracold atomic systems. Due to their highly-excited electron, Rydberg atoms have a number of exaggerated properties: in addition to being physically large, they have long radiative lifetimes, and interact strongly both with one another and with applied external fields. Rydberg atoms consequently find many interesting applications within ultracold atomic physics. We begin this thesis by analysing the way in which a rubidium atom prepared in an excited Rydberg state decays to the ground state. Using quantum defect theory to model the wavefunction of the excited electron, we compute branching ratios for the various decay channels that lead out of the Rydberg states of rubidium. By using these results to carry out detailed simulations of the radiative cascade process, we show that the dynamics of spontaneous emission from Rydberg states cannot be adequately described by a truncated atomic level structure. We then investigate the stability of ultra-large diatomic molecules formed by pairs of Rydberg atoms. Using quantum defect theory to model the electronic wavefunctions, we apply molecular integral techniques to calculate the equilibrium distance and binding energy of these molecular Rydberg states. Our results indicate that these Ryberg macro-dimers are predicted to show a potential minimum, with equilibrium distances of up to several hundred nanometres. In the second half of this thesis, we present a new method of symbolically evaluating functions of matrices. This method, which we term the method of path-sums, has applications to the simulation of strongly-correlated many-body Rydberg systems, and is based on the combination of a mapping between matrix multiplications and walks on weighted directed graphs with a universal result on the structure of such walks. After presenting and proving this universal graph theoretic result, we develop the path-sum approach to matrix functions. We discuss the application of path-sums to the simulation of strongly-correlated many-body quantum systems, and indicate future directions for the method.

•Jan 1, 2012•0 citations

Stability of atomic and molecular systems in strong external fields

Qi Wei

Two projects are studied in this thesis: (1) Atomic and Molecular Stabilization in Super-Intense High-Frequency Laser Fields. (2) Entanglement of Dipole Arrays in External Electric Fields. Chapter 1 presents a general introduction and the motivation for these two projects. Chapter 2 focuses on atomic stabilization of negative multiple charged onions in linearly polarized super-intense high-frequency laser field in 3-dimensional space using both frequency independent (Section 2.2) and dependent (Section 2.3) potentials. By theoretical calculation, it is predicted that He-, He2-, Li- and Li2- are stable in super-intense high-frequency laser field. Chapter 3 studies atomic stabilization in both linearly and circularly polarized super-intense high-frequency laser field in both 3 dimensional space and large-D limit. Chapter 4 studies stabilization of simple diatomic molecules in linearly polarized super-intense high-frequency laser field in both 3 dimensional space and large-D limit. It was proved, in chapter 3 and 4, that dimensional scaling, combined with the High-Frequency Floquet theory, provides a useful means to evaluate the stability of gas phase atomic anions in a superintense laser field. Chapter 5 focuses on He-He bonding in linearly polarized super-intense high-frequency laser field. The distribution of the vibronic transitions from electric ground state to [special characters omitted] excited state for He2 in superintense high frequency laser fields is obtained by numerical methods. Chapter 6 studies entanglement of multi-dimensional systems of dipoles in external electric fields. A new entanglement switch of qubits consisting of electric dipoles oriented along or against an external electric field and coupled by the electric dipole-dipole interaction is proposed in this chapter. The pairwise entanglement can be tuned and controlled by the ratio of the Rabi frequency and the dipole-dipole coupling strength. Tuning the entanglement can be achieved for one, two and three-dimensional arrangements of the qubits. The feasibility of building such an entanglement switch is also discussed in this chapter.

•Jan 1, 2010•1 citation

Rubidium Rydberg atoms in strong fields

Giulio Casati, Boris V. Chirikov

In this chapter experiments on rubidium Rydberg atoms in external fields are reviewed [1 – 8]. In the first part results on the interaction of microwave radiation with rubidium Rydberg atoms are described. The Rydberg atoms interact with a microwave pulse of a well-defined duration. When applying coherent microwave radiation with a frequency exceeding a certain value, the experimentally observed microwave field strength at which 10% of the atoms are ionized has to be much larger than the value found by classical trajectory calculations. The atoms are stabilized by the dynamical localization. An extremely weak microwave broadband noise which is added to the coherent wave at least partially destroys the localization. This phenomenon depends on the bandwidth of the added noise. In further experiments the dependence of the 10% ionization microwave field strength on the duration τ of the microwave pulse has been investigated. For increasing noise level the 10% ionization field strength ∈ 0.1 develops from a behavior ∈ 0.1 ∼ τ −1/4 to a ∈ 0.1 ∼ τ −1/2 dependence, which is characteristic for a classical diffusion process. The second part of the chapter deals with experiments in strong static crossed electric and magnetic fields. Below as well as above the ionization energy the observed quasi-Landau(QL)-resonances are explained using classical trajectories. The ionization behavior of the QL-resonances is clearly influenced by the spatial structure of the associated classical orbits. In further experiments the dependence of the observed ionization energy on the magnetic field was investigated in the presence of a fixed static electric field.

Cambridge University Press eBooks•Apr 27, 1995•0 citations

Rydberg-ground state interaction in ultracold quantum gases

Thomas Niederprüm

Combining ultracold atomic gases with the peculiar properties of Rydberg excited atoms gained a lot of theoretical and experimental attention in recent years. Embedded in the ultracold gas, an interaction between the Rydberg atom and the surrounding ground state atoms arises through the scattering of the Rydberg electron from an intruding perturber atom. This peculiar interaction gives rise to a plenitude of previously unobserved effects. Within the framework of the present thesis, this interaction is studied in detail for Rydberg \(P\)-states in rubidium. Due to their long lifetime, atoms in Rydberg states are subject to scattering with the surrounding ground state atoms in the ultracold cloud. By measuring their lifetime as a function of the ground state atom flux, we are able to obtain the total inelastic scattering cross section as well as the partial cross section for associative ionisation. The fact that the latter is three orders of magnitude larger than the size of the formed molecular ion indicates the presence of an efficient mass transport mechanism that is mediated by the Rydberg–ground state interaction. The immense acceleration of the collisional process shows a close analogy to a catalytic process. The increase of the scattering cross section renders associative ionisation an important process that has to be considered for experiments in dense ultracold systems. The interaction of the Rydberg atom with a ground state perturber gives rise to a highly oscillatory potential that supports molecular bound states. These so-called ultralong-range Rydberg molecules are studied with high resolution time-of-flight spectroscopy, where we are able to determine the binding energies and lifetimes of the molecular states between the two fine structure split \(25P\)-states. Inside an electric field, we observe a broadening of the molecular lines that indicates the presence of a permanent electric dipole moment, induced by the mixing with high angular momentum states. Due to the mixing of the ground state atom’s hyperfine states by the molecular interaction, we are able to observe a spin-flip of the perturber upon creation of a Rydberg molecule. Furthermore, an incidental near-degeneracy in the underlying level scheme of the \(25P\)-state gives rise to highly entangled states between the Rydberg fine structure state and the perturber’s hyperfine structure. These mechanisms can be used to manipulate the quantum state of a remote particle over distances that exceed by far the typical contact interaction range. Apart from the ultralong-range Rydberg molecules that predominantly consist of only one low angular momentum state, a class of Rydberg molecules is predicted to exist that strongly mixes the high angular momentum states of the degenerate hydrogenic manifolds. These states, the so-called trilobite- and butterfly Rydberg molecules, show very peculiar properties that cannot be observed for conventional molecules. Here we present the first experimental observation of butterfly Rydberg molecules. In addition to an extensive spectroscopy that reveals the binding energy, we are also able to observe the rotational structure of these exotic molecules. The arising pendular states inside an electric field allow us, in comparison to the model of a dipolar rotor, to extract the precise bond length and dipole moment of the molecule. With the information obtained in the present study, it is possible to photoassociate butterfly molecules with a selectable bond length, vibrational state, rotational state, and orientation inside an electric field. By shedding light on various previously unrevealed aspects, the experiments presented in this thesis significantly deepen our knowledge on the Rydberg–ground state interaction and the peculiar effects arising from it. The obtained spectroscopic information on Rydberg molecules and the changed reaction dynamics for molecular ion creation will surely provide valuable data for quantum chemical simulations and provide necessary data to plan future experiments. Beyond that, our study reveals that the hyperfine interaction in Rydberg molecules and the peculiar properties of butterfly states provide very promising new ways to alter the short- and long-range interactions in ultracold many-body systems. In this sense the investigated Rydberg–ground state interaction not only lies right at the interface between quantum chemistry, quantum many-body systems, and Rydberg physics, but also creates many new and fascinating possibilities by combining these fields.

•Jan 1, 2016•1 citation

Spatial and temporal correlations in cold Rydberg gases

Markus Stecker

Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.

•Jan 1, 2018•0 citations
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.
Subject of this thesis is the theoretical investigation of ensembles of atoms that are coherently laser-excited to a Rydberg state. Rydberg excited atoms interact with each other over large distances, which leads to strongly correlated many-body dynamics, demanding powerful numerical tools for their modeling. The first part of the thesis deals with effective two-level atoms consisting of a ground and a Rydberg state only. For resonant laser excitation a modified scaling behavior of the excitation number is observed, which is caused by effects of finite system size and coarse graining of the medium due to the finite atomic density. For off-resonant excitation, ordered structures arise out of an initially homogeneous gas, which are reflected in strongly peaked spatial correlations and modified excitation statistics. In the second part a fast decaying intermediate level is additionally taken into account. In this situation the phenomenon of electromagnetically induced transparency (EIT) is encountered. This effect is suppressed in the presence of strong interactions between the Rydberg atoms leading to an optical nonlinearity. A model predicting the properties of a cloud of Rydberg atoms in EIT configuration is developed. In both parts the models are validated by comparing their predictions to recent experimental observations.
The past three decades have seen extraordinary progress in the manipulation of neutral atoms with laser light, to the point where it is now routine to trap and cool both individual atoms and entire atomic clouds to temperatures of only a few tens of nanoKelvin in a controlled and repeatable fashion. In this thesis we study several applications of Rydberg atoms – atoms with an electron in a highly excited state – within such ultracold atomic systems. Due to their highly-excited electron, Rydberg atoms have a number of exaggerated properties: in addition to being physically large, they have long radiative lifetimes, and interact strongly both with one another and with applied external fields. Rydberg atoms consequently find many interesting applications within ultracold atomic physics. We begin this thesis by analysing the way in which a rubidium atom prepared in an excited Rydberg state decays to the ground state. Using quantum defect theory to model the wavefunction of the excited electron, we compute branching ratios for the various decay channels that lead out of the Rydberg states of rubidium. By using these results to carry out detailed simulations of the radiative cascade process, we show that the dynamics of spontaneous emission from Rydberg states cannot be adequately described by a truncated atomic level structure. We then investigate the stability of ultra-large diatomic molecules formed by pairs of Rydberg atoms. Using quantum defect theory to model the electronic wavefunctions, we apply molecular integral techniques to calculate the equilibrium distance and binding energy of these molecular Rydberg states. Our results indicate that these Ryberg macro-dimers are predicted to show a potential minimum, with equilibrium distances of up to several hundred nanometres. In the second half of this thesis, we present a new method of symbolically evaluating functions of matrices. This method, which we term the method of path-sums, has applications to the simulation of strongly-correlated many-body Rydberg systems, and is based on the combination of a mapping between matrix multiplications and walks on weighted directed graphs with a universal result on the structure of such walks. After presenting and proving this universal graph theoretic result, we develop the path-sum approach to matrix functions. We discuss the application of path-sums to the simulation of strongly-correlated many-body quantum systems, and indicate future directions for the method.
Two projects are studied in this thesis: (1) Atomic and Molecular Stabilization in Super-Intense High-Frequency Laser Fields. (2) Entanglement of Dipole Arrays in External Electric Fields. Chapter 1 presents a general introduction and the motivation for these two projects. Chapter 2 focuses on atomic stabilization of negative multiple charged onions in linearly polarized super-intense high-frequency laser field in 3-dimensional space using both frequency independent (Section 2.2) and dependent (Section 2.3) potentials. By theoretical calculation, it is predicted that He-, He2-, Li- and Li2- are stable in super-intense high-frequency laser field. Chapter 3 studies atomic stabilization in both linearly and circularly polarized super-intense high-frequency laser field in both 3 dimensional space and large-D limit. Chapter 4 studies stabilization of simple diatomic molecules in linearly polarized super-intense high-frequency laser field in both 3 dimensional space and large-D limit. It was proved, in chapter 3 and 4, that dimensional scaling, combined with the High-Frequency Floquet theory, provides a useful means to evaluate the stability of gas phase atomic anions in a superintense laser field. Chapter 5 focuses on He-He bonding in linearly polarized super-intense high-frequency laser field. The distribution of the vibronic transitions from electric ground state to [special characters omitted] excited state for He2 in superintense high frequency laser fields is obtained by numerical methods. Chapter 6 studies entanglement of multi-dimensional systems of dipoles in external electric fields. A new entanglement switch of qubits consisting of electric dipoles oriented along or against an external electric field and coupled by the electric dipole-dipole interaction is proposed in this chapter. The pairwise entanglement can be tuned and controlled by the ratio of the Rabi frequency and the dipole-dipole coupling strength. Tuning the entanglement can be achieved for one, two and three-dimensional arrangements of the qubits. The feasibility of building such an entanglement switch is also discussed in this chapter.
In this chapter experiments on rubidium Rydberg atoms in external fields are reviewed [1 – 8]. In the first part results on the interaction of microwave radiation with rubidium Rydberg atoms are described. The Rydberg atoms interact with a microwave pulse of a well-defined duration. When applying coherent microwave radiation with a frequency exceeding a certain value, the experimentally observed microwave field strength at which 10% of the atoms are ionized has to be much larger than the value found by classical trajectory calculations. The atoms are stabilized by the dynamical localization. An extremely weak microwave broadband noise which is added to the coherent wave at least partially destroys the localization. This phenomenon depends on the bandwidth of the added noise. In further experiments the dependence of the 10% ionization microwave field strength on the duration τ of the microwave pulse has been investigated. For increasing noise level the 10% ionization field strength ∈ 0.1 develops from a behavior ∈ 0.1 ∼ τ −1/4 to a ∈ 0.1 ∼ τ −1/2 dependence, which is characteristic for a classical diffusion process. The second part of the chapter deals with experiments in strong static crossed electric and magnetic fields. Below as well as above the ionization energy the observed quasi-Landau(QL)-resonances are explained using classical trajectories. The ionization behavior of the QL-resonances is clearly influenced by the spatial structure of the associated classical orbits. In further experiments the dependence of the observed ionization energy on the magnetic field was investigated in the presence of a fixed static electric field.
Combining ultracold atomic gases with the peculiar properties of Rydberg excited atoms gained a lot of theoretical and experimental attention in recent years. Embedded in the ultracold gas, an interaction between the Rydberg atom and the surrounding ground state atoms arises through the scattering of the Rydberg electron from an intruding perturber atom. This peculiar interaction gives rise to a plenitude of previously unobserved effects. Within the framework of the present thesis, this interaction is studied in detail for Rydberg PPP-states in rubidium. Due to their long lifetime, atoms in Rydberg states are subject to scattering with the surrounding ground state atoms in the ultracold cloud. By measuring their lifetime as a function of the ground state atom flux, we are able to obtain the total inelastic scattering cross section as well as the partial cross section for associative ionisation. The fact that the latter is three orders of magnitude larger than the size of the formed molecular ion indicates the presence of an efficient mass transport mechanism that is mediated by the Rydberg–ground state interaction. The immense acceleration of the collisional process shows a close analogy to a catalytic process. The increase of the scattering cross section renders associative ionisation an important process that has to be considered for experiments in dense ultracold systems. The interaction of the Rydberg atom with a ground state perturber gives rise to a highly oscillatory potential that supports molecular bound states. These so-called ultralong-range Rydberg molecules are studied with high resolution time-of-flight spectroscopy, where we are able to determine the binding energies and lifetimes of the molecular states between the two fine structure split 25P25P25P-states. Inside an electric field, we observe a broadening of the molecular lines that indicates the presence of a permanent electric dipole moment, induced by the mixing with high angular momentum states. Due to the mixing of the ground state atom’s hyperfine states by the molecular interaction, we are able to observe a spin-flip of the perturber upon creation of a Rydberg molecule. Furthermore, an incidental near-degeneracy in the underlying level scheme of the 25P25P25P-state gives rise to highly entangled states between the Rydberg fine structure state and the perturber’s hyperfine structure. These mechanisms can be used to manipulate the quantum state of a remote particle over distances that exceed by far the typical contact interaction range. Apart from the ultralong-range Rydberg molecules that predominantly consist of only one low angular momentum state, a class of Rydberg molecules is predicted to exist that strongly mixes the high angular momentum states of the degenerate hydrogenic manifolds. These states, the so-called trilobite- and butterfly Rydberg molecules, show very peculiar properties that cannot be observed for conventional molecules. Here we present the first experimental observation of butterfly Rydberg molecules. In addition to an extensive spectroscopy that reveals the binding energy, we are also able to observe the rotational structure of these exotic molecules. The arising pendular states inside an electric field allow us, in comparison to the model of a dipolar rotor, to extract the precise bond length and dipole moment of the molecule. With the information obtained in the present study, it is possible to photoassociate butterfly molecules with a selectable bond length, vibrational state, rotational state, and orientation inside an electric field. By shedding light on various previously unrevealed aspects, the experiments presented in this thesis significantly deepen our knowledge on the Rydberg–ground state interaction and the peculiar effects arising from it. The obtained spectroscopic information on Rydberg molecules and the changed reaction dynamics for molecular ion creation will surely provide valuable data for quantum chemical simulations and provide necessary data to plan future experiments. Beyond that, our study reveals that the hyperfine interaction in Rydberg molecules and the peculiar properties of butterfly states provide very promising new ways to alter the short- and long-range interactions in ultracold many-body systems. In this sense the investigated Rydberg–ground state interaction not only lies right at the interface between quantum chemistry, quantum many-body systems, and Rydberg physics, but also creates many new and fascinating possibilities by combining these fields.
Rydberg atoms, i.e. atoms with one or more highly excited electrons, show exaggerated properties compared to ground state atoms. For example, their energy levels are very sensitive to external electric fields (Stark effect) and they exhibit strong interatomic interactions, which can lead to a suppression of excitation known as the Rydberg blockade. The latter property makes Rydberg atoms promising candidates for quantum simulation and quantum computing. This work describes the direct observation of the excitation blockade for highly Stark-shifted Rydberg atoms induced by controllable dipole-dipole interactions. We investigate the electric field region around and above the classical ionization threshold, which is typically not considered suitable for blockade experiments. We excite Rydberg atoms in the energy region corresponding to the unperturbed 43S1/2 state at electric fields around 127V/cm out of a magneto-optically trapped cloud of 87Rb atoms with a temperature of 150 μK. We tune the dipole-dipole interaction by the applied electric field thus changing the electric dipole moment of the excited state. The position of the Rydberg atoms is detected by ionization and subsequent ion imaging; the controlled ionization of the atoms is achieved by adiabatic transfer of the Rydberg state to an ionizing state. For the spatially resolved detection of the atoms, a high resolution ion microscope for cold atoms has been developed and experimentally characterized. It features a maximum magnification of 1000 and sub-micrometer spatial resolution. A theoretical treatment of highly Stark-shifted Rydberg states is developed introducing a complex absorbing potential. It is capable of predicting the ionization rates of the Rydberg states for a wide range of electric fields and energies with only one free parameter. Together with the numerical calculations, measurements of the ionization spectra for different Rydberg states are presented. The 43S1/2 state is measured in an electric-field range from 125V/cm to 165V/cm (classical ionization limit 127V/cm), the 70S1/2 state in an electric-field range from 15V/cm to 35V/cm (classical ionization limit 16.1V/cm) and the 100S1/2 state in an electric-field range from 7V/cm to 19V/cm (classical ionization limit 3.7V/cm). Our results show an intricate energy level structure with broad, strongly ionizing states as well as sharp, nearly non-ionizing states. The numerical calculations are also used for the prediction of selective field ionization spectra and the results are used to identify Förster resonances in the Stark spectrum of the 45D5/2 state. Complementary to the spatially resolved measurements in high electric fields, the Rydberg blockade effect is also observed via the excitation number statistics at Förster resonances.