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.
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.
The energy level spectrum of a many-body system containing two shared, collective Rydberg excitations is measured using cold atoms in an optical dipole trap. Two pairs of independently tunable laser pulses are employed to spectroscopically probe the spectrum in a double-resonance excitation scheme. Depending on the magnitude of an applied electric field, the Rydberg-atom interactions can vary from resonant dipole-dipole to attractive or repulsive van der Waals, leading to characteristic signatures in the measured spectra. Our results agree with theoretical estimates of the magnitude and sign of the interactions.
We review here the studies performed about interactions in an assembly of cold Rydberg atoms. We focus especially on the review of the dipole–dipole interactions and on the effect of the dipole blockade in the laser Rydberg excitation, which offers attractive possibilities for quantum engineering. We present first the various interactions between Rydberg atoms. The laser Rydberg excitation of such an assembly is then described with the introduction of the dipole blockade phenomenon. We report recent experiments performed in this subject by starting with the case of a pair of atoms allowing the entanglement of the wave-functions of the atoms and opening a fascinating way for the realization of quantum bits and quantum gates. We consider then several works on the blockade effect in a large assembly of atoms for three different configurations: blockade through electric-field induced dipole, through Förster resonance, and in van der Waals interaction. The properties of coherence and cooperativity are analyzed. Finally, we treat the role of dipole–dipole interactions between Rydberg atoms responsible for Penning ionization. The perturbation of the dipole blockade by ions and the evolution of the Rydberg towards an ultracold plasma are discussed.
Rydberg atoms are increasingly being used as a means of introducing long-range, tunable interactions into atomic systems through their strong dipole-dipole interactions. When creating such interactions, however, there are a variety of potential effects that can occur, such as state (n and/or L) changing or Penning ionization, which can complicate the dynamics of the system. In the following work, such interactions are investigated for Rydberg-Rydberg collisions using very high-n, n ~300, strontium Rydberg atoms in an atomic beam configuration. By exploiting Rydberg blockade and the inherent distribution of atomic velocities present in an atomic beam, it is possible to create a 1D array of moving Rydberg atoms which will naturally overtake each other over time. Measurements of both Penning ionization and state changing for such collisions are made and compared with classical trajectory Monte-Carlo (CTMC) simulations, with both indicating large collisional cross sections on the order of 1 x 10-6 cm2 for Penning ionization and nearly 8 x 10-5 cm2 for state changing interactions. In a second series of experiments, previous work involving doubly-excited Rydberg states is expanded upon by investigating autoionization with high-n, L > 3, Rydberg states. Past research involving autoionization has shown that the effect is strongly L-dependent, with high-L states having significantly smaller autoionizing rates. To create well-defined, L > 3 states, the use of microwave fields to drive various high-n, n ~ 150, n1F3 → (n+1)1G4, (n+2)1H5 transitions is investigated, with spectroscopic measurements of these transitions providing quantum defect values for n1G4 and n1H5 states. These measurements provide a basis for future studies into the L-dependence of high-n, n ~ 300, autoionizing Rydberg atoms, with the eventual goal of creating a long-lived, doubly-excited “planetary” Rydberg state.
We use perturbation theory to directly calculate the van der Waals and dipole-dipole energy shifts of pairs of interacting Rb Rydberg atoms for different quantum numbers n, $\ensuremath{\ell}$, j, and mj, taking into account a large number of perturbing states. Our results can be used to identify good experimental parameters and illuminate important considerations for applications of the ``Rydberg-excitation blockade.'' We also use the results of the calculation to explain features of previous experimental data on the Rydberg-excitation blockade. To explore control methods for the blockade, we discuss energy shifts due to atom-atom interaction in an external electric field.
We have observed the evolution of cold Rydberg gases and ultracold plasmas in an environment that allows for the control of interactions of the blackbody radiation temperature from 4K to 300K. The work in this thesis describes the influence of initial densities, populations, excitation state, evolution time and thermal background temperature on the evolution of cold Rydberg gases as well as directly excited ultracold plasmas. With some initial ionization, cold-Rydberg-atom gases easily develop a positive space charge that traps electrons for times on the order of tens of mus. This acts as a catalyst for electron-Rydberg atom collisions, increasing the collision probabilities by orders of magnitude and profoundly altering the final state of the Rydberg gas. Using state-selective field ionization, we have provided direct proof that these collisions cause changes in l-states, and we have seen the first experimental evidence that they also lead to inelastic n-changing collisions, as predicted by theory. We have also found evidence for Rydberg-Rydberg collisions, enabled by the attractive electric-dipole forces between atoms in high-l states and possibly by van-der-Waal's interactions at very high-n . Thermal interactions are seen to influence the formation of a plasma from a cold Rydberg gas. Plasmas form more easily in the presence of a 300K radiation field than at 4K, due to the contribution of thermal ionization to the plasma formation. The background temperature also appears to affect the electron temperature in both the directly excited plasma and the plasma spontaneously formed from a cold Rydberg gas. In Rydberg atom gases that have undergone partial ionization, electron temperatures were estimated using the dependence of n-changing collisions on the electron temperature.
Using state-selective field ionization, the state distributions of Rydberg atoms in cold Rydberg gases are measured for various initially excited Rydberg levels, populations, and evolution times. We provide direct experimental evidence for l-changing collisions that we previously observed indirectly [S. K. Dutta, D. Feldbaum, A. Walz-Flannigan, J. R. Guest, and G. Raithel, Phys. Rev. Lett. 86, 3993 (2001)]. We also observe n-mixing and find that its effects are largely in agreement with recent theoretical work on n-changing collisions between electrons and Rydberg atoms, thus enabling an estimation of the electron temperature. Unexpectedly large populations of atoms are found in states with principal quantum numbers much lower than that of the initially excited atoms. We explain this observation by collisions between high-l Rydberg atoms, which are highly polar and can collide due to static electric-dipole forces between them.