In Situ Observation of Nonpolar to Strongly Polar Atom-Ion Collision Dynamics
Moritz Berngruber, Daniel J. Bosworth, O. A. Herrera-Sancho, Viraatt S. V. Anasuri, N. Zuber, Frederic Hummel, Johann Krauter, Florian Meinert, R. Löw, Peter Schmelcher, Tilman Pfau
The onset of collision dynamics between an ion and a Rydberg atom is studied in a regime characterized by a multitude of collision channels. These channels arise from coupling between a nonpolar Rydberg state and numerous highly polar Stark states. The interaction potentials formed by the polar Stark states show a substantial difference in spatial gradient compared to the nonpolar state leading to a separation of collisional timescales, which is observed in situ. For collision energies in the range of k_{B}μK to k_{B}K, the dynamics exhibit a counterintuitive dependence on temperature, resulting in faster collision dynamics for cold-initially "slow"-systems. Dipole selection rules enable us to prepare the collision pair on the nonpolar potential in a highly controlled manner, which determines occupation of the collision channels. The experimental observations are supported by semiclassical simulations, which model the pair state evolution and provide evidence for tunable nonadiabatic dynamics.
The onset of collision dynamics between an ion and a Rydberg atom is studied in a regime characterized by a multitude of collision channels. These channels arise from coupling between a nonpolar Rydberg state and numerous highly polar Stark states. The interaction potentials formed by the polar Stark states show a substantial difference in spatial gradient compared to the nonpolar state leading to a separation of collisional timescales, which is observed in situ. For collision energies in the range of k_{B}μK to k_{B}K, the dynamics exhibit a counterintuitive dependence on temperature, resulting in faster collision dynamics for cold-initially "slow"-systems. Dipole selection rules enable us to prepare the collision pair on the nonpolar potential in a highly controlled manner, which determines occupation of the collision channels. The experimental observations are supported by semiclassical simulations, which model the pair state evolution and provide evidence for tunable nonadiabatic dynamics.
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.
Scattering of K(np) Rydberg atoms by electron-attaching molecules can result in the formation of positive-negative ion pairs through electron transfer reactions. These reactions can involve the dissociation of a transient intermediate negative ion into a smaller negative ion and a neutral fragment, or they can result in the parent molecule forming a metastable negative ion, with the excess energy being distributed among its internal modes. For Rydberg atoms of intermediate n, it is possible for these ion pairs to orbit each other at large separation, weakly bound by their mutual electrostatic attraction, forming what are known as heavy-Rydberg states. Measurements of the binding energy and velocity distributions of the ion pairs are used to probe the dynamics of electron transfer reactions. The data are analyzed using a semiclassical Monte Carlo collision code to explore the lifetime of the intermediate, the nature of its dissociation, the distribution of the excess energy of reaction, and the branching ratio of the various reaction channels. Results obtained using a variety of attaching targets including CF3I, CCl4, SF6, CH2Br2, 1,1,1-C2Cl3F3, CCl3Br, Fe(CO)5, and CH3NO2 have demonstrated both the wide variety of different behaviors that can accompany electron capture as well as the different behaviors of the product ion-pair states themselves. Remarkably, despite previous work showing that it was possible for CH3NO2 to form long-lived valence-bound negative ions through Rydberg electron transfer, the present work showed that such collisions do not result in the formation of long-lived bound ion-pair states. Rather, the data show that collisions lead to very strong Rydberg atom scattering through formation of transient ion-pair states. These results are consistent with theoretical work that predicts significant collisional quenching of Rydberg atoms by highly polar molecules and highlight a new mechanism for Rydberg atom scattering.
Heavy-Rydberg ion-pair states, molecular quantum systems that are bound by their long-range pure Coulomb attraction, are formed through Rydberg atom collisions with molecules that attach low energy electrons. Collisions of potassium Rydberg atoms K(np) with the attaching species CCl4 and SF6 lead, respectively, to dissociative and non-dissociative electron attachment with subsequent formation of bound ion-pair states K+..Cl- and K+..SF6-.\nThe experimental apparatus used to produce and detect heavy-Rydberg ion-pair states consists of a reaction region and a separate analysis region. It separates a fraction of the product ion pairs from the parent Rydberg atoms, eliminating spurious background signals associated with blackbody-induced and electric-field ionization of Rydberg atoms. A position sensitive detector in the analysis region is employed to measure their velocity, angular, and binding energy distribution and lifetimes. Measurements of the spatial distribution of ion pairs provide information on their velocity and angular distributions, and their binding energy distribution is measured using electric field-induced dissociation. The lifetime of the ion-pair states is influenced by multiple processes including internal-to-translational energy transfer, autodetachment of the electron, and neutralization through charge transfer.\nThe experimental results are compared with the results of a Monte Carlo collision code that models both the initial Rydberg electron attachment and the subsequent evolution and molecular dynamics of the ion pairs. This model highlights the factors such as the kinematics of the Rydberg atom and the attaching particle and energy released in dissociation (in the case of dissociative attachment) that are important in governing ion pair formation. The model calculations are in good agreement with the experimental data.
Rydberg-atom ensembles are switched from a weakly to a strongly interacting regime via adiabatic transformation of the atoms from an approximately nonpolar into a highly dipolar quantum state. The resultant electric dipole-dipole forces are probed using a device akin to a field ion microscope. Ion imaging and pair-correlation analysis reveal the kinetics of the interacting atoms. Dumbbell-shaped pair-correlation images demonstrate the anisotropy of the binary dipolar force. The dipolar C_{3} coefficient, derived from the time dependence of the images, agrees with the value calculated from the permanent electric-dipole moment of the atoms. The results indicate many-body dynamics akin to disorder-induced heating in strongly coupled particle systems.
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.
Cold polar molecules offer fascinating prospects for ultracold chemistry and quantum physics. However, their inherent collision properties remain largely unknown, as it seems fundamentally impossible to reach sufficiently low energies by merging two beams of molecules with substantial dipole moments. Here we report measurements of state-to-state cross-sections for collisions between ammonia isotopologues at energies between 0.3 and 100 cm−1 using an advanced beam-merging protocol. We experimentally observed a local maximum in the cross-sections, which indicates that the dipole moments can switch off at low collision energies. Scattering calculations reproduced this maximum in good agreement and explained the observed scaling with the molecule’s parity splitting energies. Measurements of the correlated energy transfer in both collision partners yielded direct evidence of the suppression of the dipole–dipole interaction at low energies. Our results demonstrate how collisions between an important class of polar molecules evolve from high temperatures towards the ultracold regime in a counterintuitive way, and offer distinctive opportunities to control cold molecular collisions with external fields. Interactions between polar molecules are expected to become increasingly strong at low collision energies through dipole–dipole forces. Now it has been shown that ammonia molecules instead exhibit suppressed dipolar interactions in the cold regime as the dipole moment effectively switches off, as shown by local maxima in the collision cross-sections.