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arXiv:1310.5137

Heavy Rydberg Photo-dissociation Cross-section Calculations and Experimental Progress Towards Cold Collisions in Lithium

Lisa Madeleine Ugray

Published Oct 18, 2013• 0 citations
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Abstract

This thesis is divided into two parts, each of which supports constructing and using a lithium magneto-optical trap for cold collision studies: Part I: One outgoing channel of interest from cold collisions is the production of ion pairs. We describe an effective method for calculating bound-to-continuum cross-sections for charged binary systems by examining transitions to states above the binding energy that become bound when the system is placed within an infinite spherical well. This approach is verified for ionization of a hydrogen atom, and is then applied to the heavy Rydberg system Li+...I-. Part II: A wavemeter previously built in the lab is redesigned for increased reliability and ease of use by replacing the optical hardware with a rocker system, which can be aligned in mere minutes rather than half a day as was previously the case. The new wavemeter has been tested through saturated absorption spectroscopy of lithium.

DOI
10.48550/arxiv.1310.5137

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This thesis is divided into two parts, each of which supports constructing and using a lithium magneto-optical trap for cold collision studies: Part I: One outgoing channel of interest from cold collisions is the production of ion pairs. We describe an effective method for calculating bound-to-continuum cross-sections for charged binary systems by examining transitions to states above the binding energy that become bound when the system is placed within an infinite spherical well. This approach is verified for ionization of a hydrogen atom, and is then applied to the heavy Rydberg system Li+...I-. Part II: A wavemeter previously built in the lab is redesigned for increased reliability and ease of use by replacing the optical hardware with a rocker system, which can be aligned in mere minutes rather than half a day as was previously the case. The new wavemeter has been tested through saturated absorption spectroscopy of lithium.
In this dissertation, I explore several aspects of Rydberg physics with laser spectroscopy. The experiments center around the use of a very deep, cavity-generated, one-dimensional optical lattice in a cold atom sample. The optical lattice produces elongated clouds of dense, cold atoms via dipole trapping and is able to generate extreme light shifts in the atoms due to its high intensity. I describe experiments which may be divided into two main classes. In the first, I use the dipole trap to prepare a dense sample of atoms for photoassociation of Rb atom pairs into diatomic Rydberg molecules. The Rydberg molecules are formed by low-energy scattering of the Rydberg electron of one atom from the other atom, which is a ground-state atom. This novel binding mechanism also has relevance for chemical physics. I present binding energy measurements for eight different cases of Rydberg molecules. The binding energies reveal information about electron-atom collisions, such as their scattering lengths, and about the spin couplings present within the molecular system. In the second class of experiments, I introduce two proposed measurements in which the optical lattice is ramped to very high intensity during the laser excitation, creating AC Stark shifts in the transition frequencies. In one measurement, low-lying atomic states are probed. Measurements of the light shifts are expected to yield data on the dynamic polarizability and the photoionization cross section of the 5D3/2D_{3/2}D3/2​-state in rubidium in a 1064-nm light field. I show corresponding preliminary experimental data. The polarizability and photo-ionization cross-section measurements will provide tests of atomic structure theory, which is important both at a fundamental level and for applications such as atomic clocks. In another proposed measurement, Rydberg atoms in the lattice experience ponderomotive shifts and strong mixing of their angular-momentum states, allowing direct optical excitation of the lattice-mixed high-angular-momentum states. I describe the theoretical basis and experimental preparation for spectroscopically characterizing the lattice-mixed states. The ability to optically excite selected high-angular-momentum states without the use of static or RF fields may be useful for quantum information processing and simulation.
The authors have designed and assembled an experiment to determine the rate of fine structure changing collisions between ultra-cold ({approximately} 1 mK) laser cooled Li atoms. The atoms are confined by a magneto-optical trap which consists of six polarized orthogonal laser beams tuned slightly below the 2S{sub 1/2}-2P{sub 3/2} resonance frequency of lithium. Measurements show that about 2 x 10{sup 7} atoms are confined to a roughly spherical region of about 1 mm in diameter. Fine structure changing collisions occur when an atom in the 2S{sub 1/2} state and an atom in the 2P{sub 3/2} state collide, and yield an atom in the 2S{sub 1/2} state and an atom in the 2P{sub 1/2} state, with an energy release corresponding to about 10 GHz. This energy adds kinetic energy to the atoms in the trap, and knocks atoms out of the trap. The authors have devised a method to measure the rate of this collisional loss mechanism. The method uses a laser diode and a dye laser to selectively photo-ionize the 2P{sub 1/2} atoms, and a channeltron particle multipiler measures the rate of ion formation. We will report the progress of this experiment.
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.
There is at present great interest in the properties of ultracold molecules. Molecules are created in traps in excited rovibrational states and any vibrational relaxation results in the trap loss. This thesis provides a theoretical study of interactions and collisions in the spin-polarized lithium -b lithium dimer system at ultralow energies. Potential energy surface of the electronic quartet ground state of lithium trimer is generated ab initio using the CCSD(T) method and represented by an IMLS/Shepard fit. Long-range nonadditive interactions are modelled using a symmetric global form with coefficients taken from a fit to the atom-molecule dispersion coefficients. The surface allows barrierless atom-exchange reactions. It has a global minimum of ≈ 4000 cm(^-1) at equilateral geometries with r(_e) = 3.1 Å. The nonadditive interactions are very strong near equilibrium. They increase the well depth by a factor of 4 and reduce the interatomic distance by ≈ 1 Å. Another surface of À symmetry in C(_s) meets the ground state surface at linear geometries at short range. Part of the seam, near D(_ooh) geometries, is in an energetically accessible region for cold collisions. Inside the seam, the lowest À surface correlates with (^4)II rather than (^4)Σ state. Inelastic and reactive collisions are investigated using a quantum mechanical coupled channel method in hyperspherical coordinates. Bosonic and fermionic systems in the spin-stretched states are considered. The inelastic rate coefficients from the rovibrationally excited states of dimer at ultralow collision energies are large, often above 10-(^-10) cm(^3)s(^-1) The elastic cross sections are ≈ 3 orders of magnitude lower at 1 nK. Atom-molecule mixtures, at the densities found in Bose-Einstein condensates of alkali metal atoms that were recently produced, would last only a fraction of a second. Classical Langevin model describes semi-quantitatively the energy dependence of inelastic cross sections above ≈ 50 mK. No systematic differences between the bosonic and fermionic systems were found. Sensitivity of the results on potential was investigated. Reactions in isotopic mixtures of lithium may be exothermic even from the molecular ground state. The reactive rate coefficients are 1 - 2 orders of magnitude smaller than those in systems involving an initially vibrationally excited dimer.
Our goal is the preparation and study of ultra- cold plasma and Rydberg matter. We assembled an ex- perimental setup for laser cooling of lithium atoms in a magneto-optical trap (MOT). Trapping of 7 Li atoms in a MOT is demonstrated for a wide range of cooling laser detunings. The number density of 7 Li atoms at different ground-state sublevels is measured by using a probe tun- able laser. The temperature of the trapped atoms is esti- mated. Obtained information is important for the prepara- tion of ultra-cold plasma and highly-excited atoms. duction of recombination in such systems. Our theoreti- cal works show the appearance of short and long-range order (7) and a large reduction of the recombination rate (a few orders of magnitude) in the ultra-cold mixture of Rydberg atoms and plasma in the presence of a strong magnetic field (8-11). The ability to control the decay and crystallization processes in an ensemble of Rydberg atoms could find an application in quantum storage and quan- tum computers. The suggested experiments can model the behavior of the plasma recombination in experiments on creating anti-hydrogen (12-14), and help to increase the number of ground state anti-hydrogen atoms in a strong magnetic field. It is noteworthy that lithium is an element which is very close to hydrogen.