Thesis (Ph. D.)--University of Canterbury, 2009. / Typescript (photocopy). "May 2009." Includes bibliographical references (p. 10/1-10/9). Also available via the World Wide Web.

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Thesis (Ph D.)--University of Nevada, Reno, 2007. / "May 2007." Includes bibliographical references (leaves 61-63). Online version available on the World Wide Web.

Thesis (Ph. D.)--University of Texas at Austin, 2001. / Vita. Includes bibliographical references. Available also in a digital version from UMI/Dissertation Abstracts International.

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This experiment was aimed at the determination of the dipole moment of the diatomic molecule HC1⁺ (in the ²π½ state). The method was to observe the Stark splitting optically by using a 3.4 meter Jarrell ash spectrograph. The charged diatomic molecule was obtained by passing HCl gas through a LoSurdo discharge tube in which a high electric field was applied; optical plates were obtained from the spectrograph and analysed. Dipole moment of HC1⁺ in the ²π½ state was found to be smaller than 0.8 debye. / Science, Faculty of / Physics and Astronomy, Department of / Graduate

Ultracold bialkali polar molecules present a wealth of opportunities in quantum science research and technology; including fields such as quantum simulation, quantum chemistry, quantum metrology, precision measurement and quantum computation. A great deal of interest lies in their rich internal rotational and vibrational state structure and their large electric dipole moment. However, the additional complexity also provides significant challenges. To date, only a limited number of molecular species are available at ultracold temperatures below 1 microkelvin. The assembly of heteronuclear ground state molecules from ultracold atoms has emerged as a promising approach for creating ultracold molecules. In this thesis, I will present the creation of the first ultracold gases of NaCs ground state molecules. First, we produce an ultracold mixture of Na and Cs. Second, we associate weakly bound molecular pairs from the Na-Cs mixture. Finally, we apply a two-photon stimulated Raman adiabatic passage (STIRAP) pulse to transfer the weakly bound NaCs molecules into the deeply bound rovibrational ground state. I report on the construction of a new apparatus that produces ultracold mixtures of Na and Cs. We use this apparatus to assemble weakly bound NaCs molecules and successfully transfer up to 20,000 ultracold dipolar NaCs molecules to their rovibrational ground state in each experimental run. On the way to these results, we demonstrated a pathway towards creating the first quantum degenerate mixtures of Na and Cs. We identified and characterized an interspecies Feshbach resonance at 864.12(5) G, adiabatically sweeping across it to form weakly bound NaCs Feshbach molecules. We characterized the Feshbach molecule formation in various parameter regimes. Next, we performed a study of accessible NaCs excited states and identified a pathway to the rovibrational ground state using one- and two-photon spectroscopy. Finally, we demonstrated STIRAP to the rovibrational ground state, and investigated basic properties of the ground state molecules.

Two different time-resolved spectroscopic techniques are discussed theoretically and demonstrated experimentally in dilute gases. The first technique involves extending the advantages of Stark-effect based time-resolved spectroscopy to non-polar molecules. This involves the development of a stable, TEM₀₀ mode, cw, CO₂ laser capable of switching rapidly and controllably between two frequencies. Design problems and output characteristics are discussed. The frequency switchable laser is applied to the CO₂ 10.6 μm P(16) coincidence with the non-polar molecule SF₆. The population relaxation time, T₁, is measured using two-pulse delayed nutation. The decay of induced dipoles is studied using the phenomenon of photon echoes. It is found that the echoes decay in a manner characteristic of dephasing dominated by velocity-changing collisions. A fit of the data to a model for such decays gives values of γ(ab) ≡ 1/T₂ (the non-velocity-changing contribution to the dipole decay rate), Γ(VC) (the total probability of a velocity-changing collision per unit time), and Δu which is related to the mean velocity change of SF₆ upon a velocity changing collision. A comparison with the published results of the similar Stark experiments on C¹³ H₃F are made. The second technique involves the development of an alternative to the pulsed excitation typically used in time-resolved T₁ studies. This involves inversion of a portion of the velocity distribution by adiabatic rapid passage (ARP) techniques. The center of this portion is then probed in the manner of previous delayed nutation experiments. The system preparation is shown theoretically to be different and simpler than the pulse case. In addition, ARP preparation gives a larger signal than two-pulse delayed nutation experiments. ARP experiments on N¹⁴H₃ and N¹⁵H₃ are described and compared to two-pulse delayed notation experiments. The single exponential decay best fits to the data from the two methods are found to be in agreement. We would expect the N¹⁵H₃ results to be very similar to the N¹⁴H₃ results, though reduced rotational resonance effects in its upper state should give it an overall slower decay. It is indeed found that the decay appears to be a simple exponential as did the N¹⁴H₃ data over the time range studied. The pressure dependent single exponential decay rate for N¹⁵H₃ is however roughly 45% larger than the rate for N¹⁴H₃ in the pressure range from 0.5 to 9 mTorr.

C. I. Beard, B. P. Dailey. / "June 3, 1949." / Bibliography: p. 11. / Office of Naval Research Contract N5ori-76 Joint Service Contract W-36-039sc-32037