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In this thesis, I present an experimental study of quantum control techniques for transferring population between vibrational states of atoms trapped in an optical lattice. Results from a range of techniques are compared, including techniques tested previously in the same system. In the study of the Adiabatic Rapid Passage (ARP) technique, control of population transfer is realized through varying the chirp rate and modulation amplitude of a frequency-chirped sinusoidal displacement of the lattice. Meanwhile, dependence of population transfer on the chirp direction is observed, which is explained by a model of ARP in a 3-level system. In the study of the coherent control technique, interference between a one-phonon transition at 2\omega and a two-phonon transition at omega is experimentally demonstrated. The omega and 2\omega transitions are realized by sinusoidally displacing the optical lattice at omega and sinusoidally modulating the lattice depth at 2\omega, respectively. The branching ratio of transitions to the first excited state and to higher excited states is controlled by varying the relative phase between these two pathways. The highest measured branching ratio of 17\pm2 is achieved among all the experiments using this coherent control scheme. In the study of the GRadient Ascent Pulse Engineering (GRAPE) technique, a "pulse" involving both displacement and depth-modulation of the lattice is used to transfer population. This pulse is theoretically engineered with the GRAPE algorithm to optimize the fidelity between the first excited state and the final state, when the lattice Hamiltonian without gravity for a specific lattice depth is considered. The experimental result shows that there is almost no excitation into higher excited states during population transfer from the ground to the first excited state, even when this process is affected by gravity and inhomogeneous broadening in reality. By comparing all the techniques, the GRAPE technique is found to be the best in terms of increasing population transfer into the first excited state while reducing excitation into higher excited states. On the other hand, the ARP technique creates the highest normalized population inversion, a ratio of the difference to the sum of the ground and the first excited state populations.

In this thesis, I present an experimental study of quantum control techniques for transferring population between vibrational states of atoms trapped in an optical lattice. Results from a range of techniques are compared, including techniques tested previously in the same system. In the study of the Adiabatic Rapid Passage (ARP) technique, control of population transfer is realized through varying the chirp rate and modulation amplitude of a frequency-chirped sinusoidal displacement of the lattice. Meanwhile, dependence of population transfer on the chirp direction is observed, which is explained by a model of ARP in a 3-level system. In the study of the coherent control technique, interference between a one-phonon transition at 2\omega and a two-phonon transition at omega is experimentally demonstrated. The omega and 2\omega transitions are realized by sinusoidally displacing the optical lattice at omega and sinusoidally modulating the lattice depth at 2\omega, respectively. The branching ratio of transitions to the first excited state and to higher excited states is controlled by varying the relative phase between these two pathways. The highest measured branching ratio of 17\pm2 is achieved among all the experiments using this coherent control scheme. In the study of the GRadient Ascent Pulse Engineering (GRAPE) technique, a "pulse" involving both displacement and depth-modulation of the lattice is used to transfer population. This pulse is theoretically engineered with the GRAPE algorithm to optimize the fidelity between the first excited state and the final state, when the lattice Hamiltonian without gravity for a specific lattice depth is considered. The experimental result shows that there is almost no excitation into higher excited states during population transfer from the ground to the first excited state, even when this process is affected by gravity and inhomogeneous broadening in reality. By comparing all the techniques, the GRAPE technique is found to be the best in terms of increasing population transfer into the first excited state while reducing excitation into higher excited states. On the other hand, the ARP technique creates the highest normalized population inversion, a ratio of the difference to the sum of the ground and the first excited state populations.

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The problem of a vibrating-rotating polyatomic molecule is treated, with emphasis given to the case of molecules with C_3v symmetry. It is shown that several of the gross features of the rotational spectra of polyatomic molecules in excited vibrational states can be predicted by group theoretical considerations. Expressions for the rotational transition frequencies of molecules of C_3v symmetry in the ground vibrational state, singly excited degenerate vibrational states, and doubly excited degenerate vibrational states are given. The derivation of these expressions by fourth order perturbation theory as given by Amat, Nielsen, and Tarrago is discussed. The ground and V_10=1 rotational spectra of propyne have been investigated in the 17 to 70 GHz, and 17 to 53 GHz regions, respectively, and compared with predictions based on higher frequency measurements. The V_9=1 and V_10=2 rotational spectra of propyne have been investigated and assigned for the first time. A perturbation of the V_9=1 rotational spectra for K=-l has been discovered and discussed.

A new intermolecular potential energy surface, rovibrational transition frequencies, and line strengths are computed for OCS-OCS and CO2-CS2. The potentials were made by fitting energies obtained from explicitly correlated coupled-cluster calculations and fit using an interpolating moving least squares method. Rovibrational transition frequencies are also calculated for four isotopologues of the N2O dimer using a previously presented potential energy surface. The rovibrational Schroedinger equation for all three dimers is solved with a symmetry-adapted Lanczos algorithm and an uncoupled product basis set. All four intermolecular coordinates are included in the calculation. On the OCS-OCS potential energy surface, a previously unknown, cross-shaped isomer is found along with polar and non-polar isomers. For CO2-CS2, the previously found cross-shaped minima is found along with a slipped-parallel configuration. The associated wavefunctions and energy levels for each of these isomers is presented. To identify states that have a permanent dipole, both calculations of line strengths and vibrational parent analysis is used. For non polar states of, OCS-OCS, and N2O-N2O isotopologues, and all CO2-CO2 states, only vibrational parent analysis was used. Calculated rotational constants differ from their experimental counterparts by less than 0.001 wavenumbers for OCS-OCS and CO2-CS2, and less than 0.002 wavenumbers for any N2O-N2O isotopologue. / Thesis (Master, Physics, Engineering Physics and Astronomy) -- Queen's University, 2012-08-23 13:19:45.294