Broad bandwidth, precision spectroscopy of the molecular ions of interest to the JILA electron electric dipole moment experiment, HfF+ and ThF+, is necessary due to the limited amount of spectroscopic information available and the large theoretical uncertainties in the energy level structure (thousands of wavenumbers). This thesis covers the development of a novel spectroscopic technique, frequency comb velocity-modulation spectroscopy, that provides high resolution, broad spectral bandwidth, ion discrimination and high sensitivity simultaneously. Frequency comb velocity-modulation spectroscopy as well as single-frequency velocity-modulation spectroscopy have been used to identify five rotational bands of HfF+. This work discusses the first spectroscopic information for HfF+ which came from our measurement of the 1Π1 – 1Σ+ (0,0) band recorded with single-frequency velocitymodulation spectroscopy with a sensitivity of 3x10-7 Hz-1/2. The development of frequency comb velocity-modulation spectroscopy allowed us to cover a thousand wavenumbers of spectral bandwidth and to identify an additional four HfF + bands. The achieved sensitivity for frequency-comb velocity-modulation spectroscopy was 4x10-8 Hz-1/2 (spectral element) -1/2 with 1500 simultaneous detection channels spanning 150 cm -1 of bandwidth. For a 30 minute acquisition time using 30 interleaved images to densely sample the whole spectrum, this corresponded to a 3x10 -7 single-pass fractional absorption sensitivity for each of the 45,000 measurement channels. The spectroscopic information from all five HfF + rotational bands is presented and molecular constants for the 1Σ+, 3Π1, and 1Π1 states were extracted.
|Advisor:||Cornell, Eric A.|
|Commitee:||Jin, Deborah, Lewandowski, Heather, Lineberger, W. Carl, Ye, Jun|
|School:||University of Colorado at Boulder|
|School Location:||United States -- Colorado|
|Source:||DAI-B 73/04, Dissertation Abstracts International|
|Subjects:||Molecular physics, Atoms & subatomic particles|
|Keywords:||Hafnium fluoride, JILA eEDM experiment, Molecular ions, Velocity-modulation spectroscopy|
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