The immaculate control of atoms and molecules with light is the defining trait of modern experiments in ultracold physics. The rich internal degrees of freedom afforded by molecules enrich the toolbox of precision spectroscopy for fundamental physics, and hold great promise for applications in quantum simulation and quantum information science. A vibrational molecular lattice clock with systematic fractional uncertainty at the 14th decimal place is demonstrated for the first time, matching the performance of the earliest optical atomic clocks. Van der Waals dimers of strontium are created at ultracold temperatures and levitated by an optical standing wave, whose wavelength is finely tuned to preserve the delicate molecular vibrational coherence.
Guided by quantum chemistry theory refined by highly accurate frequency-comb-assisted laser spectroscopy, record-long Rabi oscillations were demonstrated between vibrational molecular states that span the entire depth of the ground molecular potential. Enabled by the narrow molecular clock linewidth, hertz-level frequency shifts were resolved, facilitating the first characterization of molecular hyperpolarizability in this context. In a parallel effort, deeply bound strontium dimers are coherently created using the technique of stimulated Raman adiabatic passage. Ultracold collisions of alkaline-earth metal molecules in the absolute ground state are studied for the first time, revealing inelastic losses at the universal rate.
This thesis reports one of the most accurate measurement of a molecule's vibrational transition frequency to date, which may potentially serve as a secondary representation of the SI unit of time in the terahertz (THz) band where standards are scarce. The prototypical molecular clock lays the important groundwork for future explorations into THz metrology, quantum chemistry, and fundamental interactions at atomic length scales.
| Identifer | oai:union.ndltd.org:columbia.edu/oai:academiccommons.columbia.edu:10.7916/q16t-2g67 |
| Date | January 2023 |
| Creators | Leung, Kon H. |
| Source Sets | Columbia University |
| Language | English |
| Detected Language | English |
| Type | Theses |
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