Laser cooling of molecules by dynamically trapped states

Loïc Anderegg

Potential wide-ranging scientific applications, spanning fundamental physics to quantum engineering, has led to significant efforts in controlling molecules at the quantum level. The rich internal structure of molecules, that gives rise to these desirable properties also complicates the task of controlling such species. Over the past decade, our ability to produce, control, and detect molecules has advanced tremendously with direct laser-cooling and magneto-optical trapping of diatomic molecules realized by several groups around the world. In this thesis, we describe the creation of the first RF MOT of CaF, which at the time of the writing of this thesis, remains the largest and densest molecular MOT. New laser cooling techniques for molecules are demonstrated, allowing laser cooling of molecules to 4 uK, 50 times colder than the Doppler limit. Optical trapping of these molecules is also achieved, which, in combination with in-trap laser cooling increased the density of trapped molecules by five orders of magnitude compared to the density in the MOT. We developed methods to cool and detect single molecules with high fidelity, which aided us in the creation of an optical tweezer array of single, ultracold CaF molecules. The densities of molecules (10^12 cm^-3) attained inside the tweezer traps also enabled us to observe both light-assisted and ground state collisions of laser cooled molecules, for the first time. The phase space density within the merged tweezers reached 5x10^-4, 10 orders of magnitude larger than the initial MOT. We implemented internal quantum state control of the molecules and dynamical control of the tweezers to build a platform for exploring state-selective ultracold quantum chemistry.

Loïc Anderegg, Benjamin L. Augenbraun, Yicheng Bao +4 more

P. Pillet, Matthieu Viteau, Amodsen Chotia +5 more

Jason Nguyen, C. Ricardo Viteri, Edward G. Hohenstein +3 more

The direct laser cooling of neutral diatomic molecules in molecular beams suggests that trapped molecular ions can also be laser cooled.The long storage time and spatial localization of trapped molecular ions provides an opportunity for multi-step cooling strategies, but also requires careful consideration of rare molecular transitions.We briefly summarize the requirements that a diatomic molecule must meet for laser cooling, and we identify a few potential molecular ion candidates.We then carry out a detailed computational study of the candidates BH + and AlH + , including improved ab initio calculations of the electronic state potential energy surfaces and transition rates for rare dissociation events.On the basis of an analysis of the population dynamics, we determine which transitions must be addressed for laser cooling, and compare experimental schemes using continuous-wave and pulsed lasers.

Yukai Lu, Connor M. Holland, Lawrence W. Cheuk

Recent work with laser-cooled molecules in attractive optical traps has shown that the differential ac Stark shifts arising from the trap light itself can become problematic, limiting collisional shielding efficiencies, rotational coherence times, and laser-cooling temperatures. In this Letter, we explore trapping and laser cooling of CaF molecules in a ring-shaped repulsive optical trap. The observed dependences of loss rates on temperature and barrier height show characteristic behavior of repulsive traps and indicate strongly suppressed average ac Stark shifts. Within the trap, we find that Λ-enhanced gray molasses cooling is effective, producing similar minimum temperatures as those obtained in free space. By combining in-trap laser cooling with dynamical reshaping of the trap, we also present a method that allows highly efficient and rapid transfer from molecular magneto-optical traps into conventional attractive optical traps, which has been an outstanding challenge for experiments to date. Notably, our method could allow nearly lossless transfer over millisecond timescales.

Eunmi Chae