Optical pumping of molecules provides unique opportunities for control of chemical
reactions at a wide range of rotational energies. This work reports a chemical reaction with …

The extraordinary success in laser cooling, trapping, and coherent manipulation of atoms
has energized the efforts in extending this exquisite control to molecules. Not only are …

Understanding molecular state evolution is central to many disciplines, including molecular
dynamics, precision measurement, and molecule-based quantum technology. Details of this …

We propose a general technique to produce cold spin-polarized molecules in the electronic
states of Σ symmetry, in which rotationally excited levels are first populated by coherent …

Fast and efficient state preparation of molecules can be accomplished by optical pumping.
Molecular structure that most obviously facilitates cycling involves a strong electronic …

Optical centrifuges are laser-based molecular traps that can rotationally accelerate
molecules to energies rivalling or exceeding molecular bond energies. Here we report time …

The electronic, laser-induced fluorescence spectrum of the B 2 Σ+← X 2 Σ+ transition in 28
Si 16 O+ and 29 Si 16 O+ has been recorded in a cryogenic buffer gas cell at≈ 100 K …

Laser cooling of translational motion of small molecules is performed by addressing
transitions that ensure spontaneous emission cannot cause net rotational excitation. This …

As demonstrated in our previous work [J. Chem. Phys. 149, 174109 (2018)], the kinetic
energy imparted to a quantum rotor by a non-resonant electromagnetic pulse with a …

Ultracold molecules are instrumental in many fields of physics, such as high-resolution
spectroscopy, quantum computation, and cold controlled chemistry. In this dissertation, we …