Probing the limits of optical cycling in a predissociative diatomic molecule

Molecular predissociation is the spontaneous, nonradiative bond breaking process that can occur upon excitation. In the context of laser cooling, predissociation is an unwanted consequence of molecular structure that limits the ability to scatter a large number of photons required to reach the ultra...

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Bibliographic Details
Published in:arXiv.org 2023-10
Main Authors: Sun, Qi, Dickerson, Claire E, Dai, Jinyu, Pope, Isaac M, Cheng, Lan, Neuhauser, Daniel, Alexandrova, Anastassia N, Mitra, Debayan, Zelevinsky, Tanya
Format: Article
Language:English
Subjects:
Cooling
Fragments
Kinetic energy
Laser cooling
Lasers
Molecular structure
Photons
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Summary:Molecular predissociation is the spontaneous, nonradiative bond breaking process that can occur upon excitation. In the context of laser cooling, predissociation is an unwanted consequence of molecular structure that limits the ability to scatter a large number of photons required to reach the ultracold regime. Unlike rovibrational branching, predissociation is irreversible since the fragments fly apart with high kinetic energy. Of particular interest is the simple diatomic molecule, CaH, for which the two lowest electronically excited states used in laser cooling lie above the dissociation threshold of the ground potential. In this work, we present measurements and calculations that quantify the predissociation probabilities affecting the cooling cycle. The results allow us to design a laser cooling scheme that will enable the creation of an ultracold and optically trapped cloud of CaH molecules. In addition, we use the results to propose a two-photon pathway to controlled dissociation of the molecules, in order to gain access to their ultracold fragments, including hydrogen.
ISSN:2331-8422
DOI:10.48550/arxiv.2306.01184