Author:

Keywords:

Science & Technology, Physical Sciences, Chemistry, Physical, Physics, Atomic, Molecular & Chemical, Chemistry, Physics, LYING ELECTRONIC STATES, AB-INITIO CALCULATIONS, MULTIREFERENCE CONFIGURATION-INTERACTION, UV PHOTOELECTRON-SPECTRUM, COUPLED-CLUSTER METHOD, TRANSITION-PROBABILITIES, VIBRATIONAL ANALYSIS, RATIONAL DESIGN, BASIS-SETS, OPEN-SHELL, 02 Physical Sciences, 03 Chemical Sciences, 09 Engineering, Chemical Physics, 34 Chemical sciences, 40 Engineering, 51 Physical sciences

Abstract:

Optical cycling, a continuous photon scattering off atoms or molecules, plays a central role in the quantum information science. While optical cycling has been experimentally achieved for many neutral species, few molecular ions have been investigated. We present a systematic theoretical search for diatomic molecular ions suitable for optical cycling using equation-of-motion coupled-cluster methods. Inspired by the electronic structure patterns of laser-cooled neutral molecules, we establish the design principles for molecular ions and explore various possible cationic molecular frameworks. The results show that finding a perfect molecular ion for optical cycling is challenging, yet possible. Among various possible diatomic molecules we suggest several candidates, which require further attention from both theory and experiment: YF+, SiO+, PN+, SiBr+, and BO+.