Prospects for laser cooling of polyatomic molecules with increasing complexity

Optical cycling transitions and direct laser cooling have recently been demonstrated for a number of alkaline-earth dimers and trimer molecules. This is made possible by diagonal Franck-Condon factors between the vibrational modes of the optical transition. Achieving a similar degree of cooling to m...

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Main Authors: Jacek Kłos, Svetlana Kotochigova
Format: Article
Language:English
Published: American Physical Society 2020-03-01
Series:Physical Review Research
Online Access:http://doi.org/10.1103/PhysRevResearch.2.013384
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author Jacek Kłos
Svetlana Kotochigova
author_facet Jacek Kłos
Svetlana Kotochigova
author_sort Jacek Kłos
collection DOAJ
description Optical cycling transitions and direct laser cooling have recently been demonstrated for a number of alkaline-earth dimers and trimer molecules. This is made possible by diagonal Franck-Condon factors between the vibrational modes of the optical transition. Achieving a similar degree of cooling to microkelvin equivalent kinetic energy for larger polyatomic molecules, however, remains challenging. Since polyatomic molecules are characterized by multiple degrees of freedom and have a correspondingly more complex structure, it is far from obvious whether there exist polyatomic molecules that can repeatedly scatter photons. Here, we propose chemical substitution approaches to engineer large polyatomic molecules with optical cycling centers (OCCs) containing alkaline-earth oxide dimers or acetylenic alkaline-earth trimers (i.e., M−C≡C) connected to (CH)_{n} chains or fullerenes. To validate the OCC-character of the selected molecules, we performed electronic structure calculations of the equilibrium configuration of both ground and excited potential energy surfaces, evaluated their vibrational and bending modes, and corresponding Franck-Condon factors for all but the most complex molecules. For fullerenes, we have shown that OCCs based on M−C≡C can perform better than those based on alkaline-earth oxide dimers. In addition, for heavier polyatomic molecules it might be advantageous to attach two OCCs, thereby potentially doubling the photon scattering rate and thus speeding up cooling rates.
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spelling doaj.art-fe6399b1f7ce4420bd68330e7b45c2402024-04-12T16:52:14ZengAmerican Physical SocietyPhysical Review Research2643-15642020-03-012101338410.1103/PhysRevResearch.2.013384Prospects for laser cooling of polyatomic molecules with increasing complexityJacek KłosSvetlana KotochigovaOptical cycling transitions and direct laser cooling have recently been demonstrated for a number of alkaline-earth dimers and trimer molecules. This is made possible by diagonal Franck-Condon factors between the vibrational modes of the optical transition. Achieving a similar degree of cooling to microkelvin equivalent kinetic energy for larger polyatomic molecules, however, remains challenging. Since polyatomic molecules are characterized by multiple degrees of freedom and have a correspondingly more complex structure, it is far from obvious whether there exist polyatomic molecules that can repeatedly scatter photons. Here, we propose chemical substitution approaches to engineer large polyatomic molecules with optical cycling centers (OCCs) containing alkaline-earth oxide dimers or acetylenic alkaline-earth trimers (i.e., M−C≡C) connected to (CH)_{n} chains or fullerenes. To validate the OCC-character of the selected molecules, we performed electronic structure calculations of the equilibrium configuration of both ground and excited potential energy surfaces, evaluated their vibrational and bending modes, and corresponding Franck-Condon factors for all but the most complex molecules. For fullerenes, we have shown that OCCs based on M−C≡C can perform better than those based on alkaline-earth oxide dimers. In addition, for heavier polyatomic molecules it might be advantageous to attach two OCCs, thereby potentially doubling the photon scattering rate and thus speeding up cooling rates.http://doi.org/10.1103/PhysRevResearch.2.013384
spellingShingle Jacek Kłos
Svetlana Kotochigova
Prospects for laser cooling of polyatomic molecules with increasing complexity
Physical Review Research
title Prospects for laser cooling of polyatomic molecules with increasing complexity
title_full Prospects for laser cooling of polyatomic molecules with increasing complexity
title_fullStr Prospects for laser cooling of polyatomic molecules with increasing complexity
title_full_unstemmed Prospects for laser cooling of polyatomic molecules with increasing complexity
title_short Prospects for laser cooling of polyatomic molecules with increasing complexity
title_sort prospects for laser cooling of polyatomic molecules with increasing complexity
url http://doi.org/10.1103/PhysRevResearch.2.013384
work_keys_str_mv AT jacekkłos prospectsforlasercoolingofpolyatomicmoleculeswithincreasingcomplexity
AT svetlanakotochigova prospectsforlasercoolingofpolyatomicmoleculeswithincreasingcomplexity