Title :

Reassessing the potential of TlCl for laser cooling experiments via four-component correlated electronic structure calculations

Author(s) :

Yuan, Xiang [Auteur correspondant]
Physico-Chimie Moléculaire Théorique [PCMT]
Severo Pereira Gomes, Andre [Auteur correspondant]
Physico-Chimie Moléculaire Théorique [PCMT]

Journal title :

The Journal of Chemical Physics

Pages :

074313

Publisher :

American Institute of Physics

Publication date :

2022-08-19

ISSN :

0021-9606

English keyword(s) :

Laser cooling of molecules
Relativistic Effects
thallium fluoride
thallium chloride
equation of motion coupled cluster
multireference configuration interaction

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

The TlCl molecule has previously been investigated theoretically and proposed as promising candidates for laser cooling searches [X. Yuan et. al. J. Chem. Phys., 149, 094306, 2018]. From these results, the cooling process, ...
Show more >The TlCl molecule has previously been investigated theoretically and proposed as promising candidates for laser cooling searches [X. Yuan et. al. J. Chem. Phys., 149, 094306, 2018]. From these results, the cooling process, which would proceed by transitions between a³Π⁺₀ and X¹Σ⁺₀ states, had as potential bottleneck the long lifetime (6.04 µs) of the excited state a³Π⁺₀, that would prohibit experimentally control the slowing region. Here, we revisit this system by employing four-component Multireference Configuration Interaction (MRCI) calculations and investigate the effect of such approaches on the calculated transition moments between a³Π⁺₀ and a³Π₁ excited states of TlCl as well as TlF, the latter serving as a benchmark between theory and experiment. Wherever possible, MRCI results have been cross-validated by, and turned out to be consistent with, four-component equation of motion coupled-cluster (EOM-CC) and polarization propagator (PP) calculations. We find that the results of TlF are very closed to experiment values, while for TlCl the lifetime of the a³Π⁺₀ state is now estimated to be 175 ns, which is much shorter than previous calculations indicated, thus yielding a different, more favorable cooling dynamics. By solving the rate-equation numerically, we provide evidence that TlCl could have cooling properties similar to those of TlF. Our investigations also point to the potential benefits of enhancing the stimulated radiation in optical cycle to improve cooling efficiency.Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

Calcul de la diffusion inélastique résonante de rayons X pour toute la classification périodique
Physiques et Chimie de l'Environnement Atmosphérique
ULNE

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL