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We report a generally applicable computational and experimental approach to determine vibronic branching ratios in linear polyatomic molecules to the $10^{-5}$ level, including for nominally symmetry forbidden transitions. These methods are…

Laser cooling of large, complex molecules is a long-standing goal, instrumental for enabling new quantum technology and precision measurements. A primary consideration for the feasibility of laser cooling, which determines the efficiency…

The vibrational branching ratios from the lowest excited electronic state for $\textrm{SrOCH}_3$, $\textrm{SrNH}_2$, and $\textrm{SrSH}$ are measured at the $< 0.1\%$ level. Spectra are obtained by driving the $\tilde{X} - \tilde{A}$…

Atomic Physics · Physics 2025-10-07 Alexander Frenett , Zack Lasner , Lan Cheng , John M. Doyle

Alkaline earth monoalkoxide free radicals (MORs) have molecular properties conducive to direct laser cooling to sub-millikelvin temperatures. Using dispersed laser induced fluorescence (DLIF) measurements from a pulsed supersonic molecular…

Atomic Physics · Physics 2019-05-22 Ivan Kozyryev , Timothy C. Steimle , Phelan Yu , Duc-Trung Nguyen , John M. Doyle

We propose a method of stimulated laser cooling of diatomic molecules by counter-propagating $\pi$-trains of ultrashort laser pulses. The cooling cycles occur on the rovibrational transitions inside the same ground electronic manifold, thus…

Atomic Physics · Physics 2015-03-13 Ekaterina Ilinova , Jonathan Weinstein , Andrei Derevianko

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…

The vibrational branching ratios of SrOH for radiative decay to the ground electronic state, $X^{2}\Sigma^{+}$, from the first two electronically excited states, $A^{2}\Pi$ and $B^{2}\Sigma^{+}$, are determined experimentally at the…

Atomic Physics · Physics 2022-08-17 Zack Lasner , Annika Lunstad , Chaoqun Zhang , Lan Cheng , John M. Doyle

The direct laser cooling of neutral diatomic molecules in molecular beams suggests that trapped molecular ions can also be laser cooled. The long storage time and spatial localization of trapped molecular ions provides the opportunity for…

The ability of laser cooling for relativistic ion beams is investigated. For this purpose, the excitation of relativistic ions with a continuous wave and a pulsed laser is analyzed, utilizing the optical Bloch equations. The laser cooling…

Accelerator Physics · Physics 2018-03-14 Lewin Eidam , Oliver Boine-Frankenheim , Danyal Winters

The LiFr diatomic represents a promising candidate for indirect laser cooling that has not yet been investigated not theoretically or experimentally. The potential energy curves of the ground and low_lying excited states of the LiFr…

Atomic Physics · Physics 2023-12-29 Maksim Shundalau , Patrizia Lamberti

We propose and demonstrate a novel laser cooling mechanism applicable to particles with narrow-linewidth optical transitions. By sweeping the frequency of counter-propagating laser beams in a sawtooth manner, we cause adiabatic transfer…

The extension of laser cooling and trapping techniques to polyatomic molecular ions would have advanced scientific applications such as search of physics outside of the Standard Model, ultracold chemistry etc. We apply the Fock space…

The simple structure of the BH molecule makes it an excellent candidate for direct laser cooling. We measure the branching ratios for the decay of the ${\rm A}^{1}\Pi (v'=0)$ state to vibrational levels of the ground state, ${\rm…

Atomic Physics · Physics 2014-08-06 R. J. Hendricks , D. A. Holland , S. Truppe , B. E. Sauer , M. R. Tarbutt

Recently a new wave of interest to spectroscopy of radioactive compounds has raised due to successful applications of the new experimental ISOL/CRIS technique to optical spectroscopy of radium monofluoride molecules. This opens great…

Chemical Physics · Physics 2022-10-19 Timur Isaev , Dmitrii Makinski , Andrei Zaitsevski

We investigate theoretically the application of tailored incoherent far-infrared fields in combination with laser excitation of a single rovibrational transition for rotational cooling of translationally cold polar diatomic molecules. The…

Atomic Physics · Physics 2009-11-10 I. S. Vogelius , L. B. Madsen , M. Drewsen

We provide a theoretical analysis for a recently demonstrated cooling method. Two-level particles undergo successive adiabatic transfers upon interaction with counter-propagating laser beams that are repeatedly swept over the transition…

We study nonadiabatic electron transfer within the biased spin-boson model. We calculate the incoherent transfer rate in analytic form at all temperatures for a power law form of the spectral density of the solvent coupling. In the Ohmic…

Statistical Mechanics · Physics 2009-10-31 G. Lang , E. Paladino , U. Weiss

We have recently demonstrated that optical pumping methods combined with photoassociation of ultra-cold atoms can produce ultra-cold and dense samples of molecules in their absolute rovibronic ground state. More generally, both the external…

Atomic Physics · Physics 2013-08-01 I. Manai , R. Horchani , M. Hamamda , A. Fioretti , M. Allegrini , H. Lignier , P. Pillet , D. Comparat

We study optical cycling in the polar free radical calcium monohydroxide (CaOH) and establish an experimental path towards scattering $\sim$$10^4$ photons. We report rovibronic branching ratio measurements with precision at the…

Recently a number of diatomic and polyatomics molecules has been identified as a prospective systems for Doppler/Sisyphus cooling. Doppler/Sisyphus cooling allows to decrease the kinetic energy of molecules down to microkelvin temperatures…

Chemical Physics · Physics 2017-11-22 T. A. Isaev , A. V. Zaitsevskii , E. Eliav
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