Dispersed-fluorescence spectroscopy of jet-cooled calcium ethoxide radical (CaOC2H5)

Paul, Anam C.; Reza, Md. Asmaul; Liu, Jinjun

doi:10.1016/j.jms.2016.09.001

Cited by 14 publications

(15 citation statements)

References 16 publications

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“…A natural chiral candidate for laser cooling is a chiral analog of calcium monomethoxide, CaOCHDT. A recent theoretical and experimental work by Liu and coworkers [66] on calcium ethoxide (CaOC 2 H 5 ) confirms that Ca-O stretching mode is the dominant vibrational loss channel for this molecule and indicates its potential suitability for optical cycling and laser cooling using a scheme outlined here for ARMs.…”

Section: Beyond Symmetric Top Moleculesmentioning

confidence: 82%

Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping

Kozyryev

Steimle

et al. 2019

New J. Phys.

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Alkaline earth monoalkoxide free radicals (MORs) have molecular properties conducive to direct laser cooling to sub-millikelvin temperatures. Using dispersed laser induced fluorescence measurements from a pulsed supersonic molecular beam source we determine vibrational branching ratios and Franck-Condon factors for the MORs CaOH and CaOCH 3 . With narrow linewidth continuous-wave dye laser excitation, we precisely measure fluorescence branching for both X Ã -˜and X B -˜electronic systems in each molecule. Weak symmetry-forbidden decays to excited bending states with non-zero vibrational angular momentum are observed. Normal mode theoretical analysis combined with ab initio structural calculations are performed and compared to experimental results. Our measurements and analysis pave the way for direct laser cooling of these (and other) complex nonlinear polyatomic molecules. We also describe a possible approach to laser cooling and trapping of molecules with fewer symmetries like chiral species.

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Section: Beyond Symmetric Top Moleculesmentioning

confidence: 82%

Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping

Kozyryev

Steimle

et al. 2019

New J. Phys.

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“…Correlation of molecular constants can be removed when both of the two coupled electronic states are accessed with rotational and fine-structure resolution. In laser spectroscopy, this is easy to realize when both states are electronic excited states, such as in the case of alkyl-substituted organometallic monomethyl and monomethoxide radicals, [79][80][81][82][83][84][85][86] e.g., CaCH2CH3, CaCH(CH3)2, CaOCH2CH3, and CaOCH(CH3)2. Experimentally obtained high-resolution laser spectra of these molecules and their analysis with the present spectroscopic model would provide valuable information about SO and vibronic interactions, as well as related effects in free radicals.…”

Section: Discussionmentioning

confidence: 99%

Rotational and fine structure of open-shell molecules in nearly degenerate electronic states

Liu

2018

The Journal of Chemical Physics

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An effective Hamiltonian without symmetry restriction has been developed to model the rotational and fine structure of two nearly degenerate electronic states of an open-shell molecule. In addition to the rotational Hamiltonian for an asymmetric top, this spectroscopic model includes the energy separation between the two states due to difference potential and zero-point energy difference, as well as the spin-orbit (SO), Coriolis, and electron spin-molecular rotation (SR) interactions. Hamiltonian matrices are computed using orbitally and fully symmetrized case (a) and case (b) basis sets. Intensity formulae and selection rules for rotational transitions between a pair of nearly degenerate states and a nondegenerate state have also been derived using all four basis sets. It is demonstrated using real examples of free radicals that the fine structure of a single electronic state can be simulated with either a SR tensor or a combination of SO and Coriolis constants. The related molecular constants can be determined precisely only when all interacting levels are simulated simultaneously. The present study suggests that analysis of rotational and fine structure can provide quantitative insights into vibronic interactions and related effects.

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“…Such species include (see Fig. 2): AE monoamides (MNH 2 ) [46][47][48][49][50][51][52][53], hydrosulfides (MSH) [54][55][56][57][58], monoethoxides (MOC 2 H 5 ) [59], pyrollyls (MC 4 H 4 N) [60], methylpentadienyls (MC 5 H 4 CH 3 ) [60-62], methanethiols (MSCH 3 ) [63], alkylamides (MNHCH 3 ) [64], and isopropoxides (MOCH(CH 3 ) 2 ) [65], where M = Mg, Ca, Sr, or Ba. 4 Chiral-substituted AE-methyls (MCHDT) [66][67][68] and AE-methoxides (MOCHDT) [69] are also considered because the chiral methyl group will cause the three moments of inertia to differ.…”

Section: Achieving Photon Cyclingmentioning

confidence: 99%

Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules

Augenbraun,

Doyle,

Zelevinsky

et al. 2020

Preprint

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We present a practical roadmap to achieve optical cycling and laser cooling of asymmetric top molecules (ATMs). Our theoretical analysis describes how reduced molecular symmetry, as compared to diatomic and symmetric non-linear molecules, plays a role in photon scattering. We present methods to circumvent limitations on rapid photon cycling in these systems. We calculate vibrational branching ratios for a diverse set of asymmetric top molecules and find that many species within a broad class of molecules can be effectively cooled with a manageable number of lasers. We also describe methods to achieve rotationally closed optical cycles in ATMs. Despite significant structural complexity, laser cooling can be made effective using extensions of the current techniques used for linear molecules. Potential scientific impacts of laser-cooled ATMs span frontiers in controlled chemistry, quantum simulation, and searches for physics beyond the Standard Model.

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Dispersed-fluorescence spectroscopy of jet-cooled calcium ethoxide radical (CaOC2H5)

Cited by 14 publications

References 16 publications

Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping

Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping

Rotational and fine structure of open-shell molecules in nearly degenerate electronic states

Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules

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Dispersed-fluorescence spectroscopy of jet-cooled calcium ethoxide radical (CaOC2H5)

Cited by 14 publications

References 16 publications

Determination of CaOH and CaOCH3 vibrational branching ratios for direct laser cooling and trapping

Determination of CaOH and CaOCH3 vibrational branching ratios for direct laser cooling and trapping

Rotational and fine structure of open-shell molecules in nearly degenerate electronic states

Molecular Asymmetry and Optical Cycling: Laser Cooling Asymmetric Top Molecules

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Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping

Determination of CaOH and CaOCH₃ vibrational branching ratios for direct laser cooling and trapping