Spectroscopy and Photochemistry of Polyatomic Alkaline Earth Containing Molecules

Bernath, P. F.

doi:10.1002/9780470133545.ch1

Cited by 44 publications

(15 citation statements)

References 133 publications

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“…While we have restricted our measurements to YbOH, it is likely that this method can be used to enhance CBGB production of many interesting species, both diatomic and polyatomic. The chemical similarity of Yb with alkaline-earth atoms, and the success of excited state chemical reactions producing a variety of Ca-, Sr-, and Ba-molecules with numerous ligands [29,33,34], suggests that CBGBs of alkaline-earth atoms with monovalent and ionic bonds (conveniently, those which can be generically laser cooled [70]) could benefit from this approach. Note, however, that the power requirements become higher for lighter species, since the radiative width of the metastable states arises from spin-orbit coupling, which is larger in heavier species [71].…”

Section: Discussionmentioning

confidence: 99%

“…In addition to modifying chemical yield, excited state chemistry has been used to study the collisional physics of atoms and molecules. In the case of atoms isoelectronic to Yb, such as Ca, Sr, Ba, and Hg, excitation of reactants to metastable states was used for molecular spectroscopy [28,29] and investigations of reactions in ovens or beams with gases such as SF 6 [19,30], H 2 [30,31] [35,36], alcohols [19,32,34], halogens [19,30], halogenated alkanes [19,31,[37][38][39], and hydrogen halides [19,30,37,40,41]. More recently, the ability to trap and cool species to ultracold temperatures has enabled research of reaction dynamics between excited ions, atoms, and molecules [27,[42][43][44].…”

Section: Introductionmentioning

confidence: 99%

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Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

et al. 2020

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We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable 3 P 1 state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb( 3 P) with the reactants H 2 O and H 2 O 2 . More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

et al. 2020

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“…One successful strategy of designing a laser-coolable molecule is to attach an alkaline earth metal (such as calcium or strontium) to a ligand that withdraws one of the two valence electrons of the metal creating a strong ionic bond. [28][29][30][31][32] The second electron remains localized at the metal, both in the ground and in the excited states, giving rise to highly diagonal FCFs and thereby closed cycling transitions, if an appropriate number of repump lasers is introduced. The ability to exploit highly localized excitation for optical cycling of such triatomic molecules as CaOH, SrOH, and YbOH spur an interest in studying optical cycling schemes in more complex polyatomic molecules.…”

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confidence: 99%

Toward Ultracold Organic Chemistry: Prospects of Laser Cooling Large Organic Molecules

Ivanov

Bangerter

Wójcik

et al. 2020

J. Phys. Chem. Lett.

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Ultracold organic chemistry enables studies of reaction dynamics and mechanisms in quantum regime. Access to ultracold molecules hinges on the ability to efficiently scatter multiple photons via quasi-closed cycling transitions and, in practice, is complicated by the complex electronic structure of polyatomic molecules. Using equation-of-motion coupled-cluster (EOM-CC) calculations, we demonstrate that an alkaline earth metal attached to various aromatic ligands (such as benzene, phenol, cyclopentadienyl and pyrrolide) feature nearly-closed cycling transitions with only a few additional repump lasers. We also show that aromatic ligands such as benzene can accommodate multiple cycling centers in various geometrical configurations and may open new avenues in quantum information science, precision measurements, and ultracold chemistry. File list (2) download file view on ChemRxiv cooling_large.pdf (10.42 MiB) download file view on ChemRxiv si.pdf (1.48 MiB)

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“…Various monovalent derivatives of alkaline earth metals have been investigated using highresolution spectroscopy and ab initio calculations [70][71][72][73][74] . Among previously investigated systems, M-F and M-OH species have been studied in the greatest detail.…”

Section: A Electronic Structure Of Alkaline Earth Metal Derivativesmentioning

confidence: 99%

Towards a Rational Design of Laser-Coolable Molecules: Insights from Equation-of-Motion Coupled-Cluster Calculations

Ivanov

Bangerter²,

Krylov³

2019

Preprint

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Access to cold molecules is critical for quantum information science, design of new sensors, ultracold chemistry, and search of new phenomena. These applications depend on the ability to laser-cool molecules. Theory and qualitative models can play a central role in narrowing down the vast pool of potential candidates amenable to laser cooling. We report a systematic study of structural and optical properties of alkaline earth metal derivatives in the context of their applicability in laser cooling using equation-of-motion coupled-cluster methods. To rationalize and generalize the results from high-level electronic structure calculations, we develop an effective Hamiltonian model. The model explains the observed trends and suggests new principles for the design of laser-coolable molecules.

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Spectroscopy and Photochemistry of Polyatomic Alkaline Earth Containing Molecules

Cited by 44 publications

References 133 publications

Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

Enhanced molecular yield from a cryogenic buffer gas beam source via excited state chemistry

Toward Ultracold Organic Chemistry: Prospects of Laser Cooling Large Organic Molecules

Towards a Rational Design of Laser-Coolable Molecules: Insights from Equation-of-Motion Coupled-Cluster Calculations

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