A combined experimental and computational study on the transition of the calcium isopropoxide radical as a candidate for direct laser cooling

Telfah, Hamzeh; Sharma, Ketan; Paul, Anam C.; Riyadh, S. M. Shah; Miller, Terry A.; Liu, Jinjun

doi:10.1039/d1cp04107j

Cited by 3 publications

(3 citation statements)

References 93 publications

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“…Although the FCF for CaO−adamantane (0.908) is worse than a those of M−O−Rs with certain smaller ligands, such as phenyl (0.933 41 ), the transition is not destroyed by adding a larger ligand. In fact, it has a better FCF than smaller molecules, such as CaOC 2 H 5 (<0.90 52 ) and CaOCH(CH 3 ) 2 (0.720 53 ), despite an increase in the number of vibrational modes.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Fully Saturated Hydrocarbons as Hosts of Optical Cycling Centers

et al. 2022

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Designing closed, laser-induced optical cycling transitions in trapped atoms or molecules is useful for quantum information processing, precision measurement, and quantum sensing. Larger molecules that feature such closed transitions are particularly desirable, as the increased degrees of freedom present new structures for optical control and enhanced measurements. The search for molecules with robust optical cycling centers is a challenge which requires design principles beyond trial-and-error. Two such principles are proposed for the particular M−O−R framework, where M is an alkaline earth metal radical, and R is a ligand: (1) Large, saturated hydrocarbons can serve as ligands, R, due to a substantial HOMO−LUMO gap that encloses the cycling transition, so long as the R group is rigid. (2) Electron-withdrawing groups, via induction, can enhance Franck−Condon factors (FCFs) of the optical cycling transition, as long as they do not disturb the locally linear structure in the M−O−R motif. With these tools in mind, larger molecules can be trapped and used as optical cycling centers, sometimes with higher FCFs than smaller molecules.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Fully Saturated Hydrocarbons as Hosts of Optical Cycling Centers

et al. 2022

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“…In this case it was the interest in laser cooling of molecules, like the metal hydroxides and alkoxides, to milli-and micro-Kelvin temperatures, for fundamental physics experiments and possible applications as quantum information devices. This interest prompted spectroscopic studies of the Ã2 E − X2 A 1 electronic transition in calcium methoxide [28], the Ã1 2 A ′′ / Ã2 2 A ′ − X2 A ′ transition in calcium ethoxide [29] and the Ã1 2 A ′ / Ã2 2 A ′′ − X2 A ′ transition in calcium isopropoxide [30]. The quite large number of vibrational modes in these molecules made it necessary to improve the efficiency of the construction of the H matrix and minimize its storage requirements.…”

Section: Introductionmentioning

confidence: 99%

Molecules with Spin and Vibronic Coupling Effects: A Computational Perspective

Sharma,

Vasilyev,

Miller

et al. 2024

J. Phys.: Conf. Ser.

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While fundamental to molecular quantum mechanics, limitations of the Born-Oppenheimer Approximation (BOA) have long been known. Nonetheless, calculations that include molecular interactions, such as vibronic coupling and electron spin effects, that violate the BOA have remained a challenge due to their large demand on computational resources. The purpose of this paper is to describe two complementary software programs, SOCJT and XSIM, designed for efficient calculations that include these interactions. The programs are sufficiently general and user friendly that they can be readily applied to a variety of molecules of different symmetries, state degeneracies, and interaction strengths. The programs can typically produce spin-vibronic eigenvalues and eigenvectors with sufficient accuracy for the analysis and interpretation of molecular spectra with features attributable to violations of the BOA. The two programs utilize different matrix representations of the molecular Hamiltonian, with XSIM being Cartesian based and SOCJT being cylindrically based, and their advantages/disadvantages are discussed. Several algorithms can be chosen to obtain the Hamiltonian’s eigenvalues and eigenvectors and their speed and memory usage are compared. Examples of application of SOCJT and XSIM to explain spectral observations for particular molecules are briefly reviewed.

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“…Functionalizing large molecules with optical cycling centers (OCCs) is being explored as a means for extending the exquisite control available in quantum information science to the chemical domain. − Success requires that these OCCs absorb and emit many photons without changing their vibrational states. To accomplish this task, molecular design rules are being developed, aided and validated by experiments, to guide the creation of the ideal quantum functional groups. − For example, prior work has demonstrated that alkaline earth alkoxides provide a general and versatile chemical moiety for optical cycling applications, as the alkaline earth radical electron can be excited without perturbing the vibrational structure of the molecule. ,,− Similarly, traditional physical organic principles, such as electron-withdrawing, have been shown to improve OCCs performance. , Further, experimental and theoretical extensions to more complex acenes, , diamondoids, and even surfaces suggest an exciting path forward for creating increasingly complex and functional quantum systems.…”

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confidence: 99%

Extending the Large Molecule Limit: The Role of Fermi Resonance in Developing a Quantum Functional Group

Zhu,

Lao,

Dickerson

et al. 2024

J. Phys. Chem. Lett.

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Polyatomic molecules equipped with optical cycling centers (OCCs), enabling continuous photon scattering during optical excitation, are exciting candidates for advancing quantum information science. However, as these molecules grow in size and complexity, the interplay of complex vibronic couplings on optical cycling becomes a critical but relatively unexplored consideration. Here, we present an extensive exploration of Fermi resonances in large-scale OCCcontaining molecules using high-resolution dispersed laser-induced fluorescence and excitation spectroscopy. These resonances manifest as vibrational coupling leading to intensity borrowing by combination bands near optically active harmonic bands, which require additional repumping lasers for effective optical cycling. To mitigate these effects, we explore altering the vibrational energy level spacing through substitutions on the phenyl ring or changes in the OCC itself. While the complete elimination of vibrational coupling in complex molecules remains challenging, our findings highlight significant mitigation possibilities, opening new avenues for optimizing optical cycling in large polyatomic molecules.

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A combined experimental and computational study on the transition of the calcium isopropoxide radical as a candidate for direct laser cooling

Abstract: Vibronically resolved laser-induced fluorescence/dispersed fluorescence (LIF/DF) and cavity ring-down (CRD) spectra of the (A_1 ) ̃(_^2)A^'/ (A_2 ) ̃(_^2)A^''-X ̃(_^2)A^' electronic transition of the calcium isopropoxide [CaOCH(CH3)2] radical have been...

Cited by 3 publications

References 93 publications

Fully Saturated Hydrocarbons as Hosts of Optical Cycling Centers

Fully Saturated Hydrocarbons as Hosts of Optical Cycling Centers

Molecules with Spin and Vibronic Coupling Effects: A Computational Perspective

Extending the Large Molecule Limit: The Role of Fermi Resonance in Developing a Quantum Functional Group

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