Optical spectra of calcium atoms in inert matrices

Andrews, Lester; Duley, W. W.; Brewer, Leo

doi:10.1016/0022-2852(78)90007-3

Cited by 41 publications

(11 citation statements)

References 20 publications

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“…Earlier thermal experiments also measured the strongest band at 556.0 cm -1 and the 44 Ca counterpart at 545.5 cm -1 . In these experiments the upper band was measured at 742.5 and 740.7 cm -1 for 40 Ca and 44 Ca, respectively, giving a 1.8 cm -1 shift. Likewise, the upper band was measured at 703.0 and 701.0 cm -1 for 40 Ca and 44 Ca with 18 O 2 giving a 2.0 cm -1 shift indicating a small amount of O-O and Ca-O 2 stretching mode mixing.…”

Section: Discussionmentioning

confidence: 80%

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules

et al. 1996

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Laser-ablated group 2 metal atoms have been reacted with O 2 in condensing N 2 to complement earlier Ar studies owing to different relaxation dynamics of N 2 and Ar with respect to excited metal atoms and ionic product molecules. In the case of Ca + O 2 , the reaction in condensing Ar gives primarily the 3 B 2 open bent OCaO dioxide product, but the reaction in condensing N 2 favors the 1 A 1 cyclic CaO 2 peroxide species. Three fundamentals are observed with 18 O and 44 Ca substitution for CaO 2 , and isotopic frequencies are in excellent agreement with the predictions of quantum chemical calculations. Although DFT/B3LYP frequencies are slightly higher than MP2 and CASSCF values, a similar pattern is calculated. Ionic molecules interact more strongly with a nitrogen matrix than with argon, and calculations of N 2 MO x and ArMO x molecules can be used to explain matrix shifts. Several N 2 MO 2 species are formed spontaneously from MO 2 molecules in solid nitrogen, and a match is found for observed matrix and DFT calculated isotopic frequencies. By comparison, the new molecule ArBeO 2 is identified in earlier argon matrix experiments. The new metal disuperoxide molecules, O 2 MO 2 , are also identified here. Calcium disuperoxide, O 2 CaO 2 , is characterized as a D 2d species with +1.12 charge on Ca and -0.28 on each O, in contrast to calcium peroxide, CaO 2 , a C 2V molecule with +1.05 charge on Ca and -0.525 on each oxygen atom.

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Section: Discussionmentioning

confidence: 80%

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules

et al. 1996

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“…IIIB above, it might be possible to further enhance the steady-state Fano coherence (and hence the fluorescence difference signal) by inducing moderate decoherence between the excited states of the calcium atoms. This could be achieved experimentally by, e.g, adding magnetic field noise or isolating the atoms in a rare-gas host matrix [43,44].…”

Section: Experimental Detection Of Steady-state Fano Coherencementioning

confidence: 99%

Steady-state Fano coherences in a V-type system driven by polarized incoherent light

Koyu,

Dodin,

Brumer

et al. 2020

Preprint

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We explore the properties of steady-state Fano coherences generated in a three-level V-system continuously pumped by polarized incoherent light in the absence of coherent driving. By solving the nonsecular Bloch-Redfield quantum master equation we obtain the ratio of the stationary coherences to excited-state populations, C = (1 + ∆ 2 γ(r+γ) ) −1 , which quantifies the impact of steadystate coherences on excited-state dynamical observables of the V-system. The ratio is maximized when the excited-state splitting ∆ is small compared to either the spontaneous decay rate γ or the incoherent pumping rate r. We demonstrate that while the detrimental effects of a strongly decohering environment generally suppress the coherence-to-population ratio by the factor γ d /γ, an intriguing regime exists where the C ratio displays a maximum as a function of the dephasing rate γ d . We attribute the surprising dephasing-induced enhancement of stationary Fano coherences to the environmental suppression of destructive interference of individual incoherent excitations generated at different times. We further clarify the physical basis for the steady-state Fano coherence, whose imaginary part is identified with the non-equilibrium flux across a pair of qubits coupled to two independent thermal baths, unraveling a direct connection between the seemingly unrelated phenomena of incoherent driving of multilevel quantum systems and non-equilibrium quantum transport in qubit networks. The real part of the steady-state Fano coherence is found to be proportional to the deviation of excited-state populations from their values in thermodynamic equilibrium, making it possible to observe signatures of steady-state Fano coherences in excitedstate populations. Finally, we put forward an experimental proposal for observing steady-state Fano coherences by detecting the total fluorescence signal emitted by Calcium atoms excited by polarized vs. isotropic incoherent light. Our analysis paves the way toward further theoretical and experimental studies of non-equilibrium coherent steady states in thermally driven atomic and molecular systems, and for the exploration of their potential role in biological processes.

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“…This effect has been observed in absorption 19 and excitation 20 work and is thought to arise from metal atom occupancy in low-symmetry sites. It has also been noted that the matrix shifts on the 3d 1 D 2 ←4s 1 S 0 transition are much smaller than on the corresponding 4p 1 P 1 ←4s 1 S 0 transition and, as expected, the absorption strengths of the former transition are about two orders of magnitude less than the fully allowed 1 P 1 ← 1 S 0 transition.…”

Section: Discussionmentioning

confidence: 80%

A synchrotron radiation study of high-lying excited states of matrix-isolated atomic magnesium

Kerins

Healy

McCaffrey

2000

Low Temperature Physics

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Previous steady-state and time-resolved luminescence spectroscopy of 3p 1 P 1 atomic magnesium, isolated in thin film samples of the solid rare gases, is extended to include the higher energy 4p 1 P 1 excitation. Well-resolved site splittings are recorded in Mg/Ar samples for excitation to the 4p 1 P 1 level. A small red shift in the absorption energy to the 4p 1 P 1 level for Mg/Ar contrasts with a small blue shift on absorption to the 3p 1 P 1 level. Direct emission from the 4p 1 P 1 level is not observed in any of the rare gas matrices; instead, intense emission from the low energy 3p 1 P 1 level is. Measurements of the emission decay curves in Mg/Ar have revealed slow rates in the steps feeding the 3p 1 P 1 level following 4p 1 P 1 excitation. The reason for the differential shifting of the 4p 1 P 1 and 3p 1 P 1 levels as well as the lack of direct 4p 1 P 1 emission is thought to be related to the strong binding interaction between Mg in the 4p 1 P 1 state and the rare gases.

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Optical spectra of calcium atoms in inert matrices

Cited by 41 publications

References 20 publications

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules

Steady-state Fano coherences in a V-type system driven by polarized incoherent light

A synchrotron radiation study of high-lying excited states of matrix-isolated atomic magnesium

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Optical spectra of calcium atoms in inert matrices

Cited by 41 publications

References 20 publications

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO2, O2MO2, and Related Molecules

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO2, O2MO2, and Related Molecules

Steady-state Fano coherences in a V-type system driven by polarized incoherent light

A synchrotron radiation study of high-lying excited states of matrix-isolated atomic magnesium

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Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules

Infrared Spectra and Quantum Chemical Calculations of Group 2 MO₂, O₂MO₂, and Related Molecules