O(<sup>1</sup>D) + N<sub>2</sub>O Reaction: NO Vibrational and Rotational Distributions

Tokel, Onur; Chen, J.; Ulrich, Constantin; Houston, Paul L.

doi:10.1021/jp1042377

Cited by 6 publications

(3 citation statements)

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“…The mixture was supersonically expanded through the nozzle and collimated by a 0.5-mm diameter conical skimmer before entering the interaction region, defined as the region between a high-voltage repeller and an extractor electrode. One molecular beam of the dual-beam time-of-flight mass spectrometer apparatus , shown in Figure was used for the experiment. In the interaction region, the ozone was crossed perpendicularly by two lasers, one used for dissociation of ozone, and another for detection of O( 3 P 2 ).…”

Section: Methodsmentioning

confidence: 99%

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

et al. 2013

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Product imaging of O((3)P2) following dissociation of ozone has been used to determine the relative yields of the product channels O((3)P2) + O2(X (3)Σg(-)) of ozone. All three channels are prominent at all wavelengths investigated. O2 vibrational distributions for each channel and each wavelength are also estimated assuming Boltzmann rotational distributions. Averaged over wavelength in the measured range, the yields of the O((3)P2) + O2(X (3)Σg(-)), O((3)P2) + O2(a (1)Δg), and O((3)P2) + O2(b (1)Σg(+)) channels are 0.36, 0.31,and 0.34, respectively. Photofragment distributions in the spin-allowed channel O((3)P) + O2(X (3)Σg(-)) are compared with the results of quantum mechanical calculations on the vibronically coupled PESs of the singlet states B (optically bright) and R (repulsive). The experiments suggest that considerably more vibrational excitation and less rotational excitation occur than predicted by the quantum calculations. The rotational distributions, adjusted to fit the experimental images, suggest that the dissociation takes place from a more linear configuration than the Franck-Condon bending angle of 117°. The dissociation at most wavelengths results in a positive value of the anisotropy parameter, β, both in the experiment and in the calculations. Calculations indicate that both nonadiabatic transitions and intersystem crossings substantially reduce β below the nominal value of 2.

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Section: Methodsmentioning

confidence: 99%

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

et al. 2013

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“…The molecular beam/velocity-map ion-imaging apparatus has been described in detail elsewhere. , In brief, the apparatus consists of three collinear regions containing the pulsed molecular beam source, the main interaction chamber, and the detector. During operation the source is evacuated by a diffusion pump and the other regions are each evacuated by a turbomolecular pump.…”

Section: Methodsmentioning

confidence: 99%

Anomalous Intensities in the 2+1 REMPI Spectrum of the E ¹Π–X ¹Σ⁺ Transition of CO

et al. 2019

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We report on one-color experiments near 214 nm involving the photodissociation of jet-cooled OCS to produce high rotational states (40 < J < 80) of CO (X 1Σ+, v = 0, 1) which were then ionized by 2+1 resonance-enhanced multiphoton ionization via the E 1Π state. The nominally forbidden Q-branch of the two-photon E 1Π–X 1Σ+ transition is observed with intensity comparable to the allowed R-branch. The bright character of the high-J Q-branch lines can be described quantitatively as intensity borrowing due to mixing of the E 1Π and C 1Σ+ states, using J-dependent mixing coefficients extrapolated from the observed Λ-doubling in the lower rotational levels of the E state. In addition to the significant enhancement of Q-branch intensities above the values predicted by conventional two-photon line strengths for a 1Π–1Σ+ transition, the high-J lines of the R- and P-branches appear to be suppressed in intensity by approximately a factor of 3 compared to the unperturbed low-J line strengths, most likely due to perturbations associated with a 1Σ– state. The E-state rotational term values for J < 80, v = 0 derived from the present spectra agree within our measurement and calibration uncertainties with the extrapolations based on the molecular constants previously derived from rotational levels with J < 50. The E–X transition is attractive for future application to photodissociation dynamics and rotational polarization measurements of CO photofragments, with convenient access to state-selective probing on multiple rotational branches, which exhibit different sensitivity to fragment alignment.

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“…Fluxes of NO from early Earth volcanism are predicted to exceed those from the present Earth. An additional source of NO in the upper atmosphere is the insertion of O( 1 D) into N 2 O (N 2 O + O( 1 D) → 2NO). , O( 1 D) is the metastable (first excited) state of atomic oxygen. It has been evident from the experiment that the vacuum ultraviolet (VUV) photolysis of CO 2 can produce O( 1 D). , Another major source of early atmospheric O( 1 D) is believed as the self-reaction of OH • .…”

Section: Introductionmentioning

confidence: 99%

Theoretical Investigations on the Possibility of Prebiotic HCN Formation via O-Addition Reactions

2020

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Until now, reactions between methane photolysis products (CH 3 • , CH 2 ) and active N atom or reactive NO radical are proposed as routes of HCN formation in the prebiotic Earth. Scientists think that the reducing atmosphere of primitive Earth was made of H 2 , He, N 2 , NO, CH 4 , H 2 O, CO 2 , etc., and there was no molecular oxygen. However, it has been evident from experiments that the vacuum ultraviolet (VUV) photolysis of CO 2 can produce atomic oxygen. Therefore, it can be presumed that atomic oxygen was likely present in early Earth's atmosphere. Was there any impact of atomic oxygen in production of early atmospheric HCN for the emergence of life? To hunt for the answer, we have employed computational methods to study the mechanism and kinetics of CH 3 NO + O( 1 D) and CH 2 NO • + O( 3 P) addition reactions. Current study suggests that the addition of O( 1 D) into nitrosomethane (CH 3 NO) and the addition of O( 3 P) into nitrosomethylene radical (CH 2 NO • ) can efficiently produce HCN through an effectively barrierless pathway. At STP, Bartis−Widom phenomenological loss rate coefficients of O( 1 D) and O( 3 P) are obtained as 2.47 × 10 −12 and 4.67 × 10 −11 cm 3 molecule −1 s −1 , respectively. We propose that addition reactions of atomic oxygen with CH 3 NO and CH 2 NO • might act as a potential source for early atmospheric HCN.

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O(¹D) + N₂O Reaction: NO Vibrational and Rotational Distributions

Cited by 6 publications

References 46 publications

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

Anomalous Intensities in the 2+1 REMPI Spectrum of the E ¹Π–X ¹Σ⁺ Transition of CO

Theoretical Investigations on the Possibility of Prebiotic HCN Formation via O-Addition Reactions

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O(1D) + N2O Reaction: NO Vibrational and Rotational Distributions

Cited by 6 publications

References 46 publications

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(3P2) with O2(X 3Σg–), O2(a 1Δg) and O2(b 1Σg+)

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(3P2) with O2(X 3Σg–), O2(a 1Δg) and O2(b 1Σg+)

Anomalous Intensities in the 2+1 REMPI Spectrum of the E 1Π–X 1Σ+ Transition of CO

Theoretical Investigations on the Possibility of Prebiotic HCN Formation via O-Addition Reactions

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O(¹D) + N₂O Reaction: NO Vibrational and Rotational Distributions

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

Photodissociation of Ozone from 321 to 329 nm: The Relative Yields of O(³P₂) with O₂(X ³Σ_g^–), O₂(a ¹Δ_g) and O₂(b ¹Σ_g⁺)

Anomalous Intensities in the 2+1 REMPI Spectrum of the E ¹Π–X ¹Σ⁺ Transition of CO