State-to-state photodynamics of nitrous oxide and the effect of long-range interaction on the alignment of O(1D2)

Teule, J.M.; Groenenboom, Gerrit C.; Neyer, David W.; Chandler, David W.; Janssen, Maurice H. M.

doi:10.1016/s0009-2614(00)00220-7

Cited by 59 publications

(37 citation statements)

References 26 publications

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“…18,19,22 We observe both atomic orbital alignment for the O( 1 D) photofragment and a non-limiting β value for N 2 (v = 0, J), on average ∼0.7 for J's between 60 and 80, in agreement with previous results. Recent calculations predict that over 97% of the absorption at 204 nm involves excitation to the 2 1 A' state, i.e., a parallel transition, which means the dipole moment lies in the plane of the molecule.…”

Section: Analysis and Discussionsupporting

confidence: 91%

“…As observed previously, [14][15][16][17][18][19][20][21][22] Since the corresponding sibling N 2 (J) photofragments do not show this effect, e.g., in Fig. 6 the angular distribution is maximum at θ = 0 o , this has been attributed to a preferential alignment of the O( 1 D 2 ) atomic orbital with respect to the recoil velocity.…”

Section: O( 1 D) Imagessupporting

confidence: 68%

“…Comparison of the angular distributions for RT and hot nozzles, shown in Fig. 6, indicate no change in the β value, i.e., β does not depend on v 2 , 19 which means that angular distributions are essentially governed by the excited state dynamics. These results, i.e., both the β(J) variation and the tail in the KER spectrum, seem to at least be in very good qualitative agreement with the conclusions of McBane et al…”

Section: Analysis and Discussionmentioning

confidence: 90%

“…This raises the possibility that a second type of photodissociation dynamics is responsible for the low energy tail. The angular distributions for the slow region, i.e., N 2 (J > 83), changes dramatically from positive anisotropy parameters (β) for N 2 (J < 83) to nearly zero, 18,19,22 providing further evidence that the photodissociation dynamics mechanism in this part of the KER spectrum could be different.…”

Section: Analysis and Discussionmentioning

confidence: 94%

“…Also due to the large change in NNO angle upon photoexcitation, N 2 photoproducts are formed with a large amount of rotational excitation (60 < J < 80). In recent years N 2 O has been subject to a number of high resolution experiments [13][14][15][16] using VMI, [17][18][19][20][21][22] as well as high level theoretical calculations. [23][24][25][26][27][28][29][30][31][32] In the most recent VMI study of Suzuki and coworkers, 22 the authors ionized individual rotational states of the N 2 photoproduct.…”

Section: Introductionmentioning

confidence: 99%

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Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle

Harding

Neugebohren

Grütter

et al. 2014

The Journal of Chemical Physics

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Laser initiated reactions in N2O clusters studied by time-sliced ion velocity imaging technique J. Chem. Phys. 139, 044307 (2013) We present a new photo-fragment imaging spectrometer, which employs a movable repeller in a single field imaging geometry. This innovation offers two principal advantages. First, the optimal fields for velocity mapping can easily be achieved even using a large molecular beam diameter (5 mm); the velocity resolution (better than 1%) is sufficient to easily resolve photo-electron recoil in (2 + 1) resonant enhanced multiphoton ionization of N 2 photoproducts from N 2 O or from molecular beam cooled N 2 . Second, rapid changes between spatial imaging, velocity mapping, and slice imaging are straightforward. We demonstrate this technique's utility in a re-investigation of the photodissociation of N 2 O. Using a hot nozzle, we observe slice images that strongly depend on nozzle temperature. Our data indicate that in our hot nozzle expansion, only pure bending vibrations -(0, v 2 , 0) -are populated, as vibrational excitation in pure stretching or bend-stretch combination modes are quenched via collisional near-resonant V-V energy transfer to the nearly degenerate bending states. We derive vibrationally state resolved absolute absorption cross-sections for (0, v 2 ≤ 7, 0). These results agree well with previous work at lower values of v 2 , both experimental and theoretical. The dissociation energy of N 2 O with respect to the O( 1 D) + N 2 1 + g asymptote was determined to be 3.65 ± 0.02 eV.

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Section: Analysis and Discussionsupporting

confidence: 91%

Section: O( 1 D) Imagessupporting

confidence: 68%

Section: Analysis and Discussionmentioning

confidence: 90%

Section: Analysis and Discussionmentioning

confidence: 94%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle

Harding

Neugebohren

Grütter

et al. 2014

The Journal of Chemical Physics

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Pulsed‐Laser Production and Detection of Spin‐Polarized Hydrogen Atoms

Rakitzis

2004

ChemPhysChem

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Spin-polarized hydrogen (SPH) atoms have traditionally been produced and detected using complex experimental methods with poor time resolution. Recently, SPH has been produced by pulsed-laser photodissociation of HCl using circularly polarized light. In combination with the proposed detection of SPH via polarized fluorescence, this approach should allow the production and spatially resolved detection of SPH with a higher sensitivity than that currently available, and with a time resolution in the nanosecond regime. This represents an improvement of several orders of magnitude over the existing methods.

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Coherent atomic orbital polarization probes the geometric phase in photodissociation of polyatomic molecules

2022

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Quantum interference between multiple pathways in molecular photodissociation often results in angular momentum polarization of atomic products and this can give deep insight into fundamental physical processes. For dissociation of diatomic molecules, the resulting orbital polarization is fully understood and consistent with quantum mechanical theory. For polyatomic molecules, however, coherent photofragment orbital polarization is frequently observed but so far has eluded theoretical explanation, and physical insight is lacking. Here, we present a model of these effects for ozone photodissociation that reveals the importance of a novel manifestation of the geometric phase. We show this geometric phase effect permits the existence of coherent polarization in cases where it would otherwise vanish, and cancels it in some cases where it might otherwise exist. The model accounts for measurements in ozone that have hitherto defied explanation, and represents a step toward a deeper understanding of coherent electronic excitation in polyatomic molecules and a new role of the geometric phase. Key Points Coherent photofragment atomic orbital polarization reveals matter wave interference in dissociation along multiple paths. In diatomic molecules, this is well‐understood, but in polyatomic molecules, large effects are seen but these have defied a rigorous explanation. A model is developed describing these phenomena in the UV dissociation of ozone that accounts for a number of conflicting observations and reveals a new manifestation of the geometric phase in molecular physics.

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State-to-state photodynamics of nitrous oxide and the effect of long-range interaction on the alignment of O(1D2)

Cited by 59 publications

References 26 publications

Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle

Single-field slice-imaging with a movable repeller: Photodissociation of N2O from a hot nozzle

Pulsed‐Laser Production and Detection of Spin‐Polarized Hydrogen Atoms

Coherent atomic orbital polarization probes the geometric phase in photodissociation of polyatomic molecules

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