Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies

Nadia Balucani, Michele Alagia, Laura Cartechini, Piergiorgio Casavecchia, Gian Gualberto Volpi, Lisa A. Pederson, George C Schatz

Research output: Contribution to journalArticle

42 Citations (Scopus)

Abstract

The dynamics of the prototypical insertion reaction N( 2D) + D 2 have been investigated in a combined experimental and theoretical study. Angular and velocity distributions of the ND product have been obtained in crossed molecular beam experiments with mass spectrometric detection at two collision energies (E c = 3.8 and 5.1 kcal mol -1). The center-of-mass product angular and translational energy distributions have been derived; at both E c's, the former is found to be nearly backward-forward symmetric, reflecting an insertion dynamics, and the latter corresponds to a fraction of total available energy released in translation of 32%, indicating that the ND product is highly internally excited. Quasiclassical trajectory (QCT) calculations were performed on an accurate potential-energy surface obtained from large-scale ab initio electronic structure computations, and the results were compared to experiment. Generally good agreement was found between the experimental results and the theoretical predictions; however, small, yet significant, discrepancies point to some inaccuracy of the QCT treatment, calling for a quantum scattering study of the title reaction.

Original languageEnglish
Pages (from-to)2414-2422
Number of pages9
JournalJournal of Physical Chemistry A
Volume105
Issue number11
Publication statusPublished - Mar 22 2001

Fingerprint

Trajectories
trajectories
Potential energy surfaces
Molecular beams
Angular distribution
insertion
products
Velocity distribution
Electronic structure
Experiments
Scattering
molecular beams
center of mass
energy distribution
angular distribution
velocity distribution
potential energy
electronic structure
collisions
energy

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Balucani, N., Alagia, M., Cartechini, L., Casavecchia, P., Volpi, G. G., Pederson, L. A., & Schatz, G. C. (2001). Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies. Journal of Physical Chemistry A, 105(11), 2414-2422.

Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies. / Balucani, Nadia; Alagia, Michele; Cartechini, Laura; Casavecchia, Piergiorgio; Volpi, Gian Gualberto; Pederson, Lisa A.; Schatz, George C.

In: Journal of Physical Chemistry A, Vol. 105, No. 11, 22.03.2001, p. 2414-2422.

Research output: Contribution to journalArticle

Balucani, N, Alagia, M, Cartechini, L, Casavecchia, P, Volpi, GG, Pederson, LA & Schatz, GC 2001, 'Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies', Journal of Physical Chemistry A, vol. 105, no. 11, pp. 2414-2422.
Balucani N, Alagia M, Cartechini L, Casavecchia P, Volpi GG, Pederson LA et al. Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies. Journal of Physical Chemistry A. 2001 Mar 22;105(11):2414-2422.
Balucani, Nadia ; Alagia, Michele ; Cartechini, Laura ; Casavecchia, Piergiorgio ; Volpi, Gian Gualberto ; Pederson, Lisa A. ; Schatz, George C. / Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies. In: Journal of Physical Chemistry A. 2001 ; Vol. 105, No. 11. pp. 2414-2422.
@article{92f6bc14b3b74b5ab6aea0995468a43e,
title = "Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies",
abstract = "The dynamics of the prototypical insertion reaction N( 2D) + D 2 have been investigated in a combined experimental and theoretical study. Angular and velocity distributions of the ND product have been obtained in crossed molecular beam experiments with mass spectrometric detection at two collision energies (E c = 3.8 and 5.1 kcal mol -1). The center-of-mass product angular and translational energy distributions have been derived; at both E c's, the former is found to be nearly backward-forward symmetric, reflecting an insertion dynamics, and the latter corresponds to a fraction of total available energy released in translation of 32{\%}, indicating that the ND product is highly internally excited. Quasiclassical trajectory (QCT) calculations were performed on an accurate potential-energy surface obtained from large-scale ab initio electronic structure computations, and the results were compared to experiment. Generally good agreement was found between the experimental results and the theoretical predictions; however, small, yet significant, discrepancies point to some inaccuracy of the QCT treatment, calling for a quantum scattering study of the title reaction.",
author = "Nadia Balucani and Michele Alagia and Laura Cartechini and Piergiorgio Casavecchia and Volpi, {Gian Gualberto} and Pederson, {Lisa A.} and Schatz, {George C}",
year = "2001",
month = "3",
day = "22",
language = "English",
volume = "105",
pages = "2414--2422",
journal = "Journal of Physical Chemistry A",
issn = "1089-5639",
publisher = "American Chemical Society",
number = "11",

}

TY - JOUR

T1 - Dynamics of the N( 2D) + D 2 reaction from crossed-beam and quasiclassical trajectory studies

AU - Balucani, Nadia

AU - Alagia, Michele

AU - Cartechini, Laura

AU - Casavecchia, Piergiorgio

AU - Volpi, Gian Gualberto

AU - Pederson, Lisa A.

AU - Schatz, George C

PY - 2001/3/22

Y1 - 2001/3/22

N2 - The dynamics of the prototypical insertion reaction N( 2D) + D 2 have been investigated in a combined experimental and theoretical study. Angular and velocity distributions of the ND product have been obtained in crossed molecular beam experiments with mass spectrometric detection at two collision energies (E c = 3.8 and 5.1 kcal mol -1). The center-of-mass product angular and translational energy distributions have been derived; at both E c's, the former is found to be nearly backward-forward symmetric, reflecting an insertion dynamics, and the latter corresponds to a fraction of total available energy released in translation of 32%, indicating that the ND product is highly internally excited. Quasiclassical trajectory (QCT) calculations were performed on an accurate potential-energy surface obtained from large-scale ab initio electronic structure computations, and the results were compared to experiment. Generally good agreement was found between the experimental results and the theoretical predictions; however, small, yet significant, discrepancies point to some inaccuracy of the QCT treatment, calling for a quantum scattering study of the title reaction.

AB - The dynamics of the prototypical insertion reaction N( 2D) + D 2 have been investigated in a combined experimental and theoretical study. Angular and velocity distributions of the ND product have been obtained in crossed molecular beam experiments with mass spectrometric detection at two collision energies (E c = 3.8 and 5.1 kcal mol -1). The center-of-mass product angular and translational energy distributions have been derived; at both E c's, the former is found to be nearly backward-forward symmetric, reflecting an insertion dynamics, and the latter corresponds to a fraction of total available energy released in translation of 32%, indicating that the ND product is highly internally excited. Quasiclassical trajectory (QCT) calculations were performed on an accurate potential-energy surface obtained from large-scale ab initio electronic structure computations, and the results were compared to experiment. Generally good agreement was found between the experimental results and the theoretical predictions; however, small, yet significant, discrepancies point to some inaccuracy of the QCT treatment, calling for a quantum scattering study of the title reaction.

UR - http://www.scopus.com/inward/record.url?scp=0035932661&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=0035932661&partnerID=8YFLogxK

M3 - Article

VL - 105

SP - 2414

EP - 2422

JO - Journal of Physical Chemistry A

JF - Journal of Physical Chemistry A

SN - 1089-5639

IS - 11

ER -