A general formulation of the quasiclassical trajectory method for reduced-dimensionality reaction dynamics calculations
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Tartalom: http://real.mtak.hu/86354/
Archívum: REAL
Gyűjtemény: Status = Published
Subject = Q Science / természettudomány: QD Chemistry / kémia: QD02 Physical chemistry / fizikai kémia
Subject = Q Science / természettudomány: QC Physics / fizika: QC01 Mechanics / mechanika
Type = Article
Cím:
A general formulation of the quasiclassical trajectory method for reduced-dimensionality reaction dynamics calculations
Létrehozó:
Nagy, Tibor
Vikár, Anna
Lendvay, György
Kiadó:
Royal Society of Chemistry
Dátum:
2018-04-18
Téma:
QC01 Mechanics / mechanika
QD02 Physical chemistry / fizikai kémia
Tartalmi leírás:
Dimension reduction by freezing the unimportant coordinates is widely used in intramolecular and reaction dynamics calculations when the solution of the accurate full-dimensional nuclear Schrödinger equation is not feasible. In this paper we report on a novel form of the exact classical internal-coordinate Hamiltonian for full and reduced-dimensional vibrational motion of polyatomic molecules with the purpose of using it in quasiclassical trajectory (QCT) calculations. The derivation is based on the internal to body-fixed frame transformation, as in the t-vector formalism, however it does not require the introduction of rotational variables to allow cancellation of non-physical rotations within the body-fixed frame. The formulas needed for QCT calculations: normal mode analysis and state sampling as well as for following the dynamics and normal-mode quantum number assignment at instantaneous states are presented. The procedure is demonstrated on the CH4, CD4, CH3D and CHD3 isotopologs of methane using three reduced-dimensional models, which were previously used in quantum reactive scattering studies of the CH4+XCH3+HX type reactions. The reduced-dimensional QCT methodology formulated this way combined with full-dimensional QCT calculations makes possible the classical validation of reduced-dimensional models that are used in the quantum mechanical description of the nuclear dynamics in reactive systems [Vikár et al., J. Phys. Chem. A 120 (2016) 5083–5093.]
Nyelv:
magyar
magyar
magyar
Típus:
Article
PeerReviewed
info:eu-repo/semantics/article
Formátum:
text
text
text
Azonosító:
Nagy, Tibor and Vikár, Anna and Lendvay, György (2018) A general formulation of the quasiclassical trajectory method for reduced-dimensionality reaction dynamics calculations. Physical Chemistry Chemical Physics, 20 (19). pp. 13224-13240. ISSN 1463-9076
Kapcsolat:
10.1039/C8CP01600C