Quantum mechanical reactive scattering by a multiconfigurational time-dependent self-consistent field (MCTDSCF) approach

Audrey Dell Hammerich; Ronnie Kosloff; Mark A. Ratner

doi:10.1016/0009-2614(90)80057-K

Quantum mechanical reactive scattering by a multiconfigurational time-dependent self-consistent field (MCTDSCF) approach

Audrey Dell Hammerich^*, Ronnie Kosloff, Mark A. Ratner

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

69 Scopus citations

Abstract

The major obstacle to the description of systems containing a large number of degrees of freedom is the exponential increase of computational time and effort with dimensionality. A strategy is presented to overcome this obstacle as well as the shortcoming of the omission of correlations, while still maintaining the simplicity and strengths of a mean-field description, based upon identifying the crucial dynamical correlations and incorporating them with multiconfigurations. The collinear reactive scattering of H + H₂ illustrates the techniques involved and their adaptability, flexibility, and breadth of applicability. MCTDSCF simulations, constructed from time-dependent variational principles, are compared with the numerically exact solution of the Schrödinger equation; agreement is found.

Original language	English (US)
Pages (from-to)	97-108
Number of pages	12
Journal	Chemical Physics Letters
Volume	171
Issue number	1-2
DOIs	https://doi.org/10.1016/0009-2614(90)80057-K
State	Published - Jul 27 1990

Funding

This researcwh ass upportebdy a grantf romt heG IF, theG erman-IsraeFlio undationfo r ScientificR esearch and DevelopmentT.h e Fritz Haber ResearchC enterf or MolecularD ynamicsis supportedb y the Minerva Gesellschafftti r die ForschungG, mbH Munich,F ederalR epublico f GermanyA. DH gratefullya cknowledges receipot f a LadyD avisp ostdoctorfael llowshipM. R thanksth eC hemicaDl ivisiono f theN SF for partiasl upport.

ASJC Scopus subject areas

General Physics and Astronomy
Physical and Theoretical Chemistry

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10.1016/0009-2614(90)80057-K

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title = "Quantum mechanical reactive scattering by a multiconfigurational time-dependent self-consistent field (MCTDSCF) approach",

abstract = "The major obstacle to the description of systems containing a large number of degrees of freedom is the exponential increase of computational time and effort with dimensionality. A strategy is presented to overcome this obstacle as well as the shortcoming of the omission of correlations, while still maintaining the simplicity and strengths of a mean-field description, based upon identifying the crucial dynamical correlations and incorporating them with multiconfigurations. The collinear reactive scattering of H + H2 illustrates the techniques involved and their adaptability, flexibility, and breadth of applicability. MCTDSCF simulations, constructed from time-dependent variational principles, are compared with the numerically exact solution of the Schr{\"o}dinger equation; agreement is found.",

author = "{Dell Hammerich}, Audrey and Ronnie Kosloff and Ratner, {Mark A.}",

note = "Funding Information: This researcwh ass upportebdy a grantf romt heG IF, theG erman-IsraeFlio undationfo r ScientificR esearch and DevelopmentT.h e Fritz Haber ResearchC enterf or MolecularD ynamicsis supportedb y the Minerva Gesellschafftti r die ForschungG, mbH Munich,F ederalR epublico f GermanyA. DH gratefullya cknowledges receipot f a LadyD avisp ostdoctorfael llowshipM. R thanksth eC hemicaDl ivisiono f theN SF for partiasl upport.",

year = "1990",

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doi = "10.1016/0009-2614(90)80057-K",

language = "English (US)",

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T1 - Quantum mechanical reactive scattering by a multiconfigurational time-dependent self-consistent field (MCTDSCF) approach

AU - Dell Hammerich, Audrey

AU - Kosloff, Ronnie

AU - Ratner, Mark A.

N1 - Funding Information: This researcwh ass upportebdy a grantf romt heG IF, theG erman-IsraeFlio undationfo r ScientificR esearch and DevelopmentT.h e Fritz Haber ResearchC enterf or MolecularD ynamicsis supportedb y the Minerva Gesellschafftti r die ForschungG, mbH Munich,F ederalR epublico f GermanyA. DH gratefullya cknowledges receipot f a LadyD avisp ostdoctorfael llowshipM. R thanksth eC hemicaDl ivisiono f theN SF for partiasl upport.

PY - 1990/7/27

Y1 - 1990/7/27

N2 - The major obstacle to the description of systems containing a large number of degrees of freedom is the exponential increase of computational time and effort with dimensionality. A strategy is presented to overcome this obstacle as well as the shortcoming of the omission of correlations, while still maintaining the simplicity and strengths of a mean-field description, based upon identifying the crucial dynamical correlations and incorporating them with multiconfigurations. The collinear reactive scattering of H + H2 illustrates the techniques involved and their adaptability, flexibility, and breadth of applicability. MCTDSCF simulations, constructed from time-dependent variational principles, are compared with the numerically exact solution of the Schrödinger equation; agreement is found.

AB - The major obstacle to the description of systems containing a large number of degrees of freedom is the exponential increase of computational time and effort with dimensionality. A strategy is presented to overcome this obstacle as well as the shortcoming of the omission of correlations, while still maintaining the simplicity and strengths of a mean-field description, based upon identifying the crucial dynamical correlations and incorporating them with multiconfigurations. The collinear reactive scattering of H + H2 illustrates the techniques involved and their adaptability, flexibility, and breadth of applicability. MCTDSCF simulations, constructed from time-dependent variational principles, are compared with the numerically exact solution of the Schrödinger equation; agreement is found.

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JF - Chemical Physics Letters

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ER -

Quantum mechanical reactive scattering by a multiconfigurational time-dependent self-consistent field (MCTDSCF) approach

Abstract

Funding

ASJC Scopus subject areas

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