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Molecular Tully Models [dataset] Open Access

Over the last decades, an important number of methods have been developed to simulate the nonadiabatic dynamics of molecules, that is, the dynamics of molecules beyond the Born-Oppenheimer approximation. These nonadiabatic methods differ in the way they approximate the dynamics emanating from the time-dependent molecular Schrödinger equation. In 1990, Tully devised a series of three one-dimensional model systems to test the approximations of the method called trajectory surface hopping. The Tully models were designed to probe different scenarios of nonadiabatic processes, such as single and multiple nonadiabatic (re)crossings. These one-dimensional models rapidly became the testbed for any new nonadiabatic dynamics strategy. In this work, we present a molecular perspective to the Tully models by highlighting a correspondence between these simple one-dimensional models and processes happening during the excited-state dynamics of molecules. More importantly, each of these nonadiabatic processes can be connected to a given exemplary molecular system, and we propose here three molecules that could serve as molecular Tully models, reproducing some of the key features of the original models but this time in a high-dimensional space. We compare trajectory surface hopping with the ab initio multiple spawning for the three molecular Tully models and highlight particular features and differences between these methods resulting from their distinct approximations. We also provide all the necessary information – initial conditions and all required parameters for the dynamics as well as the electronic structure – employed in our simulations such that the molecular Tully models can become in the future a unified and standardized test for ab initio nonadiabatic molecular dynamics methods. The molecular Tully models also offer an exciting link between the world of low-dimensional model systems for nonadiabatic dynamics and the excited-state dynamics of molecular systems in their full dimensionality.

Descriptions

Resource type

Dataset

Contributors

Creator: Curchod, Basile ¹
Contact person: Curchod, Basile ¹
Ibele, Lea M. ¹

¹ Durham University, UK

Funder

European Research Council
Engineering and Physical Sciences Research Council

Research methods

Other description

Initial conditions (nuclear positions and momenta) for the Molecular Tully Models (ethylene, DMABN, and ethylene).

Keyword

Nonadiabatic dynamics
Tully models
Surface hopping
Ab initio multiple spawning

Subject

Location

Language

Cited in

Identifier

ark:/32150/r1qj72p715m
doi:10.15128/r1qj72p715m

Rights

Creative Commons Attribution 4.0 International (CC BY)

Publisher

Durham University

Date Created

File Details

Depositor

B. Curchod

Date Uploaded

13 May 2020, 14:05:01

Date Modified

5 June 2020, 09:06:15

Audit Status

Audits have not yet been run on this file.

Characterization

File format: zip (ZIP Format)

Mime type: application/zip

File size: 112768

Last modified: 2020:06:05 09:19:38+01:00

Filename: molecular_tully_models.zip

Original checksum: 4cf1910828487f65a091c897ff9e8bff