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Modeling excited-state molecular dynamics beyond the Born–Oppenheimer regime

Nature Computational Science volume 2, pages 689–692 (2022)Cite this article

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Nonadiabatic molecular dynamics is the method of choice for modeling a wide range of excited-state phenomena. Although much progress has been made in improving the usability and efficiency of ground-state calculations, there are still challenges in translating this advance to the excited state.

Herein, we present a broad overview of NAMD methodologies and recent advances in the field. We then pinpoint several of the outstanding limitations and technical challenges that remain to be solved and survey emerging developments in these areas. The schematic flow of NAMD developments as new methods emerge to overcome limitations is summarized in Fig. 1. We conclude with an outlook on where the field is heading and the new theoretical advances that will be needed in order to get there.

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Fig. 1: Schematic flow of NAMD development.

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Acknowledgements

The work at Los Alamos National Laboratory (LANL) was supported by the LANL Directed Research and Development Funds (LDRD) and the Center for Integrated Nanotechnologies (CINT), a US Department of Energy, Office of Science user facility at LANL. S.F.-A. was supported by CONICET, UNQ, and ANPCyT (grant no. PICT-2018-02360). LANL is operated by Triad National Security, LLC, for the US Department of Energy National Nuclear Security Administration under contract no. 89233218CNA000001.

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Authors and Affiliations

  1. Physics and Chemistry of Materials, Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM, USA

    Tammie R. Nelson & Sergei Tretiak

  2. Departamento de Ciencia y Tecnologia, Universidad Nacional de Quilmes/CONICET, Bernal, Argentina

    Sebastian Fernandez-Alberti

  3. Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory, Los Alamos, NM, USA

    Sergei Tretiak

Authors
  1. Tammie R. Nelson
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  2. Sebastian Fernandez-Alberti
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  3. Sergei Tretiak
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Contributions

All authors developed the core manuscript content and outline, wrote the manuscript, and provided revisions. T.R.N. wrote the first manuscript draft. S.T. proposed the illustration concept and T.R.N. created the illustration.

Corresponding author

Correspondence to Sergei Tretiak.

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The authors declare no competing interests.

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Nelson, T.R., Fernandez-Alberti, S. & Tretiak, S. Modeling excited-state molecular dynamics beyond the Born–Oppenheimer regime. Nat Comput Sci 2, 689–692 (2022). https://doi.org/10.1038/s43588-022-00357-3

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