https://doi.org/10.1140/epjs/s11734-023-00905-6
Review
Current status of deMon2k for the investigation of the early stages of matter irradiation by time-dependent DFT approaches
1
Université Paris Saclay, CNRS, Institut de Chimie Physique, UMR 8000, 91405, Orsay, France
2
Department of Chemistry, College of Education, University of Sulaimani, 41005, Sulaimani, Kurdistan, Iraq
3
Theoretical Chemistry and Modelling Group (CTM), Institute of Chemistry for Life and Health Sciences (I-CLeHS), Chimie ParisTech-PSL, PSL University, CNRS, 75005, Paris, France
4
CEA, DES, ISEC, DMRC, Université Montpellier, Marcoule, 30207, Bagnols-Sur-Cèze, France
5
Department of Physics and Living Systems Institute, University of Exeter, Stocker Road, EX4 4QD, Exeter, UK
6
Department of Physics and Astronomy, University College London, WC1E 6BT, London, UK
7
Consiglio Nazionale Delle Ricerche/National Research Council (CNR)-IOM C/o International School for Advanced Studies (SISSA/ISAS), Via Bonomea 265, 34136, Trieste, Italy
8
Department of Physics, AlbaNova University Center, Stockholm University, 106 91, Stockholm, Sweden
9
Institut Charles Gerhardt de Montpellier, CNRS, ENSCM, Université de Montpellier, 34296, Montpellier, France
10
Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 99352, Richland, WA, USA
11
Institut du Développement Et Des Ressources en Informatique Scientifique, CNRS, UAR 851, Bat. 506, BP 167, 91403, Orsay Cedex, France
12
Maison de La Simulation, UAR 3441, Bâtiment 565 PC 190, Digiteo CEA Saclay, 91191, Gif-Sur-Yvette Cedex, France
s
aurelien.de-la-lande@universite-paris-saclay.fr
Received:
22
July
2022
Accepted:
15
June
2023
Published online:
3
July
2023
We summarize in this article the recent progress made in our laboratories in the development of numerical approaches dedicated to investigating ultrafast physicochemical responses of biological matter subjected to ionizing radiations. Our modules are integrated into the deMon2k software which is a readily available program with highly optimized algorithms for conducting Auxiliary Density Functional Theory (ADFT) calculations. We have developed a computational framework based on Real-Time Time-dependent ADFT to simulate the electronic responses of molecular systems to strong perturbations, while molecular dynamics simulations in the ground and excited states (Ehrenfest dynamics) are available to simulate irradiation-induced ultrafast bond breaking/formation. Constrained ADFT and Multi-component ADFT have also been incorporated to simulate charge transfer processes and nuclear quantum effects, respectively. Finally, a coupling to polarizable force fields further permits to realistically account for the electrostatic effects that the systems’ environment has on the perturbed electron density. The code runs on CPU or hybrid CPU/GPU architectures affording simulations of systems comprised up to 1000 atoms at the DFT level with controlled numerical accuracy. We illustrate the applications of these methodologies by taking results from our recent articles that aimed principally at understanding experimental data from pulse radiolysis experiments.
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© The Author(s), under exclusive licence to EDP Sciences, Springer-Verlag GmbH Germany, part of Springer Nature 2023. Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
